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<article xmlns:xlink="http://www.w3.org/1999/xlink" xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:oasis="http://docs.oasis-open.org/ns/oasis-exchange/table" xml:lang="en" dtd-version="3.0" article-type="research-article">
  <front>
    <journal-meta><journal-id journal-id-type="publisher">BG</journal-id><journal-title-group>
    <journal-title>Biogeosciences</journal-title>
    <abbrev-journal-title abbrev-type="publisher">BG</abbrev-journal-title><abbrev-journal-title abbrev-type="nlm-ta">Biogeosciences</abbrev-journal-title>
  </journal-title-group><issn pub-type="epub">1726-4189</issn><publisher>
    <publisher-name>Copernicus Publications</publisher-name>
    <publisher-loc>Göttingen, Germany</publisher-loc>
  </publisher></journal-meta>
    <article-meta>
      <article-id pub-id-type="doi">10.5194/bg-23-3279-2026</article-id><title-group><article-title>Subsurface dissolution reduces the efficiency of mineral-based open-ocean alkalinity enhancement</article-title><alt-title>Mineral-based alkalinity enhancement in the open ocean</alt-title>
      </title-group>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1 aff2">
          <name><surname>Burger</surname><given-names>Friedrich A.</given-names></name>
          <email>friedrich.burger@unibe.ch</email>
        <ext-link>https://orcid.org/0000-0002-7781-8498</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1 aff2">
          <name><surname>Hofmann Elizondo</surname><given-names>Urs</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-4576-471X</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1 aff2">
          <name><surname>Grosselindemann</surname><given-names>Hendrik</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-4477-6874</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1 aff2">
          <name><surname>Frölicher</surname><given-names>Thomas L.</given-names></name>
          
        </contrib>
        <aff id="aff1"><label>1</label><institution>Climate and Environmental Physics, Physics Institute, University of Bern, Bern, Switzerland</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Oeschger Centre for Climate Change Research, University of Bern, Bern, Switzerland</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Friedrich A. Burger (friedrich.burger@unibe.ch)</corresp></author-notes><pub-date><day>12</day><month>May</month><year>2026</year></pub-date>
      
      <volume>23</volume>
      <issue>9</issue>
      <fpage>3279</fpage><lpage>3298</lpage>
      <history>
        <date date-type="received"><day>28</day><month>November</month><year>2025</year></date>
           <date date-type="rev-request"><day>8</day><month>December</month><year>2025</year></date>
           <date date-type="rev-recd"><day>14</day><month>April</month><year>2026</year></date>
           <date date-type="accepted"><day>15</day><month>April</month><year>2026</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2026 Friedrich A. Burger et al.</copyright-statement>
        <copyright-year>2026</copyright-year>
      <license license-type="open-access"><license-p>This work is licensed under the Creative Commons Attribution 4.0 International License. To view a copy of this licence, visit <ext-link ext-link-type="uri" xlink:href="https://creativecommons.org/licenses/by/4.0/">https://creativecommons.org/licenses/by/4.0/</ext-link></license-p></license></permissions><self-uri xlink:href="https://bg.copernicus.org/articles/23/3279/2026/bg-23-3279-2026.html">This article is available from https://bg.copernicus.org/articles/23/3279/2026/bg-23-3279-2026.html</self-uri><self-uri xlink:href="https://bg.copernicus.org/articles/23/3279/2026/bg-23-3279-2026.pdf">The full text article is available as a PDF file from https://bg.copernicus.org/articles/23/3279/2026/bg-23-3279-2026.pdf</self-uri>
      <abstract><title>Abstract</title>

      <p id="d2e114">Carbon dioxide removal (CDR) from the atmosphere will likely be required to offset hard-to-abate emissions and limit global warming to well below 2 <inline-formula><mml:math id="M1" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">°</mml:mi><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>, in line with the Paris Agreement. Among proposed CDR strategies, ocean alkalinity enhancement (OAE) is increasingly discussed because it offers high carbon sequestration potential, long storage timescales, and potentially mitigates ocean acidification. OAE is often envisioned to occur in the open ocean through the dissolution of alkaline mineral powders, such as forsterite, the most abundant form of olivine. Fine-grained powders dissolve near the surface, where the added alkalinity can efficiently enhance oceanic carbon uptake, whereas coarser grains sink and dissolve at depth. Most modeling studies assume complete surface dissolution, leaving the impact of subsurface dissolution on ocean carbon uptake poorly understood. Here, we develop idealized vertical mineral dissolution profiles that vary with environmental conditions and grain size. These profiles are implemented in a comprehensive Earth system model to assess the capture efficiency of OAE, defined as the additional carbon taken up by the ocean per alkalinity added. We find that the efficiency is very sensitive to grain size and may decrease by more than 75 % when grain size doubles, as larger grains release the alkalinity at deeper depth. Efficiency further decreases when particles are not uniformly sized but follow a particle size distribution with the same mean particle volume. In addition, efficiency is time-dependent: it is lower in the first decades of OAE and increases as alkalinity previously released in the ocean interior eventually resurfaces, often far from deployment sites. For forsterite particles with diameter 3.4 <inline-formula><mml:math id="M2" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, the efficiency is less than one-fourth of that achieved with surface alkalinity addition over the first decade, less than one-third over the first 30 years, and less than half over 175 years. Our results indicate that forsterite grain sizes would need to be around 1.7 <inline-formula><mml:math id="M3" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> to achieve effective open-ocean alkalinity enhancement and that monitoring, reporting, and verification would be challenged by delayed and spatially dispersed carbon uptake, questioning the suitability of olivine. Minerals with faster dissolution rates may present more viable alternatives when mineral particle properties are closely controlled.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <label>1</label><title>Introduction</title>
      <p id="d2e156">Carbon dioxide removal (CDR) is widely considered necessary for achieving net-zero <inline-formula><mml:math id="M4" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> emissions targets and limiting global warming in line with the Paris Agreement <xref ref-type="bibr" rid="bib1.bibx2" id="paren.1"/>. Among various CDR approaches, marine-based methods have gained growing scientific and policy interest. In particular, ocean alkalinity enhancement (OAE) has emerged as a promising option due to its well-understood carbonate chemistry, high carbon sequestration potential, long storage timescales <xref ref-type="bibr" rid="bib1.bibx3 bib1.bibx5" id="paren.2"/>, and its potential for ocean acidification mitigation <xref ref-type="bibr" rid="bib1.bibx8" id="paren.3"/>.</p>
      <p id="d2e179">OAE is often thought to be implemented by adding alkaline mineral powders, such as the silicate mineral olivine, to the open ocean surface, where dissolution increases seawater alkalinity and enhances carbon uptake from the atmosphere <xref ref-type="bibr" rid="bib1.bibx24 bib1.bibx31" id="paren.4"/>. Global modeling studies of OAE commonly assume instantaneous and complete alkalinity release at the surface of the open ocean <xref ref-type="bibr" rid="bib1.bibx22 bib1.bibx28 bib1.bibx37 bib1.bibx42 bib1.bibx49 bib1.bibx29" id="paren.5"/> or coastal ocean <xref ref-type="bibr" rid="bib1.bibx12 bib1.bibx20" id="paren.6"/>. However, this assumption holds only if the added minerals dissolve rapidly, which depends strongly on particle size <xref ref-type="bibr" rid="bib1.bibx3 bib1.bibx31" id="paren.7"/>. Outside shallow and well-mixed coastal waters, slowly dissolving coarser particles sink quickly, releasing alkalinity at depth rather than near the surface. Alkalinity released in the ocean interior contributes to oceanic carbon uptake only when those waters re-emerge at the surface, a process that can take decades to centuries depending on the regional ocean ventilation timescales. Conversely, grinding minerals to finer sizes increases dissolution rates but comes at the cost of higher life-cycle energy demand and associated <inline-formula><mml:math id="M5" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> emissions <xref ref-type="bibr" rid="bib1.bibx13" id="paren.8"/>.</p>
      <p id="d2e209">A few studies have analyzed the mineral dissolution dynamics, particularly for the silicate mineral olivine, using simplified analytical shrinking core models that idealize mineral particles as smooth spheres <xref ref-type="bibr" rid="bib1.bibx19" id="paren.9"/>. These models have been used to estimate dissolution times and carbon uptake in coastal OAE settings <xref ref-type="bibr" rid="bib1.bibx19 bib1.bibx12" id="paren.10"/> and to approximate alkalinity release within the surface mixed layer of the open ocean <xref ref-type="bibr" rid="bib1.bibx25 bib1.bibx35 bib1.bibx48" id="paren.11"/>. In contrast, <xref ref-type="bibr" rid="bib1.bibx11" id="text.12"/> employed a complex mineral particle model to simulate alkalinity release in an Earth system model of reduced complexity and coarse spatial resolution. These studies show that dissolution time increases strongly with particle size, highlight regional differences in mixed layer alkalinity release, and identify potential interactions between seeded particles and planktonic communities. Nevertheless, we currently lack knowledge about the impact of particle sinking during dissolution on OAE efficiency, which needs to be assessed with ocean-biogeochemical models or Earth system models.</p>
      <p id="d2e224">Here, we analyze the efficiency of mineral-based OAE using a comprehensive, fully coupled Earth system model that explicitly accounts for the interplay between particle sinking and dissolution, represented through a shrinking core model <xref ref-type="bibr" rid="bib1.bibx19" id="paren.13"/>. We derive simple analytical vertical alkalinity release profiles and apply them as boundary conditions to the Earth system model. The analysis focuses on the influence of particle size, particle size distribution, and deployment location on alkalinity release and OAE-induced carbon uptake. We mainly discuss the alkaline mineral olivine, often considered for its relatively high dissolution rate compared to other silicate minerals, and also draw a comparison to the faster dissolving mineral brucite. Following the CDRMIP protocol <xref ref-type="bibr" rid="bib1.bibx23" id="paren.14"/>, mineral powders are homogeneously added to the world ocean, totaling to 4.92<inline-formula><mml:math id="M6" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">Gt</mml:mi></mml:mrow></mml:math></inline-formula> forsterite (the most abundant form of olivine) or 4.08<inline-formula><mml:math id="M7" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">Gt</mml:mi></mml:mrow></mml:math></inline-formula> brucite per year. For both minerals, the current annual world production is on the order of a few <inline-formula><mml:math id="M8" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">Mt</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>  <xref ref-type="bibr" rid="bib1.bibx6" id="paren.15"/>, highlighting the idealized character of the model experiment. Section <xref ref-type="sec" rid="Ch1.S2"/> describes the alkalinity release profiles, the treatment of varying environmental conditions for these profiles, as well as the experimental design for the Earth system model. Section <xref ref-type="sec" rid="Ch1.S3"/> presents the resulting regional variations in the vertical alkalinity release profiles and quantifies the sensitivity of carbon uptake efficiency to particle size, both for uniform particles and a particle size distribution. The results and their limitations are discussed in Sect. <xref ref-type="sec" rid="Ch1.S4"/>.</p>
</sec>
<sec id="Ch1.S2">
  <label>2</label><title>Methods</title>
<sec id="Ch1.S2.SS1">
  <label>2.1</label><title>Alkalinity release profiles</title>
<sec id="Ch1.S2.SS1.SSS1">
  <label>2.1.1</label><title>Particle dissolution in the shrinking core model</title>
      <p id="d2e298">We consider spherical particles with a dissolution rate that is proportional to the surface area (constant area-normalized dissolution rate <inline-formula><mml:math id="M9" display="inline"><mml:mi>r</mml:mi></mml:math></inline-formula> in <inline-formula><mml:math id="M10" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>). The decrease in the number of moles of the mineral stored in the particle <inline-formula><mml:math id="M11" display="inline"><mml:mrow><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> per time is given by the product of <inline-formula><mml:math id="M12" display="inline"><mml:mi>r</mml:mi></mml:math></inline-formula> and the surface area <inline-formula><mml:math id="M13" display="inline"><mml:mi>A</mml:mi></mml:math></inline-formula>:

              <disp-formula id="Ch1.E1" content-type="numbered"><label>1</label><mml:math id="M14" display="block"><mml:mrow><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>=</mml:mo><mml:mo>-</mml:mo><mml:mi>r</mml:mi><mml:mo>⋅</mml:mo><mml:mi>A</mml:mi></mml:mrow></mml:math></disp-formula></p>
      <p id="d2e390">As a result, the particle diameter (<inline-formula><mml:math id="M15" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula>) decreases linearly with time <xref ref-type="bibr" rid="bib1.bibx19" id="paren.16"><named-content content-type="pre">see also</named-content></xref>:

              <disp-formula id="Ch1.E2" content-type="numbered"><label>2</label><mml:math id="M16" display="block"><mml:mrow><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>d</mml:mi></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>=</mml:mo><mml:munder><mml:munder class="underbrace"><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>d</mml:mi></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>V</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo mathvariant="normal">︸</mml:mo></mml:munder><mml:mrow><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2</mml:mn><mml:mo>/</mml:mo><mml:mi>A</mml:mi></mml:mrow></mml:munder><mml:mo>⋅</mml:mo><mml:munder><mml:munder class="underbrace"><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>V</mml:mi></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub></mml:mrow></mml:mfrac></mml:mstyle><mml:mo mathvariant="normal">︸</mml:mo></mml:munder><mml:mrow><mml:mo>=</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mtext>mol</mml:mtext></mml:msub></mml:mrow></mml:munder><mml:mo>⋅</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>=</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn><mml:mi>r</mml:mi><mml:msub><mml:mi>V</mml:mi><mml:mtext>mol</mml:mtext></mml:msub></mml:mrow></mml:math></disp-formula>

            with <inline-formula><mml:math id="M17" display="inline"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mtext>mol</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> as the molar volume of the mineral (the molar mass of the mineral divided by its density). Such a simple particle dissolution model is referred to as a <italic>shrinking core model</italic>.  When this particle is sinking with speed <inline-formula><mml:math id="M18" display="inline"><mml:mrow><mml:msub><mml:mi>v</mml:mi><mml:mtext>sink</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> during dissolution, the change in <inline-formula><mml:math id="M19" display="inline"><mml:mrow><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> per depth is given by the change per time divided by sinking speed:

              <disp-formula id="Ch1.E3" content-type="numbered"><label>3</label><mml:math id="M20" display="block"><mml:mrow><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>z</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>⋅</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mrow><mml:msub><mml:mi>v</mml:mi><mml:mtext>sink</mml:mtext></mml:msub></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>=</mml:mo><mml:mo>-</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi>r</mml:mi><mml:mo>⋅</mml:mo><mml:mi>A</mml:mi></mml:mrow><mml:mrow><mml:msub><mml:mi>v</mml:mi><mml:mtext>sink</mml:mtext></mml:msub></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>.</mml:mo></mml:mrow></mml:math></disp-formula></p>
      <p id="d2e617">The term <inline-formula><mml:math id="M21" display="inline"><mml:mrow><mml:msub><mml:mi>v</mml:mi><mml:mtext>sink</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> is the Stokes settling velocity of a sinking spherical particle of diameter <inline-formula><mml:math id="M22" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula>,

              <disp-formula id="Ch1.E4" content-type="numbered"><label>4</label><mml:math id="M23" display="block"><mml:mrow><mml:msub><mml:mi>v</mml:mi><mml:mtext>sink</mml:mtext></mml:msub><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mo>(</mml:mo><mml:msub><mml:mi mathvariant="italic">ρ</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi mathvariant="italic">ρ</mml:mi><mml:mi mathvariant="normal">w</mml:mi></mml:msub><mml:mo>)</mml:mo><mml:mi>g</mml:mi><mml:msup><mml:mi>d</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow><mml:mrow><mml:mn mathvariant="normal">18</mml:mn><mml:mi mathvariant="italic">μ</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>

            with the gravitational acceleration <inline-formula><mml:math id="M24" display="inline"><mml:mi>g</mml:mi></mml:math></inline-formula>, particle density <inline-formula><mml:math id="M25" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">ρ</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, seawater density <inline-formula><mml:math id="M26" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">ρ</mml:mi><mml:mi mathvariant="normal">w</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, and the dynamic viscosity of seawater <inline-formula><mml:math id="M27" display="inline"><mml:mi mathvariant="italic">μ</mml:mi></mml:math></inline-formula>. Since both <inline-formula><mml:math id="M28" display="inline"><mml:mrow><mml:msub><mml:mi>v</mml:mi><mml:mtext>sink</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> and the particle surface area <inline-formula><mml:math id="M29" display="inline"><mml:mrow><mml:mi>A</mml:mi><mml:mo>=</mml:mo><mml:mi mathvariant="italic">π</mml:mi><mml:msup><mml:mi>d</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> are proportional to <inline-formula><mml:math id="M30" display="inline"><mml:mrow><mml:msup><mml:mi>d</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula>, the dependence of <inline-formula><mml:math id="M31" display="inline"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub><mml:mo>/</mml:mo><mml:mi mathvariant="normal">d</mml:mi><mml:mi>z</mml:mi></mml:mrow></mml:math></inline-formula> on <inline-formula><mml:math id="M32" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> cancels out and <inline-formula><mml:math id="M33" display="inline"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub><mml:mo>/</mml:mo><mml:mi mathvariant="normal">d</mml:mi><mml:mi>z</mml:mi></mml:mrow></mml:math></inline-formula> does not change with particle size. Therefore, larger particles release more alkalinity per unit time due to their larger surface area but also sink faster, such that they lose the same number of moles per depth as smaller particles.</p>

      <fig id="F1" specific-use="star"><label>Figure 1</label><caption><p id="d2e809">Alkalinity release profiles for <bold>(a)</bold> uniform particles (Sect. <xref ref-type="sec" rid="Ch1.S2.SS1.SSS2"/>) and <bold>(b)</bold> for particles with an exponential particle size distribution (Sect. <xref ref-type="sec" rid="Ch1.S2.SS1.SSS3"/>).</p></caption>
            <graphic xlink:href="https://bg.copernicus.org/articles/23/3279/2026/bg-23-3279-2026-f01.png"/>

          </fig>

      <p id="d2e828">The penetration depth <inline-formula><mml:math id="M34" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is the depth at which a particle with an initial diameter <inline-formula><mml:math id="M35" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> is completely dissolved. It is given by

              <disp-formula id="Ch1.E5" content-type="numbered"><label>5</label><mml:math id="M36" display="block"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:munder><mml:munder class="underbrace"><mml:mrow><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub><mml:mo>(</mml:mo><mml:mn mathvariant="normal">0</mml:mn><mml:mo>)</mml:mo></mml:mrow><mml:mo mathvariant="normal">︸</mml:mo></mml:munder><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mi mathvariant="normal">d</mml:mi></mml:msub><mml:mo>/</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mtext>mol</mml:mtext></mml:msub></mml:mrow></mml:munder><mml:mo mathsize="2.0em">/</mml:mo><mml:mfenced close=")" open="("><mml:mrow><mml:mo>-</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>z</mml:mi></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:mfenced><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mo>(</mml:mo><mml:msub><mml:mi mathvariant="italic">ρ</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi mathvariant="italic">ρ</mml:mi><mml:mi mathvariant="normal">w</mml:mi></mml:msub><mml:mo>)</mml:mo><mml:mi>g</mml:mi><mml:msub><mml:mi>V</mml:mi><mml:mi mathvariant="normal">d</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mn mathvariant="normal">18</mml:mn><mml:mi mathvariant="italic">π</mml:mi><mml:mi mathvariant="italic">μ</mml:mi><mml:mi>r</mml:mi><mml:msub><mml:mi>V</mml:mi><mml:mtext>mol</mml:mtext></mml:msub></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:math></disp-formula></p>
      <p id="d2e953">The penetration depth <inline-formula><mml:math id="M37" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is much larger for larger particles, since it is proportional to the initial particle volume <inline-formula><mml:math id="M38" display="inline"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mi mathvariant="normal">d</mml:mi></mml:msub><mml:mo>=</mml:mo><mml:mstyle displaystyle="false"><mml:mfrac style="text"><mml:mi mathvariant="italic">π</mml:mi><mml:mn mathvariant="normal">6</mml:mn></mml:mfrac></mml:mstyle><mml:msup><mml:mi>d</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula>, and thus proportional to the cube of its initial particle diameter.</p>
</sec>
<sec id="Ch1.S2.SS1.SSS2">
  <label>2.1.2</label><title>Alkalinity release profile for a flux of uniform particles</title>
      <p id="d2e999">With a flux of incoming mineral particles <inline-formula><mml:math id="M39" display="inline"><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> (number of particles per <inline-formula><mml:math id="M40" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi mathvariant="normal">s</mml:mi></mml:mrow></mml:math></inline-formula>), the total alkalinity (<inline-formula><mml:math id="M41" display="inline"><mml:mrow><mml:msub><mml:mi>A</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) release per unit time at depth <inline-formula><mml:math id="M42" display="inline"><mml:mi>z</mml:mi></mml:math></inline-formula> (<inline-formula><mml:math id="M43" display="inline"><mml:mi>z</mml:mi></mml:math></inline-formula> defined positive and increasing with depth) is the product of the incoming particle flux and the alkalinity release of each particle:

              <disp-formula id="Ch1.E6" content-type="numbered"><label>6</label><mml:math id="M44" display="block"><mml:mrow><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>A</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>)</mml:mo><mml:mo>=</mml:mo><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub><mml:mo>⋅</mml:mo><mml:mfenced open="(" close=")"><mml:mrow><mml:mo>-</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>z</mml:mi></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:mfenced><mml:mo>⋅</mml:mo><mml:msub><mml:mi>n</mml:mi><mml:mtext>Alk</mml:mtext></mml:msub><mml:mo>=</mml:mo><mml:mfenced open="{" close=""><mml:mtable rowspacing="0.2ex" class="cases" columnspacing="1em" columnalign="left left" framespacing="0em"><mml:mtr><mml:mtd><mml:mstyle displaystyle="false"><mml:mstyle displaystyle="false"><mml:mfrac style="text"><mml:mi>F</mml:mi><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:mfrac></mml:mstyle></mml:mstyle></mml:mtd><mml:mtd><mml:mrow><mml:mtext>for </mml:mtext><mml:mi>z</mml:mi><mml:mo>≤</mml:mo><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mrow><mml:mtext>for </mml:mtext><mml:mi>z</mml:mi><mml:mo>&gt;</mml:mo><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mo>.</mml:mo></mml:mrow></mml:mtd></mml:mtr></mml:mtable></mml:mfenced></mml:mrow></mml:math></disp-formula>

            with alkalinity in units <inline-formula><mml:math id="M45" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>. The factor <inline-formula><mml:math id="M46" display="inline"><mml:mrow><mml:msub><mml:mi>n</mml:mi><mml:mtext>Alk</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> represents the alkalinity release per dissolved mineral molecule (<inline-formula><mml:math id="M47" display="inline"><mml:mrow><mml:msub><mml:mi>n</mml:mi><mml:mtext>Alk</mml:mtext></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">4</mml:mn></mml:mrow></mml:math></inline-formula> for olivine). <inline-formula><mml:math id="M48" display="inline"><mml:mi>F</mml:mi></mml:math></inline-formula> denotes the flux of alkalinity stored in the mineral particles entering the ocean (in <inline-formula><mml:math id="M49" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>), related to the particle flux <inline-formula><mml:math id="M50" display="inline"><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> through <inline-formula><mml:math id="M51" display="inline"><mml:mrow><mml:mi>F</mml:mi><mml:mo>=</mml:mo><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub><mml:mo>⋅</mml:mo><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub><mml:mo>(</mml:mo><mml:mn mathvariant="normal">0</mml:mn><mml:mo>)</mml:mo><mml:mo>⋅</mml:mo><mml:msub><mml:mi>n</mml:mi><mml:mtext>Alk</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>. Similarly as before, the factor <inline-formula><mml:math id="M52" display="inline"><mml:mrow><mml:msub><mml:mi>n</mml:mi><mml:mtext>Alk</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> here translates from the initial number of moles of the mineral in each particle to the corresponding number of moles of alkalinity. Thus, the alkalinity release per unit time is simply given by the mineral alkalinity flux <inline-formula><mml:math id="M53" display="inline"><mml:mi>F</mml:mi></mml:math></inline-formula> applied to the surface divided by the penetration depth <inline-formula><mml:math id="M54" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> for <inline-formula><mml:math id="M55" display="inline"><mml:mrow><mml:mi>z</mml:mi><mml:mo>≤</mml:mo><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and vanishing for <inline-formula><mml:math id="M56" display="inline"><mml:mrow><mml:mi>z</mml:mi><mml:mo>&gt;</mml:mo><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>. The alkalinity release profile for uniform particles is depicted in Fig. <xref ref-type="fig" rid="F1"/>a and validated by an explicit numerical simulation of sinking particles in Appendix Fig. <xref ref-type="fig" rid="FA2"/>.</p>
</sec>
<sec id="Ch1.S2.SS1.SSS3">
  <label>2.1.3</label><title>Alkalinity release profile for an exponential particle size distribution</title>
      <p id="d2e1360">Now, we consider the case where the mineral particles are not uniform but follow a certain particle size distribution (PSD). To test the effect of particle size dispersion, we here assume an exponential PSD for the distribution of particle number over particle volumes, with the probability density function given by

              <disp-formula id="Ch1.E7" content-type="numbered"><label>7</label><mml:math id="M57" display="block"><mml:mrow><mml:mi>f</mml:mi><mml:mo>(</mml:mo><mml:mi>V</mml:mi><mml:mo>)</mml:mo><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mi mathvariant="normal">d</mml:mi></mml:msub></mml:mrow></mml:mfrac></mml:mstyle><mml:msup><mml:mi>e</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mi>V</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mi mathvariant="normal">d</mml:mi></mml:msub></mml:mrow></mml:msup><mml:mo>.</mml:mo></mml:mrow></mml:math></disp-formula></p>
      <p id="d2e1405">The mean particle volume for this PSD is <inline-formula><mml:math id="M58" display="inline"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mi mathvariant="normal">d</mml:mi></mml:msub><mml:mo>=</mml:mo><mml:mstyle displaystyle="false"><mml:mfrac style="text"><mml:mi mathvariant="italic">π</mml:mi><mml:mn mathvariant="normal">6</mml:mn></mml:mfrac></mml:mstyle><mml:msup><mml:mi>d</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> for a given mean volume diameter <inline-formula><mml:math id="M59" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula>. As such, the PSD does not change the average particle volume and alkalinity content relative to uniform particles with the same mean volume diameter <inline-formula><mml:math id="M60" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula>, but adds dispersion around this average volume. As a function of diameter, the PSD is equivalent to a Rosin–Rammler (or identically Weibull) distribution with shape 3 and scale given by the mean volume diameter <inline-formula><mml:math id="M61" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> (shown in Appendix Fig. <xref ref-type="fig" rid="FA1"/>a).</p>
      <p id="d2e1455">The Rosin–Rammler distribution is a common model for mineral particle size distributions <xref ref-type="bibr" rid="bib1.bibx21" id="paren.17"><named-content content-type="pre">e.g.,</named-content></xref>. The shape parameter of 3 indicates a light-tailed distribution. The distribution of particle mass for this PSD is a generalized gamma distribution with shape parameters 3 and 6 and scale <inline-formula><mml:math id="M62" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> (Appendix Fig. <xref ref-type="fig" rid="FA1"/>b), obtained by weighing the probability density for particle number by particle mass and then normalizing the result to 1. The P80 is the 80th percentile of this mass distribution.</p>
      <p id="d2e1472">This PSD can now be used to derive the corresponding alkalinity release profile. As discussed before, each particle within the exponential PSD releases the same amount of alkalinity per unit depth. However, smaller particles from the PSD vanish with increasing depth, such that the overall alkalinity release at depth originates from the remaining larger particles, leading to a decrease in alkalinity release with depth.</p>
      <p id="d2e1476">Equation (<xref ref-type="disp-formula" rid="Ch1.E5"/>) can be used to determine the minimum initial volume (<inline-formula><mml:math id="M63" display="inline"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mtext>min</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>) for which a particle is still present at depth <inline-formula><mml:math id="M64" display="inline"><mml:mi>z</mml:mi></mml:math></inline-formula>. Realizing that <inline-formula><mml:math id="M65" display="inline"><mml:mrow><mml:mi>z</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mtext>min</mml:mtext></mml:msub><mml:mo>=</mml:mo><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mo>/</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mi mathvariant="normal">d</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, one obtains

              <disp-formula id="Ch1.E8" content-type="numbered"><label>8</label><mml:math id="M66" display="block"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mtext>min</mml:mtext></mml:msub><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>)</mml:mo><mml:mo>=</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mi mathvariant="normal">d</mml:mi></mml:msub><mml:mo>⋅</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mi>z</mml:mi><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>.</mml:mo></mml:mrow></mml:math></disp-formula></p>
      <p id="d2e1565">The alkalinity release per unit time at depth <inline-formula><mml:math id="M67" display="inline"><mml:mi>z</mml:mi></mml:math></inline-formula> is the product of the remaining incoming particles at depth <inline-formula><mml:math id="M68" display="inline"><mml:mi>z</mml:mi></mml:math></inline-formula> and the alkalinity release of each particle:

              <disp-formula id="Ch1.E9" content-type="numbered"><label>9</label><mml:math id="M69" display="block"><mml:mtable class="split" rowspacing="0.2ex" displaystyle="true" columnalign="right left"><mml:mtr><mml:mtd><mml:mrow><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>A</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:mo>=</mml:mo><mml:mfenced close=")" open="("><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub><mml:mo>⋅</mml:mo><mml:munderover><mml:mo movablelimits="false">∫</mml:mo><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mtext>min</mml:mtext></mml:msub><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>)</mml:mo></mml:mrow><mml:mi mathvariant="normal">∞</mml:mi></mml:munderover><mml:mi>f</mml:mi><mml:mo>(</mml:mo><mml:mi>V</mml:mi><mml:mo>)</mml:mo><mml:mi mathvariant="normal">d</mml:mi><mml:mi>V</mml:mi></mml:mrow></mml:mfenced><mml:mo>⋅</mml:mo><mml:mfenced close=")" open="("><mml:mrow><mml:mo>-</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>z</mml:mi></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:mfenced><mml:mo>⋅</mml:mo><mml:msub><mml:mi>n</mml:mi><mml:mtext>Alk</mml:mtext></mml:msub></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><mml:mo>=</mml:mo><mml:mfenced close=")" open="("><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub><mml:mo>⋅</mml:mo><mml:msup><mml:mi>e</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mtext>min</mml:mtext></mml:msub><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>)</mml:mo><mml:mo>/</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mi mathvariant="normal">d</mml:mi></mml:msub></mml:mrow></mml:msup></mml:mrow></mml:mfenced><mml:mo>⋅</mml:mo><mml:mfenced open="(" close=")"><mml:mrow><mml:mo>-</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>z</mml:mi></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:mfenced><mml:mo>⋅</mml:mo><mml:msub><mml:mi>n</mml:mi><mml:mtext>Alk</mml:mtext></mml:msub></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mi>F</mml:mi><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:mfrac></mml:mstyle><mml:msup><mml:mi>e</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mi>z</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:msup><mml:mo>.</mml:mo></mml:mrow></mml:mtd></mml:mtr></mml:mtable></mml:math></disp-formula></p>
      <p id="d2e1781">As such, we get an exponentially declining alkalinity release profile when the particle volume is distributed according to an exponential distribution (depicted in Fig. <xref ref-type="fig" rid="F1"/>b). The exponential decline in alkalinity release is controlled by the penetration depth <inline-formula><mml:math id="M70" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, the depth at which particles with mean volume diameter <inline-formula><mml:math id="M71" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> are completely dissolved. The alkalinity release at the surface is equal to that of the uniform particle profile.</p>
</sec>
</sec>
<sec id="Ch1.S2.SS2">
  <label>2.2</label><title>Alkalinity release in the ocean mixed layer</title>
      <p id="d2e1813">The fraction <inline-formula><mml:math id="M72" display="inline"><mml:mi mathvariant="italic">χ</mml:mi></mml:math></inline-formula> of alkalinity that is released in the mixed layer can be calculated by integrating the alkalinity release profile down to the mixed layer depth (<inline-formula><mml:math id="M73" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow></mml:math></inline-formula>), divided by the total alkalinity release per area and time, <inline-formula><mml:math id="M74" display="inline"><mml:mi>F</mml:mi></mml:math></inline-formula>. Here, we use the mean annual maximum mixed layer depth for <inline-formula><mml:math id="M75" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow></mml:math></inline-formula>, representing the frequently ventilated ocean volume. For the uniform particle profile (Eq. <xref ref-type="disp-formula" rid="Ch1.E6"/>), the fraction dissolving in the mixed layer is given by

            <disp-formula id="Ch1.E10" content-type="numbered"><label>10</label><mml:math id="M76" display="block"><mml:mrow><mml:mi mathvariant="italic">χ</mml:mi><mml:mo>=</mml:mo><mml:mfenced open="{" close=""><mml:mtable rowspacing="0.2ex" class="cases" columnspacing="1em" columnalign="left left" framespacing="0em"><mml:mtr><mml:mtd><mml:mrow><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow><mml:mo>/</mml:mo><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:mtext>for </mml:mtext><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>≤</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd><mml:mn mathvariant="normal">1</mml:mn></mml:mtd><mml:mtd><mml:mrow><mml:mtext>for </mml:mtext><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>&gt;</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mo>.</mml:mo></mml:mrow></mml:mtd></mml:mtr></mml:mtable></mml:mfenced></mml:mrow></mml:math></disp-formula></p>
      <p id="d2e1915">Previous studies have calculated the fraction of alkalinity released in the mixed layer based on the decline in particle size during the mixed layer residence time <inline-formula><mml:math id="M77" display="inline"><mml:mrow><mml:msub><mml:mi>t</mml:mi><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> in the shrinking core model, <inline-formula><mml:math id="M78" display="inline"><mml:mrow><mml:mi mathvariant="italic">χ</mml:mi><mml:mo>(</mml:mo><mml:msub><mml:mi>t</mml:mi><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow></mml:msub><mml:mo>)</mml:mo><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>-</mml:mo><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msup><mml:mo>(</mml:mo><mml:msub><mml:mi>t</mml:mi><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow></mml:msub><mml:mo>)</mml:mo><mml:mo>/</mml:mo><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msup><mml:mo>(</mml:mo><mml:mn mathvariant="normal">0</mml:mn><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>, assuming a constant sinking velocity within the mixed layer such that <inline-formula><mml:math id="M79" display="inline"><mml:mrow><mml:msub><mml:mi>t</mml:mi><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow></mml:msub><mml:mo>=</mml:mo><mml:mstyle displaystyle="false"><mml:mfrac style="text"><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow><mml:mrow><mml:msub><mml:mi>v</mml:mi><mml:mtext>sink</mml:mtext></mml:msub><mml:mo>(</mml:mo><mml:mi>R</mml:mi><mml:mo>(</mml:mo><mml:mn mathvariant="normal">0</mml:mn><mml:mo>)</mml:mo><mml:mo>)</mml:mo></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:math></inline-formula>
<xref ref-type="bibr" rid="bib1.bibx25 bib1.bibx35 bib1.bibx48" id="paren.18"/>. Our result (Eq. <xref ref-type="disp-formula" rid="Ch1.E10"/>) does not require this approximation and is equivalent to computing <inline-formula><mml:math id="M80" display="inline"><mml:mrow><mml:mi mathvariant="italic">χ</mml:mi><mml:mo>(</mml:mo><mml:msub><mml:mi>t</mml:mi><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow></mml:msub><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> using the exact residence time obtained from <inline-formula><mml:math id="M81" display="inline"><mml:mrow><mml:msubsup><mml:mo>∫</mml:mo><mml:mn mathvariant="normal">0</mml:mn><mml:mrow><mml:msub><mml:mi>t</mml:mi><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:msubsup><mml:msub><mml:mi>v</mml:mi><mml:mtext>sink</mml:mtext></mml:msub><mml:mo>(</mml:mo><mml:mi>R</mml:mi><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo><mml:mo>)</mml:mo><mml:mi mathvariant="normal">d</mml:mi><mml:mi>t</mml:mi><mml:mo>=</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> for <inline-formula><mml:math id="M82" display="inline"><mml:mrow><mml:msub><mml:mi>t</mml:mi><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula>.</p>
      <p id="d2e2101">For the exponential PSD profile (Eq. <xref ref-type="disp-formula" rid="Ch1.E9"/>), integrating the alkalinity release profile down to the <inline-formula><mml:math id="M83" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow></mml:math></inline-formula> and normalizing by <inline-formula><mml:math id="M84" display="inline"><mml:mi>F</mml:mi></mml:math></inline-formula> results in

            <disp-formula id="Ch1.E11" content-type="numbered"><label>11</label><mml:math id="M85" display="block"><mml:mrow><mml:mi mathvariant="italic">χ</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>-</mml:mo><mml:mi>exp⁡</mml:mi><mml:mo>(</mml:mo><mml:mo>-</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow><mml:mo>/</mml:mo><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mo>)</mml:mo><mml:mo>.</mml:mo></mml:mrow></mml:math></disp-formula></p>
</sec>
<sec id="Ch1.S2.SS3">
  <label>2.3</label><title>Variation of alkalinity release profiles with environmental conditions</title>
      <p id="d2e2163">The analytical alkalinity release profiles from Sects. <xref ref-type="sec" rid="Ch1.S2.SS1.SSS2"/> and <xref ref-type="sec" rid="Ch1.S2.SS1.SSS3"/> make the assumption of constant environmental conditions throughout particle dissolution. In the ocean, however, temperature and pH typically decrease with depth. A decrease in temperature (<inline-formula><mml:math id="M86" display="inline"><mml:mi>T</mml:mi></mml:math></inline-formula>) reduces the area-normalized dissolution rate <inline-formula><mml:math id="M87" display="inline"><mml:mi>r</mml:mi></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx19 bib1.bibx36" id="paren.19"/>, which, to a lesser extent, is countered by an increase in the dissolution rate from the co-occurring decrease in pH. In addition, a reduction in temperature will also increase dynamic viscosity, reducing the particles' sinking velocity. The impact of vertical temperature and pH variations on alkalinity release is further discussed in Sect. <xref ref-type="sec" rid="Ch1.S4.SS2"/>.</p>
      <p id="d2e2190">To obtain simple analytical alkalinity release profiles, in particular for non-uniform PSDs, we here use local vertically averaged temperature and pH to determine the penetration depths <inline-formula><mml:math id="M88" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> for the dissolution profiles. However, <inline-formula><mml:math id="M89" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> depends on the vertical range over which the mean temperature and pH are determined. For example, using average conditions over the upper 100 <inline-formula><mml:math id="M90" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> will result in higher dissolution rates and a shallower penetration depth <inline-formula><mml:math id="M91" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> than using average conditions over the upper 1000 <inline-formula><mml:math id="M92" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, due to the colder temperatures in the ocean interior. The former would be more appropriate for smaller particles that dissolve close to the surface while the latter would be more appropriate for larger particles. To take into account that larger particles experience colder temperatures (and a often lower pH), we calculate the penetration depth <inline-formula><mml:math id="M93" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> from Eq. (<xref ref-type="disp-formula" rid="Ch1.E5"/>) with the mean conditions in temperature and pH between the surface and the penetration depth itself (<inline-formula><mml:math id="M94" display="inline"><mml:mrow><mml:msub><mml:mover accent="true"><mml:mi>T</mml:mi><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mrow><mml:mn mathvariant="normal">0</mml:mn><mml:mo>→</mml:mo><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M95" display="inline"><mml:mrow><mml:msub><mml:mover accent="true"><mml:mtext>pH</mml:mtext><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mrow><mml:mn mathvariant="normal">0</mml:mn><mml:mo>→</mml:mo><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula>). In other words, <inline-formula><mml:math id="M96" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is calculated self-consistently with mean conditions in temperature and pH over the same vertical range. To do so, we solve

            <disp-formula id="Ch1.E12" content-type="numbered"><label>12</label><mml:math id="M97" display="block"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:mi>f</mml:mi><mml:mo>(</mml:mo><mml:mi>r</mml:mi><mml:mo>(</mml:mo><mml:msub><mml:mover accent="true"><mml:mi>T</mml:mi><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mrow><mml:mn mathvariant="normal">0</mml:mn><mml:mo>→</mml:mo><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:msub><mml:mo>,</mml:mo><mml:msub><mml:mover accent="true"><mml:mtext>pH</mml:mtext><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mrow><mml:mn mathvariant="normal">0</mml:mn><mml:mo>→</mml:mo><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:msub><mml:mo>)</mml:mo><mml:mo>,</mml:mo><mml:mi mathvariant="italic">μ</mml:mi><mml:mo>(</mml:mo><mml:msub><mml:mover accent="true"><mml:mi>T</mml:mi><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mrow><mml:mn mathvariant="normal">0</mml:mn><mml:mo>→</mml:mo><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:msub><mml:mo>)</mml:mo><mml:mo>)</mml:mo><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>

          numerically for <inline-formula><mml:math id="M98" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>. Following this approach, a particle that dissolves close to the surface (small <inline-formula><mml:math id="M99" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>) is modeled to dissolve under a warmer average temperature than a particle that penetrates the colder deep ocean (large <inline-formula><mml:math id="M100" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>).</p>
</sec>
<sec id="Ch1.S2.SS4">
  <label>2.4</label><title>Experimental design with GFDL ESM2M</title>
      <p id="d2e2439">In this study, we use the Earth system model GFDL ESM2M to determine OAE efficiency for the here developed alkalinity release profiles. GFDL ESM2M <xref ref-type="bibr" rid="bib1.bibx9 bib1.bibx10" id="paren.20"/> is a fully coupled carbon-climate Earth system model from NOAA GFDL, which contributed to the Coupled Model Intercomparison Project phase 5 (CMIP5). Its ocean component MOM4p1 <xref ref-type="bibr" rid="bib1.bibx16" id="paren.21"/> uses a horizontal grid with 1° nominal resolution and 50 vertical layers with 10 <inline-formula><mml:math id="M101" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> vertical resolution in the upper ocean. Ocean biogeochemistry is simulated by the Tracers of Ocean Phytoplankton with Allometric Zooplankton version two <xref ref-type="bibr" rid="bib1.bibx10" id="paren.22"><named-content content-type="pre">TOPAZv2</named-content></xref>, and carbonate chemistry follows the OCMIP2 recommendations <xref ref-type="bibr" rid="bib1.bibx30" id="paren.23"/> with air-sea <inline-formula><mml:math id="M102" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> exchange determined by the bulk parameterization by <xref ref-type="bibr" rid="bib1.bibx45" id="text.24"/>.</p>
      <p id="d2e2479">As a first step, the penetration depth parameter <inline-formula><mml:math id="M103" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is calculated for forsterite (the most common form of olivine) for three different diameters, <inline-formula><mml:math id="M104" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M105" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 1.72 <inline-formula><mml:math id="M106" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M107" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M108" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 2.58 <inline-formula><mml:math id="M109" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, and <inline-formula><mml:math id="M110" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M111" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 3.44 <inline-formula><mml:math id="M112" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> (hereafter rounded to 1.7, 2.6, and 3.4 <inline-formula><mml:math id="M113" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> for better readability), with environmental conditions from GFDL ESM2M. The three diameters were selected to show the transition from shallow to deep particle penetration depth. <inline-formula><mml:math id="M114" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is calculated for each vertical column of the ocean model grid separately, based on temporally averaged temperature and pH profiles over the period 2016–2025 and for five initial-condition ensemble members (50 years in total). The period 2016–2025, extending an emission-driven historical simulation <xref ref-type="bibr" rid="bib1.bibx26" id="paren.25"/>, is forced with Global Carbon Budget <inline-formula><mml:math id="M115" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> emissions over 2016–2020 extended with NDCs for 2021–2025 <xref ref-type="bibr" rid="bib1.bibx14" id="paren.26"/>, and non-<inline-formula><mml:math id="M116" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> forcing as well as land use changes prescribed from RCP2.6 <xref ref-type="bibr" rid="bib1.bibx43" id="paren.27"/>. Since <inline-formula><mml:math id="M117" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is determined in a fixed time-period, the impact of climate change on the dissolution profiles is not considered here. We take the area-normalized dissolution rate of forsterite for geometric surfaces as a function of temperature and pH from <xref ref-type="bibr" rid="bib1.bibx36" id="text.28"/>, also validated in <xref ref-type="bibr" rid="bib1.bibx32" id="text.29"/> and <xref ref-type="bibr" rid="bib1.bibx15" id="text.30"/> (see Appendix Fig. <xref ref-type="fig" rid="FA3"/>). Dynamic seawater viscosity as a function of temperature is interpolated from the tabulated data in <xref ref-type="bibr" rid="bib1.bibx41" id="text.31"/>. Forsterite density is taken from <xref ref-type="bibr" rid="bib1.bibx1" id="text.32"/> and seawater density is set to global surface ocean conditions of <inline-formula><mml:math id="M118" display="inline"><mml:mi>T</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M119" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 18 <inline-formula><mml:math id="M120" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">°</mml:mi><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M121" display="inline"><mml:mi>S</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M122" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 35 <inline-formula><mml:math id="M123" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">PSU</mml:mi></mml:mrow></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx41" id="paren.33"/>. Variations in seawater density are negligible for particle sinking velocity since they are small compared to the density difference between the mineral particles and seawater. Alkalinity release that is prescribed below the ocean bottom cell is added to the bottom cell.</p>
      <p id="d2e2699">Based on the spatially-varying penetration depths for the three diameters and the two alkalinity release profile types (uniform particles and exponential PSD), we run six OAE experiments with differing alkalinity release profiles in GFDL ESM2M. Following the CDRMIP protocol, alkalinity is continuously added to the global ocean between 60° S and 70° N, totaling to 0.14 <inline-formula><mml:math id="M124" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">Pmol</mml:mi></mml:mrow></mml:math></inline-formula> alkalinity per year <xref ref-type="bibr" rid="bib1.bibx23" id="paren.34"/>. For each of the six OAE experiments, GFDL ESM2M is run over the period 2026–2200, under a <inline-formula><mml:math id="M125" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> emission trajectory that stabilizes at 2 <inline-formula><mml:math id="M126" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">°</mml:mi><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula> global warming relative to the preindustrial period in absence of OAE <xref ref-type="bibr" rid="bib1.bibx40 bib1.bibx39" id="paren.35"><named-content content-type="pre">based on the AERA protocol;</named-content></xref>. These six simulations are compared to a simulation where alkalinity is added at the ocean surface. For the uniform alkalinity release profiles with <inline-formula><mml:math id="M127" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M128" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 2.6 <inline-formula><mml:math id="M129" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M130" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M131" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 3.4 <inline-formula><mml:math id="M132" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> and for surface alkalinity addition, we ran four additional ensemble members for the period 2026–2035 to analyze the role of internal variability over the first 10 years of OAE. All simulations are run with interactive atmospheric <inline-formula><mml:math id="M133" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> rather than prescribed concentrations. Thus, the OAE efficiency; calculated as the difference in air-sea carbon uptake between the OAE experiment and the baseline simulation without OAE divided by the alkalinity addition; includes carbon cycle feedbacks between the ocean, atmosphere, and land biosphere. This net ocean capture efficiency including the carbon cycle feedbacks is lower than the gross efficiency, which is calculated without the adjustments in natural carbon reservoirs <xref ref-type="bibr" rid="bib1.bibx17" id="paren.36"/>. The net efficiency is relevant for studying the carbon, climate and ocean acidification responses to OAE, while the gross efficiency characterizes the negative emissions due to OAE, thus important for emission budgets and carbon credits.</p>

      <fig id="F2" specific-use="star"><label>Figure 2</label><caption><p id="d2e2806">Regional variation in penetration depth and mixed layer alkalinity release for particle diameters <inline-formula><mml:math id="M134" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M135" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 1.7 <inline-formula><mml:math id="M136" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> (left column), <inline-formula><mml:math id="M137" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M138" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 2.6 <inline-formula><mml:math id="M139" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> (middle column), and <inline-formula><mml:math id="M140" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M141" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 3.4 <inline-formula><mml:math id="M142" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> (right column). <bold>(a–c)</bold> Penetration depth determined with temperature and pH data from GFDL ESM2M over the period 2016–2025 (see Sects. <xref ref-type="sec" rid="Ch1.S2.SS3"/> and <xref ref-type="sec" rid="Ch1.S2.SS4"/>). The fraction of alkalinity released above the annual maximum mixed layer depth (<inline-formula><mml:math id="M143" display="inline"><mml:mi mathvariant="italic">χ</mml:mi></mml:math></inline-formula>) for uniform particle profiles are shown in panels <bold>(d–f)</bold> and those for exponential particle size distribution profiles in panels <bold>(g-i)</bold> for each penetration depth. The gray dashed lines enclose the region between 60° S and 70° N, where alkaline minerals are added to the surface ocean in this study.</p></caption>
          <graphic xlink:href="https://bg.copernicus.org/articles/23/3279/2026/bg-23-3279-2026-f02.png"/>

        </fig>

</sec>
</sec>
<sec id="Ch1.S3">
  <label>3</label><title>Results</title>
<sec id="Ch1.S3.SS1">
  <label>3.1</label><title>Regional variation in alkalinity release</title>
      <p id="d2e2925">The penetration depth <inline-formula><mml:math id="M144" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, calculated from Eqs. (<xref ref-type="disp-formula" rid="Ch1.E5"/>) and (<xref ref-type="disp-formula" rid="Ch1.E12"/>), increases strongly with particle size (Fig. <xref ref-type="fig" rid="F2"/>a–c). Globally averaged, <inline-formula><mml:math id="M145" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> values are 165 <inline-formula><mml:math id="M146" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, 638 <inline-formula><mml:math id="M147" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, and 1945 <inline-formula><mml:math id="M148" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> for particle diameters of <inline-formula><mml:math id="M149" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M150" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 1.7 <inline-formula><mml:math id="M151" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M152" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M153" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 2.6 <inline-formula><mml:math id="M154" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, and <inline-formula><mml:math id="M155" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M156" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 3.4 <inline-formula><mml:math id="M157" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, respectively. Thus, doubling the diameter from <inline-formula><mml:math id="M158" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M159" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 1.7 <inline-formula><mml:math id="M160" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M161" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M162" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 3.4 <inline-formula><mml:math id="M163" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> increases <inline-formula><mml:math id="M164" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> by about a factor of twelve. Under constant environmental conditions, Eq. (<xref ref-type="disp-formula" rid="Ch1.E5"/>) predicts a scaling of <inline-formula><mml:math id="M165" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mo>∝</mml:mo><mml:msup><mml:mi>d</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula>, corresponding to an eightfold increase. The stronger increase in <inline-formula><mml:math id="M166" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> arises from overall cooler conditions experienced by larger particles that sink deeper into the water column as discussed in Sect. <xref ref-type="sec" rid="Ch1.S2.SS3"/>.</p>
      <p id="d2e3148">The penetration depth shows a pronounced latitudinal gradient (Fig. <xref ref-type="fig" rid="F2"/>a–c). It is substantially greater at high latitudes than at low latitudes. For example, for <inline-formula><mml:math id="M167" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M168" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 2.6 <inline-formula><mml:math id="M169" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, the average penetration depth increases from 367 <inline-formula><mml:math id="M170" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> in the tropics (10° S–10° N) to 1043 <inline-formula><mml:math id="M171" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> in the Southern Ocean (60 to 45° S). This pattern arises primarily from lower water temperatures in high latitude regions, which suppress mineral dissolution rates and thereby increase penetration depth. The effect of reduced dissolution is partially counteracted by the higher viscosity of colder waters, which slows particle sinking and limits penetration. However, the change in dissolution rate with temperature dominates: a 1 <inline-formula><mml:math id="M172" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">°</mml:mi><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula> cooling at 18 <inline-formula><mml:math id="M173" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">°</mml:mi><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula> results in a 9.2 % decrease in area-normalized dissolution rate, whereas viscosity only increases by 2.6 %. Latitudinal variations in pH exert a negligible impact on mineral dissolution rate (Appendix Fig. <xref ref-type="fig" rid="FA3"/>). Even variations in pH of <inline-formula><mml:math id="M174" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1 alter <inline-formula><mml:math id="M175" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> by only a few meters.</p>
      <p id="d2e3234">Based on these penetration depths, the fraction of alkalinity released within the annual maximum mixed layer can be calculated (Sect. <xref ref-type="sec" rid="Ch1.S2.SS2"/>, Fig. <xref ref-type="fig" rid="F2"/>d–i). Because waters above the annual maximum <inline-formula><mml:math id="M176" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow></mml:math></inline-formula> are well ventilated, alkalinity released in this layer directly contributes to oceanic carbon uptake. The fraction of alkalinity released in the mixed layer decreases with increasing particle size and is larger for the uniform particle profile than for the exponential profile, as larger particles in the latter are exported to greater depths. Globally, uniform particles with <inline-formula><mml:math id="M177" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M178" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 1.7 <inline-formula><mml:math id="M179" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> release 72 % of their alkalinity within the annual maximum mixed layer (Fig. <xref ref-type="fig" rid="F2"/>d), compared to 52 % for the exponential PSD profile with the same mean volume diameter (Fig. <xref ref-type="fig" rid="F2"/>g). Increasing the (mean volume) diameter to <inline-formula><mml:math id="M180" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M181" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 2.6 <inline-formula><mml:math id="M182" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> lowers the fraction to 20 % and 18 % for the uniform and exponential profile, respectively, and further to 6 % for both profiles at <inline-formula><mml:math id="M183" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M184" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 3.4 <inline-formula><mml:math id="M185" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>. For large diameters, the penetration depth is often much larger than the mixed layer depth and the alkalinity release within the mixed layer between profiles is similar, because: <inline-formula><mml:math id="M186" display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>-</mml:mo><mml:mi>exp⁡</mml:mi><mml:mo>(</mml:mo><mml:mo>-</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow><mml:mo>/</mml:mo><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mo>)</mml:mo><mml:mo>≈</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow><mml:mo>/</mml:mo><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> for <inline-formula><mml:math id="M187" display="inline"><mml:mrow><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow><mml:mo>/</mml:mo><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mo>≪</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula>.</p>

      <fig id="F3" specific-use="star"><label>Figure 3</label><caption><p id="d2e3391"><bold>(a)</bold> Global mean difference in total alkalinity between the OAE simulations (surface dissolution and uniform as well as exponentially distributed particle size distributions) and the baseline simulation without OAE, averaged over 2026–2200. The horizontal gray lines indicate the global mean penetration depths <inline-formula><mml:math id="M188" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> for the three particle diameters 1.7, 2.6, and 3.4 <inline-formula><mml:math id="M189" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>. <bold>(b)</bold> The OAE efficiency for these simulations over time, defined as the number of moles of additional carbon uptake in the OAE simulations divided by the number of moles alkalinity added. The lines show 31 year running means. The dots indicate averages over the first 10 years of the experiment, with open dots for the PSD experiments. For surface dissolution and the 2.6 and 3.4 <inline-formula><mml:math id="M190" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> uniform cases, the five-member ensemble ranges and ensemble means shown.</p></caption>
          <graphic xlink:href="https://bg.copernicus.org/articles/23/3279/2026/bg-23-3279-2026-f03.png"/>

        </fig>

      <p id="d2e3436">Regionally, alkalinity release in the mixed layer is large either where penetration depths are shallow (low to mid-latitudes; Fig. <xref ref-type="fig" rid="F2"/>a–c) or where mixed layers are deep (e.g., western boundary current extension in the North Atlantic and North Pacific, the mode water formation regions of the Southern Ocean, and deep convection zones in the North Atlantic and Weddell Sea; Appendix Fig. <xref ref-type="fig" rid="FA4"/>). Since regions are often either warm, associated with shallow penetration depths, or have deep mixed layers, the latitudinal gradients of alkalinity release in the mixed layer are relatively small. For example, uniform particles with <inline-formula><mml:math id="M191" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M192" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 2.6 <inline-formula><mml:math id="M193" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> release 14 % of their alkalinity in the mixed layer in the tropics (10° S–10° N) and 20 % in the Southern Ocean (60 to 45° S).</p>
</sec>
<sec id="Ch1.S3.SS2">
  <label>3.2</label><title>Ocean carbon uptake and efficiency</title>
      <p id="d2e3475">Each profile type (uniform and exponential PSD) and particle size results in a characteristic vertical distribution of additional alkalinity relative to the reference simulation without OAE (Fig. <xref ref-type="fig" rid="F3"/>a, Appendix Fig. <xref ref-type="fig" rid="FA5"/>). Averaged over 2026–2200, the additional alkalinity profile of the smallest mean volume diameter <inline-formula><mml:math id="M194" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M195" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 1.7 <inline-formula><mml:math id="M196" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> closely resembles that from surface dissolution, with only slightly lower concentrations close to the surface (57 <inline-formula><mml:math id="M197" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">kg</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> for surface dissolution vs. 55 and 52 <inline-formula><mml:math id="M198" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">kg</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> for the uniform and exponential PSD profiles, respectively). With increasing particle diameter, additional alkalinity accumulates at larger depths. This is particularly the case for the exponential PSD profile, where 37 % of the alkalinity is released below <inline-formula><mml:math id="M199" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> compared to no release below <inline-formula><mml:math id="M200" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> for the uniform profile (global mean values for <inline-formula><mml:math id="M201" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> are shown as dashed lines in Fig. <xref ref-type="fig" rid="F3"/>a). As a result, additional alkalinity near the surface declines. For <inline-formula><mml:math id="M202" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M203" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 3.4 <inline-formula><mml:math id="M204" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, additional surface alkalinity reduces to 21 and 18 <inline-formula><mml:math id="M205" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">kg</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> for the uniform and exponential PSD profiles, respectively.</p>
      <p id="d2e3624">Relative to surface alkalinity release, this deeper alkalinity release reduces OAE capture efficiency, defined as the ratio of additional carbon uptake to the alkalinity added (Fig. <xref ref-type="fig" rid="F3"/>b). The reduction is most pronounced in the first decades of continuous alkalinity addition. Over the first 30 years, efficiency decreases by more than two thirds for <inline-formula><mml:math id="M206" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M207" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 3.4 <inline-formula><mml:math id="M208" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, to 0.20 and 0.18 <inline-formula><mml:math id="M209" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi>C</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>(</mml:mo><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi>A</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:msup><mml:mo>)</mml:mo><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> for the uniform and exponential PSD profiles, respectively, compared to 0.65 <inline-formula><mml:math id="M210" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi>C</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>(</mml:mo><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi>A</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:msup><mml:mo>)</mml:mo><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> for surface dissolution and alkalinity release. For reference, an efficiency of 0.65 <inline-formula><mml:math id="M211" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi>C</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>(</mml:mo><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi>A</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:msup><mml:mo>)</mml:mo><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> corresponds to an uptake of 0.81 Gt <inline-formula><mml:math id="M212" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> per Gt forsterite. For the intermediate mean volume diameter <inline-formula><mml:math id="M213" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M214" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 2.6 <inline-formula><mml:math id="M215" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, efficiency is reduced to 0.44 <inline-formula><mml:math id="M216" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi>C</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>(</mml:mo><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi>A</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:msup><mml:mo>)</mml:mo><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> (<inline-formula><mml:math id="M217" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>32 %) and 0.39 <inline-formula><mml:math id="M218" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi>C</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>(</mml:mo><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi>A</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:msup><mml:mo>)</mml:mo><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>(<inline-formula><mml:math id="M219" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>40 %) for the uniform and exponential PSD profiles, respectively. For the exponential PSD profile with the smallest mean volume diameter <inline-formula><mml:math id="M220" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M221" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 1.7 <inline-formula><mml:math id="M222" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, we find a 16 % decrease in efficiency to 0.54 <inline-formula><mml:math id="M223" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi>C</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>(</mml:mo><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi>A</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:msup><mml:mo>)</mml:mo><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>. Efficiency is further reduced during the first decade with 0.32 and 0.14 mol C<sub>T</sub> (mol A<sub>T</sub>)<sup>−1</sup> for uniform particles with <inline-formula><mml:math id="M225" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M226" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 2.6 and 3.4 <inline-formula><mml:math id="M227" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, respectively, compared to 0.65 <inline-formula><mml:math id="M228" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi>C</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>(</mml:mo><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi>A</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:msup><mml:mo>)</mml:mo><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> for surface dissolution (on ensemble mean, ensemble ranges are shown in Fig. <xref ref-type="fig" rid="F3"/>b). As such, efficiency decreases by more than 75 % over the first 10 years for particles with 3.4 <inline-formula><mml:math id="M229" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> diameter. We also find a reduced efficiency of 0.47 <inline-formula><mml:math id="M230" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi>C</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>(</mml:mo><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi>A</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:msup><mml:mo>)</mml:mo><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> (<inline-formula><mml:math id="M231" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>27 %) for uniform particles with <inline-formula><mml:math id="M232" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M233" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 1.7 <inline-formula><mml:math id="M234" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> during the first decade.</p>

      <fig id="F4" specific-use="star"><label>Figure 4</label><caption><p id="d2e4082">Regional carbon uptake for the OAE experiment with uniform particles of diameter <inline-formula><mml:math id="M235" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M236" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 2.6 <inline-formula><mml:math id="M237" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> relative to the baseline simulation without ocean alkalinity enhancement over <bold>(a)</bold> the first 10 years (2026–2035), averaged over five ensemble members to increase robustness, and <bold>(b)</bold> over the full simulation (2026–2200). The difference between the carbon uptake for this uniform particle size and that for surface alkalinity addition is shown in panels <bold>(c)</bold> for the first 10 years and <bold>(d)</bold> for the full period.</p></caption>
          <graphic xlink:href="https://bg.copernicus.org/articles/23/3279/2026/bg-23-3279-2026-f04.png"/>

        </fig>

      <p id="d2e4129">Over time, the difference in efficiency relative to surface alkalinity release decreases, reflecting the gradual transport of alkalinity released at depth back to the surface. Nevertheless, the average efficiency over 2026–2200 remains less than half of that of surface addition for <inline-formula><mml:math id="M238" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M239" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 3.4 <inline-formula><mml:math id="M240" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> (0.29 and 0.25 <inline-formula><mml:math id="M241" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi>C</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>(</mml:mo><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi>A</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:msup><mml:mo>)</mml:mo><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, respectively, compared to 0.60 <inline-formula><mml:math id="M242" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi>C</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>(</mml:mo><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi>A</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:msup><mml:mo>)</mml:mo><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>). Year-to-year variability in OAE efficiency is substantial in all experiments (standard deviation around 0.18 <inline-formula><mml:math id="M243" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi>C</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>(</mml:mo><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi>A</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:msup><mml:mo>)</mml:mo><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>). These strong fluctuations in carbon uptake mainly arise because we run the experiments in a fully coupled Earth system model, where natural variations in air-sea <inline-formula><mml:math id="M244" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> flux in the OAE experiment and the baseline simulation are superimposed onto the carbon uptake signal from OAE. For larger particle sizes, the standard deviation of OAE efficiency approaches mean efficiency (coefficients of variation are 0.56 and 0.72 for the uniform and exponential PSD profiles with <inline-formula><mml:math id="M245" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M246" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 3.4 <inline-formula><mml:math id="M247" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>). Thus, the OAE carbon uptake signal is less significant compared to flux variability when alkalinity is released from larger particles.</p>
      <p id="d2e4291">During the first 10 years of alkalinity addition, OAE with vertical alkalinity release profiles results in additional carbon uptake over most of the ocean (see Fig. <xref ref-type="fig" rid="F4"/>a for the additional <inline-formula><mml:math id="M248" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> uptake for uniform particles with diameter <inline-formula><mml:math id="M249" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M250" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 2.6 <inline-formula><mml:math id="M251" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>). However, carbon uptake and efficiency are generally lower than when alkalinity is released directly at the surface (Fig. <xref ref-type="fig" rid="F4"/>c). As expected, regions with particularly low alkalinity release in the mixed layer (Fig. <xref ref-type="fig" rid="F2"/>e) partially overlap with regions of low carbon uptake (Fig. <xref ref-type="fig" rid="F4"/>a), such as in the northern and eastern North Pacific or the Atlantic section of the Southern Ocean. Carbon uptake is higher in the Kuroshio current extension, the Gulf Stream region in the North Atlantic, and mode water source regions in the Southern Ocean, where the fraction of alkalinity release in the mixed layer is also relatively high. However, despite relatively low alkalinity release in the mixed layer, the tropical upwelling regions show considerable carbon uptake, which may indicate the upwelling of alkalinity back to the surface. Overall, the fraction of alkalinity release in the annual maximum mixed layer only partially explains the regional variations in carbon uptake even on short timescales such as 10 years. The pattern correlation between the fraction of alkalinity release in the mixed layer and OAE-induced carbon uptake for <inline-formula><mml:math id="M252" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M253" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 2.6 <inline-formula><mml:math id="M254" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> particles, averaged over the 5 ensemble members, is only 0.34 between 60° S and 70° N. However, the carbon uptake pattern also varies strongly among the five ensemble members. We analyze this by calculating the pattern correlation coefficients between the carbon uptake patterns of the different ensemble members over the first 10 years of experiment. The mean of the ten pairwise pattern correlation coefficients across the five ensemble members is 0.15 and 0.37 for uniform <inline-formula><mml:math id="M255" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M256" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 3.4 <inline-formula><mml:math id="M257" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M258" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M259" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 2.6 <inline-formula><mml:math id="M260" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> particles, respectively. As such, regional carbon uptake is more uncertain for larger particles where alkalinity is released deeper in the water column.</p>
      <p id="d2e4411">At longer timescales, ocean carbon uptake increases in regions with deep mixed layers (cf. Fig. <xref ref-type="fig" rid="F4"/>b and Appendix Fig. <xref ref-type="fig" rid="FA4"/>), in the upwelling region of the tropical Pacific, as well as in Eastern Boundary upwelling systems (Fig. <xref ref-type="fig" rid="F4"/>b). The increase in carbon uptake in these regions suggests that additional alkalinity released at subsurface in other regions is transported there, where it comes in contact with the atmosphere. In the eastern and central equatorial Pacific, for example, we find a distinct buildup of alkalinity in the upper 1000 m, likely due to an inflow of alkalinity from North and South of the equator (Appendix Fig. <xref ref-type="fig" rid="FA5"/>f). As these waters with additional alkalinity have not yet equilibrated with the atmosphere, additional carbon is taken up. As a result, carbon uptake becomes larger than in the simulation with direct alkalinity addition at the surface in these regions (Fig. <xref ref-type="fig" rid="F4"/>d). Increased carbon uptake is also observed south of 60° S where no alkalinity is added, indicating an increased southward transport of alkalinity from regions north of 60° S when alkalinity is released at subsurface.  Yet, carbon uptake remains lower over most of the low-to-mid latitudes, such that global carbon uptake remains 16 % lower than when alkalinity is added to the surface (Fig. <xref ref-type="fig" rid="F3"/>b).</p>
</sec>
</sec>
<sec id="Ch1.S4" sec-type="conclusions">
  <label>4</label><title>Discussion</title>
<sec id="Ch1.S4.SS1">
  <label>4.1</label><title>Comparison to earlier studies</title>
      <p id="d2e4443">Our study suggests a shallower release of alkalinity compared to <xref ref-type="bibr" rid="bib1.bibx25" id="text.37"/>, who estimated that about 80 % of alkalinity from forsterite olivine particles with a 1 <inline-formula><mml:math id="M261" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> diameter is released within the maximum mixed layer. Repeating the analysis from Sect. <xref ref-type="sec" rid="Ch1.S3.SS1"/> for particles of 1 <inline-formula><mml:math id="M262" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> diameter, we find a release of 98 % in the annual maximum mixed layer. The shallower release of alkalinity in our study primarily arises from the higher area-normalized dissolution rate adopted here, based on geometric surfaces from <xref ref-type="bibr" rid="bib1.bibx36" id="text.38"/>. For example, the dissolution rate is 84 % higher at 25  <inline-formula><mml:math id="M263" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">°</mml:mi><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula> than the rate from <xref ref-type="bibr" rid="bib1.bibx19" id="text.39"/> used in <xref ref-type="bibr" rid="bib1.bibx25" id="text.40"/>. A secondary contribution stems from the deeper maximum <inline-formula><mml:math id="M264" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">MLD</mml:mi></mml:mrow></mml:math></inline-formula> in our model, 123 <inline-formula><mml:math id="M265" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> on global average <xref ref-type="bibr" rid="bib1.bibx9" id="paren.41"><named-content content-type="pre">34 <inline-formula><mml:math id="M266" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> deeper than observations;</named-content></xref>, compared to 64 <inline-formula><mml:math id="M267" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> in <xref ref-type="bibr" rid="bib1.bibx25" id="text.42"/>. As the dissolution rate from <xref ref-type="bibr" rid="bib1.bibx36" id="text.43"/> has been validated against observations in multiple studies <xref ref-type="bibr" rid="bib1.bibx32" id="paren.44"/>, the mixed layer alkalinity release fractions obtained here are likely more robust. Nonetheless, the comparison underscores the strong sensitivity of vertical alkalinity release to the assumed mineral dissolution rate. Despite the shallower release, the spatial patterns of mixed layer alkalinity release are broadly consistent with those of <xref ref-type="bibr" rid="bib1.bibx25" id="text.45"/> (cf. Fig. <xref ref-type="fig" rid="F2"/> and their Fig. 3d).</p>
      <p id="d2e4543">Our results are also qualitatively consistent with <xref ref-type="bibr" rid="bib1.bibx11" id="text.46"/>, who modeled alkalinity release using a more complex mineral particle model that includes particle aggregation and zooplankton interaction. Their study employed an experimental PSD from <xref ref-type="bibr" rid="bib1.bibx34" id="text.47"/>, in which 80 % of particle mass is contained in particles smaller than 10 <inline-formula><mml:math id="M268" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> in diameter. To enable comparison, we discretize the experimental PSD into 14 discrete size classes and convert the experimentally determined mass fractions per size class into particle number fractions (see Appendix Sect. <xref ref-type="sec" rid="App1.Ch1.S1"/> and Fig. <xref ref-type="fig" rid="FA7"/>a). The resulting cumulative alkalinity release profiles (Fig. <xref ref-type="fig" rid="FA7"/>b) are qualitatively similar to those reported by <xref ref-type="bibr" rid="bib1.bibx11" id="text.48"/> though our model predicts a shallower release. While <xref ref-type="bibr" rid="bib1.bibx11" id="text.49"/> found 25 % to 45 % of alkalinity release in the upper 80 <inline-formula><mml:math id="M269" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, with increased release for higher feedstock application rates where aggregates are less likely packed into zooplankton fecal pellets, we obtain 54 % to 61 % for temperatures of 10 to 25 <inline-formula><mml:math id="M270" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">°</mml:mi><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>. This difference suggests that including particle aggregation and zooplankton ingestion, as in <xref ref-type="bibr" rid="bib1.bibx11" id="text.50"/>, may further reduce the efficiency of olivine-based ocean alkalinity enhancement by enhancing particle settling velocities.</p>
</sec>
<sec id="Ch1.S4.SS2">
  <label>4.2</label><title>Limitations of the analytical shrinking core treatment of mineral particles</title>
      <p id="d2e4604">The analytical framework presented here involves several simplifying assumptions. The main limitations include (i) the idealized representation of particle geometry and sinking, (ii) the omission of particle interactions with the environment such as aggregation, scavenging, or the formation of coating layers, (iii) the use of mean rather than depth-resolved environmental conditions, and (iv) the omission of particle advection during dissolution.</p>
      <p id="d2e4607">First, the shrinking core model assumes smooth, spherical particles. We use an area-normalized dissolution rate determined for geometric spherical particles with equivalent diameters determined by sieving the mineral grains <xref ref-type="bibr" rid="bib1.bibx36" id="paren.51"/>. The particles' sinking velocity, on the other hand, is characterized by the equivalent diameter from Stokes settling. While the two equivalent diameters are often similar <xref ref-type="bibr" rid="bib1.bibx46" id="paren.52"/>, implying that the treatment of dissolution and sinking in our study is consistent, this may not always be the case. When the two equivalent diameters diverge, one cannot assign a single equivalent spherical diameter to a mineral particle that is representative for both dissolution and sinking as assumed in our alkalinity release profiles. Additionally, when mineral particles are added over a small area such that high mineral particle concentrations near 15 <inline-formula><mml:math id="M271" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">g</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">L</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> are reached, fluid instabilities may considerably enhance the sinking velocity <xref ref-type="bibr" rid="bib1.bibx47 bib1.bibx48" id="paren.53"/>. While such mineral particle concentrations in the mixed layer are not reached in our idealized global experiments, where only 15 <inline-formula><mml:math id="M272" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">g</mml:mi></mml:mrow></mml:math></inline-formula> olivine per square meter and year are added, instabilities may occur in more realistic localized application schemes.</p>
      <p id="d2e4644">Second, we also neglect potential particle interactions with the environment. Smaller mineral particles may aggregate, forming larger particles that sink faster <xref ref-type="bibr" rid="bib1.bibx25" id="paren.54"/>. Mineral particles may also attach to biogenic particles through scavenging or zooplankton ingestion, suppressing near-surface alkalinity release <xref ref-type="bibr" rid="bib1.bibx11" id="paren.55"/>. Mineral or microbial coating layers may form on the particles' surfaces <xref ref-type="bibr" rid="bib1.bibx44 bib1.bibx32" id="paren.56"/>, which can reduce the contact area with the surrounding water and mineral dissolution.</p>
      <p id="d2e4656">Third, to obtain analytical alkalinity release profiles, we assume that dissolution occurs at the mean temperature and pH between surface and penetration depth <inline-formula><mml:math id="M273" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> (Sect. <xref ref-type="sec" rid="Ch1.S2.SS3"/>). This simplification neglects vertical and seasonal gradients that could enhance dissolution in warmer surface waters and reduce it at depth. The approximation performs best where such gradients are small (e.g., at high latitudes or for shallow-sinking particles). For instance, in a subtropical Atlantic column with a 9.2 <inline-formula><mml:math id="M274" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">°</mml:mi><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula> temperature range between surface and a particle's penetration depth of 300 <inline-formula><mml:math id="M275" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, surface alkalinity release is 27 % higher and deep release is 28 % lower than predicted using mean conditions, whereas in the Southern Ocean (1.8 <inline-formula><mml:math id="M276" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">°</mml:mi><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula> range) the differences are only 9 % and 2 %, respectively (Fig. <xref ref-type="fig" rid="FA6"/>a,b). The stronger mismatch at low latitudes thus reflects the larger vertical temperature contrast.  The use of mean environmental conditions to determine a particle’s penetration depth also neglects the nonlinear dependence of dissolution rate on temperature and pH <xref ref-type="bibr" rid="bib1.bibx36" id="paren.57"/>. Because the dissolution rate is a convex function of these variables, the rate at vertically averaged conditions is slightly lower than the average rate computed over the full profile, resulting in a deeper predicted penetration depth. This effect is generally small: across the global ocean, penetration depths differ by less than 10 % over 90 % of the area for 2.6 <inline-formula><mml:math id="M277" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> particles (Fig. <xref ref-type="fig" rid="FA6"/>d). For these particles, explicit profiles yield a globally averaged penetration depth that is only 14 <inline-formula><mml:math id="M278" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> shallower than the idealized case, though mixed-layer release fractions increase by about 6 % (a relative rise of 28 %, Fig. <xref ref-type="fig" rid="FA6"/>f). Hence, while vertically resolved profiles yield higher surface release, the idealized treatment remains a good first-order approximation.  For the exponential PSD profile, we also assume that all particle sizes experience identical mean temperature and pH, although larger particles typically penetrate into colder, more acidic waters than smaller ones. Accounting for these variations would increase the spread in penetration depth across the PSD, resulting in a deeper alkalinity export for larger particles.</p>
      <p id="d2e4729">Fourth, the present framework neglects the horizontal and vertical advection of mineral particles during dissolution. Because dissolution can span several years (Appendix Fig. <xref ref-type="fig" rid="FA2"/>a), advection of mineral particles in the subsurface may modify the depth and spatial patterns of alkalinity release. This aspect should be assessed in subsequent studies.</p>
      <p id="d2e4734">Overall, these simplifications may lead to a modest underestimation of mineral export and deep alkalinity release, primarily due to the omission of particle aggregation. Nevertheless, the simplified vertical profiles developed here capture the first-order effects of environmental conditions and feedstock properties on alkalinity release, providing a robust basis for sensitivity analyses of ocean alkalinity enhancement efficiency.</p>
</sec>
<sec id="Ch1.S4.SS3">
  <label>4.3</label><title>Implications for feasibility of open-ocean mineral-based OAE</title>
      <p id="d2e4745">Our study confirms that olivine must be milled to grain sizes near 1 <inline-formula><mml:math id="M279" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> to achieve feasible carbon removal through open-ocean alkalinity enhancement <xref ref-type="bibr" rid="bib1.bibx25 bib1.bibx3" id="paren.58"/>. When particles are uniformly milled to a diameter of 1.7 <inline-formula><mml:math id="M280" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, carbon capture efficiency is reduced over the first decade but comparable to that of instantaneous surface dissolution on longer timescales. In contrast, doubling the diameter to 3.4 <inline-formula><mml:math id="M281" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> reduces the efficiency to less than one third within the first decades.</p>
      <p id="d2e4781">Olivine powder with an exponential PSD at a mean volume diameter of 1.7 <inline-formula><mml:math id="M282" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> marks a transition between near-optimal and considerably reduced capture efficiency. In this case, efficiency is 16 % lower than with direct surface alkalinity addition over the first 3 decades, with full efficiency reached only by the end of the 21st century (Fig. <xref ref-type="fig" rid="F3"/>b). These long timescales until full efficiency result from an overproportionally larger fraction of alkalinity stored in the larger particles that sink deeper. While 80 % of particles are smaller than 2 <inline-formula><mml:math id="M283" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, they only contain 48 % of the alkalinity. In contrast, the largest 0.3 % of particles in the PSD, exceeding 3.1 <inline-formula><mml:math id="M284" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, still contain 2 % of the alkalinity. In natural or industrially milled powders, more heavy-tailed PSDs can further exacerbate this problem. For example, in the experimental PSD from <xref ref-type="bibr" rid="bib1.bibx34" id="text.59"/>, 73 % of the alkalinity resides in the largest 0.3 % of particles, resembling a power law distribution (Fig. <xref ref-type="fig" rid="FA7"/>a). For this heavy-tailed PSD, 20 % of the alkalinity is contained in particles with diameters larger than 10 <inline-formula><mml:math id="M285" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, compared to only 2.5 <inline-formula><mml:math id="M286" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> for the exponential PSD, despite a smaller mean particle volume in the experimental PSD. Thus, beyond minimizing mean volume diameter, achieving a rapid decay of particle abundance at larger sizes is essential for efficient OAE. As such, separating and regrinding the largest particles in the mineral powder would, if possible, improve OAE efficiency.</p>
      <p id="d2e4842">The strong dependence of carbon capture efficiency on the particle size distribution makes particle comminution to grain sizes near 1 <inline-formula><mml:math id="M287" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> for olivine-based open-ocean OAE imperative. However, grinding olivine to such fine grain sizes strongly increases energy demand and associated costs and emissions. <xref ref-type="bibr" rid="bib1.bibx13" id="text.60"/> estimated <inline-formula><mml:math id="M288" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> emissions to increase from 0.04 <inline-formula><mml:math id="M289" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">t</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>(</mml:mo><mml:mn mathvariant="normal">1.25</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi mathvariant="normal">t</mml:mi><mml:mspace width="0.25em" linebreak="nobreak"/><mml:mi mathvariant="normal">olivine</mml:mi><mml:msup><mml:mo>)</mml:mo><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> for 10 <inline-formula><mml:math id="M290" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> particles to about 0.21 <inline-formula><mml:math id="M291" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">t</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>(</mml:mo><mml:mn mathvariant="normal">1.25</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi mathvariant="normal">t</mml:mi><mml:mspace width="0.25em" linebreak="nobreak"/><mml:mi mathvariant="normal">olivine</mml:mi><mml:msup><mml:mo>)</mml:mo><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> for 1 <inline-formula><mml:math id="M292" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> particles from comminution alone, translating to reductions in OAE capture efficiency by 0.03 and 0.13 <inline-formula><mml:math id="M293" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi mathvariant="normal">C</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>(</mml:mo><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi>A</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:msup><mml:mo>)</mml:mo><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, respectively. Additionally, such fine olivine powders may increase particle aggregation <xref ref-type="bibr" rid="bib1.bibx25" id="paren.61"/>, negatively impact zooplankton <xref ref-type="bibr" rid="bib1.bibx11" id="paren.62"/>, and pose risks to human health <xref ref-type="bibr" rid="bib1.bibx7" id="paren.63"/>. These problems with olivine grain sizes near 1 <inline-formula><mml:math id="M294" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> call into question the feasibility of olivine-based OAE in the open ocean. However, olivine may remain suitable for coastal applications where the mixed layer extends to the seafloor, such that alkalinity released from coarser olivine grains in the sediments enhances carbon uptake from the atmosphere <xref ref-type="bibr" rid="bib1.bibx34 bib1.bibx27 bib1.bibx13" id="paren.64"/>. Future research should therefore focus on shallow coastal seas. The micrometer scale olivine grain size necessary for open-ocean OAE and associated high particle amounts may also impact marine ecosystems due to increases in turbidity. While no detrimental impacts were observed for coastal plankton communities with coarser olivine powder <xref ref-type="bibr" rid="bib1.bibx18" id="paren.65"/>, turbidity-associated impacts on plankton should be investigated with micrometer-scale olivine powder, and ideally also for open-ocean ecosystems.</p>
      <p id="d2e5012">Alternative alkaline materials with higher dissolution rates, such as brucite, relax the particle-size constraints. Using Eq. (<xref ref-type="disp-formula" rid="Ch1.E5"/>), one can calculate the permissible increase in particle volume for a more quickly dissolving material (indicated by primes) such that the penetration depth stays constant:

            <disp-formula id="Ch1.E13" content-type="numbered"><label>13</label><mml:math id="M295" display="block"><mml:mrow><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msubsup><mml:mi>V</mml:mi><mml:mi mathvariant="normal">d</mml:mi><mml:mo>′</mml:mo></mml:msubsup></mml:mrow><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mi mathvariant="normal">d</mml:mi></mml:msub></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msup><mml:mi>r</mml:mi><mml:mo>′</mml:mo></mml:msup></mml:mrow><mml:mi>r</mml:mi></mml:mfrac></mml:mstyle><mml:mo>⋅</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msubsup><mml:mi>V</mml:mi><mml:mtext>mol</mml:mtext><mml:mo>′</mml:mo></mml:msubsup></mml:mrow><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mtext>mol</mml:mtext></mml:msub></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>⋅</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mi mathvariant="italic">ρ</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi mathvariant="italic">ρ</mml:mi><mml:mi mathvariant="normal">w</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">ρ</mml:mi><mml:mi mathvariant="normal">p</mml:mi><mml:mo>′</mml:mo></mml:msubsup><mml:mo>-</mml:mo><mml:msub><mml:mi mathvariant="italic">ρ</mml:mi><mml:mi mathvariant="normal">w</mml:mi></mml:msub></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:math></disp-formula></p>
      <p id="d2e5101">Because brucite dissolves roughly 100 times faster than forsterite at <inline-formula><mml:math id="M296" display="inline"><mml:mi>T</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M297" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 25 <inline-formula><mml:math id="M298" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">°</mml:mi><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula> and pH <inline-formula><mml:math id="M299" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 8 <xref ref-type="bibr" rid="bib1.bibx33" id="paren.66"/>, the allowable particle volume increases by a factor of 90, corresponding to an increase in diameter by a factor of 4.5. Thus, an exponential PSD with mean volume diameter of 1.7 <inline-formula><mml:math id="M300" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> for forsterite corresponds to an equally efficient PSD with mean volume diameter of 7.7 <inline-formula><mml:math id="M301" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> for brucite. Importantly, dissolution rates of brucite have been shown to vary by orders of magnitude depending on crystalline structure <xref ref-type="bibr" rid="bib1.bibx38" id="paren.67"/>, making particle size constraints for effective brucite-based OAE in the open ocean uncertain.</p>
      <p id="d2e5162">The framework developed here can be generalized to other PSDs by deriving corresponding vertical alkalinity release profiles, as illustrated for the exponential and discrete PSDs. This approach provides a direct estimate of the alkalinity released within the mixed layer (Sect. <xref ref-type="sec" rid="Ch1.S2.SS2"/>), improving on earlier approaches assuming constant sinking velocity in the mixed layer <xref ref-type="bibr" rid="bib1.bibx35 bib1.bibx25 bib1.bibx48" id="paren.68"/>. Our Earth system model simulations indicate, however, that regional variation in oceanic carbon uptake is only partly explained by mixed-layer dissolution. The remaining differences highlight the role of ocean circulation and alkalinity redistribution, which can only be captured with ocean-biogeochemical models.</p>
      <p id="d2e5170">Such ocean-biogeochemical models are also essential for assessing how mineral OAE with subsurface alkalinity release affects ocean acidification (OA). Relative to surface dissolution, and averaged over 2026–2200, mineral OAE with an exponential PSD at a mean volume diameter of 3.4 <inline-formula><mml:math id="M302" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> results in a 0.015 unit lower pH (weaker OA mitigation) in the upper 482 <inline-formula><mml:math id="M303" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> of the water column, and a 0.015 unit higher pH (stronger OA mitigation) at greater depths (Appendix Fig. <xref ref-type="fig" rid="FA8"/>c). Notably, OA mitigation is increased below 482 <inline-formula><mml:math id="M304" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> even though the alkalinity enhancement is smaller than under surface dissolution down to 792 <inline-formula><mml:math id="M305" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> (Fig. <xref ref-type="fig" rid="F3"/>a). This occurs because waters contain lower dissolved inorganic carbon concentrations as a result of the lower ocean carbon uptake under subsurface alkalinity addition. Overall, these results indicate a downward shift in the depth of OA mitigation and an enhanced mitigation potential driven by the reduced carbon uptake and efficiency of the mineral-based OAE.</p>
</sec>
</sec>
<sec id="Ch1.S5" sec-type="conclusions">
  <label>5</label><title>Conclusions</title>
      <p id="d2e5222">In summary, the efficiency of mineral-based alkalinity enhancement in the open ocean and associated <inline-formula><mml:math id="M306" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> uptake is highly sensitive to feedstock particle-size characteristics. Insufficient comminution can substantially reduce carbon capture efficiency and delay <inline-formula><mml:math id="M307" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> uptake by decades to centuries, often shifting it far away from the deployment site. Such temporal and spatial lags complicate monitoring, reporting and verification and challenge carbon crediting schemes based on short-term removal. For olivine, required grain sizes of around 1.7 <inline-formula><mml:math id="M308" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> likely render its application in the open ocean unfeasible. More rapidly dissolving minerals may prove to be suitable for efficient alkalinity enhancement when mineral particle properties are closely controlled. Our findings emphasize the need for integrated process–energy–climate assessments to evaluate the feasibility of mineral-based alkalinity enhancement in the open ocean.</p>
</sec>

      
      </body>
    <back><app-group>

<app id="App1.Ch1.S1">
  <label>Appendix A</label><title>Alkalinity release for the experimental PSD by Renforth (2012)</title>
      <p id="d2e5268">To derive an alkalinity release profile, we first discretize the particle size distribution from Table 1 in <xref ref-type="bibr" rid="bib1.bibx34" id="text.69"/> by assuming all particles within the 14 particle size intervals to have the respective mean diameters of the intervals <inline-formula><mml:math id="M309" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mrow><mml:mi>i</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>,</mml:mo><mml:mi mathvariant="normal">…</mml:mi><mml:mn mathvariant="normal">14</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula>. We then calculate the particle volume for each size class as <inline-formula><mml:math id="M310" display="inline"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>=</mml:mo><mml:mstyle displaystyle="false"><mml:mfrac style="text"><mml:mrow><mml:mi mathvariant="italic">π</mml:mi><mml:msubsup><mml:mi>d</mml:mi><mml:mi>i</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msubsup></mml:mrow><mml:mn mathvariant="normal">6</mml:mn></mml:mfrac></mml:mstyle></mml:mrow></mml:math></inline-formula>. As a next step, the retained mass fractions <inline-formula><mml:math id="M311" display="inline"><mml:mrow><mml:msub><mml:mi>m</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> in each interval are transformed into number fractions <inline-formula><mml:math id="M312" display="inline"><mml:mrow><mml:msub><mml:mi>n</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>. The number of particles in size class <inline-formula><mml:math id="M313" display="inline"><mml:mi>i</mml:mi></mml:math></inline-formula> is given by <inline-formula><mml:math id="M314" display="inline"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mtext>tot</mml:mtext></mml:msub><mml:mo>⋅</mml:mo><mml:msub><mml:mi>m</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>/</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, with the total volume of all particles <inline-formula><mml:math id="M315" display="inline"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mtext>tot</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> and that in size class <inline-formula><mml:math id="M316" display="inline"><mml:mi>i</mml:mi></mml:math></inline-formula> given by <inline-formula><mml:math id="M317" display="inline"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mtext>tot</mml:mtext></mml:msub><mml:mo>⋅</mml:mo><mml:msub><mml:mi>m</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> when assuming constant density. The number fraction in size class <inline-formula><mml:math id="M318" display="inline"><mml:mi>i</mml:mi></mml:math></inline-formula> then follows as

          <disp-formula id="App1.Ch1.S1.Ex1"><mml:math id="M319" display="block"><mml:mrow><mml:msub><mml:mi>n</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mtext>tot</mml:mtext></mml:msub><mml:mo>⋅</mml:mo><mml:msub><mml:mi>m</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>/</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:msub><mml:mo>∑</mml:mo><mml:mi>i</mml:mi></mml:msub><mml:msub><mml:mi>V</mml:mi><mml:mtext>tot</mml:mtext></mml:msub><mml:mo>⋅</mml:mo><mml:msub><mml:mi>m</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>/</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mi>m</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>/</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:msub><mml:mo>∑</mml:mo><mml:mi>i</mml:mi></mml:msub><mml:msub><mml:mi>m</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>/</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>.</mml:mo></mml:mrow></mml:math></disp-formula></p>
      <p id="d2e5518">The probability density function for these discrete number fractions <inline-formula><mml:math id="M320" display="inline"><mml:mrow><mml:msub><mml:mi>n</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> at volumes <inline-formula><mml:math id="M321" display="inline"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is then given by

          <disp-formula id="App1.Ch1.S1.Ex2"><mml:math id="M322" display="block"><mml:mrow><mml:mi>f</mml:mi><mml:mo>(</mml:mo><mml:mi>V</mml:mi><mml:mo>)</mml:mo><mml:mo>=</mml:mo><mml:munder><mml:mo movablelimits="false">∑</mml:mo><mml:mi>i</mml:mi></mml:munder><mml:msub><mml:mi>n</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>⋅</mml:mo><mml:mi mathvariant="italic">δ</mml:mi><mml:mo>(</mml:mo><mml:mi>V</mml:mi><mml:mo>-</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>)</mml:mo><mml:mo>.</mml:mo></mml:mrow></mml:math></disp-formula></p>
      <p id="d2e5588">The mean particle volume of the distribution is calculated as <inline-formula><mml:math id="M323" display="inline"><mml:mrow><mml:mover accent="true"><mml:mi>V</mml:mi><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mo>=</mml:mo><mml:msub><mml:mo>∑</mml:mo><mml:mi>i</mml:mi></mml:msub><mml:msub><mml:mi>n</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:msub><mml:mi>V</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>. The penetration depth <inline-formula><mml:math id="M324" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, the depth at which particles with mean volume <inline-formula><mml:math id="M325" display="inline"><mml:mover accent="true"><mml:mi>V</mml:mi><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:math></inline-formula> are completely dissolved, is calculated according to Eq. (<xref ref-type="disp-formula" rid="Ch1.E5"/>). The alkalinity release profile can now be calculated as done for the exponential PSD in Eq. (<xref ref-type="disp-formula" rid="Ch1.E9"/>):

          <disp-formula id="App1.Ch1.S1.Ex3"><mml:math id="M326" display="block"><mml:mtable class="split" rowspacing="0.2ex" displaystyle="true" columnalign="right left"><mml:mtr><mml:mtd><mml:mrow><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>A</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:mo>=</mml:mo><mml:mfenced open="(" close=")"><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub><mml:mo>⋅</mml:mo><mml:munderover><mml:mo movablelimits="false">∫</mml:mo><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mtext>min</mml:mtext></mml:msub><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>)</mml:mo></mml:mrow><mml:mi mathvariant="normal">∞</mml:mi></mml:munderover><mml:mi>f</mml:mi><mml:mo>(</mml:mo><mml:mi>V</mml:mi><mml:mo>)</mml:mo><mml:mi mathvariant="normal">d</mml:mi><mml:mi>V</mml:mi></mml:mrow></mml:mfenced><mml:mo>⋅</mml:mo><mml:mfenced close=")" open="("><mml:mrow><mml:mo>-</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>z</mml:mi></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:mfenced><mml:mo>⋅</mml:mo><mml:msub><mml:mi>n</mml:mi><mml:mtext>Alk</mml:mtext></mml:msub></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><mml:mo>=</mml:mo><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub><mml:mfenced close=")" open="("><mml:mrow><mml:mo>-</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>z</mml:mi></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:mfenced><mml:mo>⋅</mml:mo><mml:msub><mml:mi>n</mml:mi><mml:mtext>Alk</mml:mtext></mml:msub><mml:mo>⋅</mml:mo><mml:munder><mml:mo movablelimits="false">∑</mml:mo><mml:mi>i</mml:mi></mml:munder><mml:msub><mml:mi>n</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:munderover><mml:mo movablelimits="false">∫</mml:mo><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mtext>min</mml:mtext></mml:msub><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>)</mml:mo></mml:mrow><mml:mi mathvariant="normal">∞</mml:mi></mml:munderover><mml:mi mathvariant="italic">δ</mml:mi><mml:mo>(</mml:mo><mml:mi>V</mml:mi><mml:mo>-</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>)</mml:mo><mml:mi mathvariant="normal">d</mml:mi><mml:mi>V</mml:mi></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><mml:mo>=</mml:mo><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub><mml:mfenced close=")" open="("><mml:mrow><mml:mo>-</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">p</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>z</mml:mi></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:mfenced><mml:mo>⋅</mml:mo><mml:msub><mml:mi>n</mml:mi><mml:mtext>Alk</mml:mtext></mml:msub><mml:mo>⋅</mml:mo><mml:munder><mml:mo movablelimits="false">∑</mml:mo><mml:mi>i</mml:mi></mml:munder><mml:msub><mml:mi>n</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mi mathvariant="italic">θ</mml:mi><mml:mo>(</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mtext>min</mml:mtext></mml:msub><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>)</mml:mo><mml:mo>)</mml:mo></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mi>F</mml:mi><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:mfrac></mml:mstyle><mml:munder><mml:mo movablelimits="false">∑</mml:mo><mml:mi>i</mml:mi></mml:munder><mml:msub><mml:mi>n</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mi mathvariant="italic">θ</mml:mi><mml:mo>(</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mtext>min</mml:mtext></mml:msub><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>)</mml:mo><mml:mo>)</mml:mo><mml:mo>,</mml:mo></mml:mrow></mml:mtd></mml:mtr></mml:mtable></mml:math></disp-formula>

        with <inline-formula><mml:math id="M327" display="inline"><mml:mi mathvariant="italic">θ</mml:mi></mml:math></inline-formula> representing the Heavyside step function (<inline-formula><mml:math id="M328" display="inline"><mml:mrow><mml:mi mathvariant="italic">θ</mml:mi><mml:mo>(</mml:mo><mml:mi>x</mml:mi><mml:mo>)</mml:mo><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0</mml:mn></mml:mrow></mml:math></inline-formula> for <inline-formula><mml:math id="M329" display="inline"><mml:mrow><mml:mi>x</mml:mi><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">0</mml:mn></mml:mrow></mml:math></inline-formula> and 1 else) and <inline-formula><mml:math id="M330" display="inline"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mtext>min</mml:mtext></mml:msub><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> the minimum initial volume of a particle to still be present at depth <inline-formula><mml:math id="M331" display="inline"><mml:mi>z</mml:mi></mml:math></inline-formula> (Eq. <xref ref-type="disp-formula" rid="Ch1.E8"/>).</p>
      <p id="d2e6022">Finally, the fraction of alkalinity release between the surface and depth <inline-formula><mml:math id="M332" display="inline"><mml:mi>z</mml:mi></mml:math></inline-formula> is calculated by integrating the alkalinity release profile and normalizing by the surface alkalinity flux (see Sect. <xref ref-type="sec" rid="Ch1.S2.SS2"/>):

          <disp-formula id="App1.Ch1.S1.Ex4"><mml:math id="M333" display="block"><mml:mtable rowspacing="0.2ex" class="split" displaystyle="true" columnalign="right left"><mml:mtr><mml:mtd><mml:mrow><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mi>F</mml:mi></mml:mfrac></mml:mstyle><mml:munderover><mml:mo movablelimits="false">∫</mml:mo><mml:mn mathvariant="normal">0</mml:mn><mml:mi>z</mml:mi></mml:munderover><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>A</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>)</mml:mo><mml:mi mathvariant="normal">d</mml:mi><mml:mi>z</mml:mi></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:mfrac></mml:mstyle><mml:munder><mml:mo movablelimits="false">∑</mml:mo><mml:mi>i</mml:mi></mml:munder><mml:msub><mml:mi>n</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:munderover><mml:mo movablelimits="false">∫</mml:mo><mml:mn mathvariant="normal">0</mml:mn><mml:mi>z</mml:mi></mml:munderover><mml:mi mathvariant="italic">θ</mml:mi><mml:mo>(</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mtext>min</mml:mtext></mml:msub><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>)</mml:mo><mml:mo>)</mml:mo><mml:mi mathvariant="normal">d</mml:mi><mml:mi>z</mml:mi></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:mfrac></mml:mstyle><mml:munder><mml:mo movablelimits="false">∑</mml:mo><mml:mi>i</mml:mi></mml:munder><mml:msub><mml:mi>n</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>⋅</mml:mo><mml:mtext>min</mml:mtext><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>,</mml:mo><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow><mml:mover accent="true"><mml:mi>V</mml:mi><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:mfrac></mml:mstyle><mml:mo>)</mml:mo><mml:mo>.</mml:mo></mml:mrow></mml:mtd></mml:mtr></mml:mtable></mml:math></disp-formula></p>
      <p id="d2e6200">In the last step, it was used that <inline-formula><mml:math id="M334" display="inline"><mml:mrow><mml:mi mathvariant="italic">θ</mml:mi><mml:mo>(</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mtext>min</mml:mtext></mml:msub><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>)</mml:mo><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> is zero if <inline-formula><mml:math id="M335" display="inline"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>&lt;</mml:mo><mml:msub><mml:mi>V</mml:mi><mml:mtext>min</mml:mtext></mml:msub><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>, which is the case if <inline-formula><mml:math id="M336" display="inline"><mml:mrow><mml:mi>z</mml:mi><mml:mo>&gt;</mml:mo><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mstyle displaystyle="false"><mml:mfrac style="text"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow><mml:mover accent="true"><mml:mi>V</mml:mi><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:mfrac></mml:mstyle></mml:mrow></mml:math></inline-formula> (Eq. <xref ref-type="disp-formula" rid="Ch1.E8"/>).</p>

      <fig id="FA1" specific-use="star"><label>Figure A1</label><caption><p id="d2e6289">Probability density functions as a function of particle diameter for the exponential PSDs analyzed in this study. Panel <bold>(a)</bold> shows the distribution of particle number across diameters (a Rosin–Rammler distribution with shape 3 and scale given by the mean volume diameter <inline-formula><mml:math id="M337" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula>) and panel <bold>(b)</bold> displays the distribution of particle mass (a generalized gamma distribution with shape parameters <inline-formula><mml:math id="M338" display="inline"><mml:mrow><mml:mi>p</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M339" display="inline"><mml:mrow><mml:mi>d</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">6</mml:mn></mml:mrow></mml:math></inline-formula> and scale <inline-formula><mml:math id="M340" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula>). Vertical dotted lines display the mean volume diameters <inline-formula><mml:math id="M341" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> of the three distributions.</p></caption>
        <graphic xlink:href="https://bg.copernicus.org/articles/23/3279/2026/bg-23-3279-2026-f05.png"/>

      </fig>

      <fig id="FA2" specific-use="star"><label>Figure A2</label><caption><p id="d2e6352">Numerical simulation used to validate the analytical uniform particle flux profile. Particles of diameter <inline-formula><mml:math id="M342" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M343" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 1.7 <inline-formula><mml:math id="M344" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> are continuously added at the surface (<inline-formula><mml:math id="M345" display="inline"><mml:mi>T</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M346" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 25 <inline-formula><mml:math id="M347" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">°</mml:mi><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>, pH <inline-formula><mml:math id="M348" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 8.2) and sink through a vertical grid of 0.1 <inline-formula><mml:math id="M349" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> resolution with a timestep of 1 <inline-formula><mml:math id="M350" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">h</mml:mi></mml:mrow></mml:math></inline-formula>. <bold>(a)</bold> The alkalinity release in each time step at different time points. The release is constant down to the depth the first-added particle reaches. At the dissolution time <inline-formula><mml:math id="M351" display="inline"><mml:mrow><mml:msub><mml:mi>t</mml:mi><mml:mtext>diss</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> and afterwards, the alkalinity release profile extends down to the penetration depth <inline-formula><mml:math id="M352" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>. <bold>(b)</bold> The cumulative alkalinity release is not strictly rectangular, since particles that were released less than <inline-formula><mml:math id="M353" display="inline"><mml:mrow><mml:msub><mml:mi>t</mml:mi><mml:mtext>diss</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M354" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 2.18 years before have not reached <inline-formula><mml:math id="M355" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> yet and have only released alkalinity at shallower depths. For longer time periods since the start of the experiment, these particles matter relatively less, such that the cumulative alkalinity release is eventually also approximately rectangular. For example, the cumulative alkalinity released at depth <inline-formula><mml:math id="M356" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is 95 % of that at the surface after 40 years.</p></caption>
        <graphic xlink:href="https://bg.copernicus.org/articles/23/3279/2026/bg-23-3279-2026-f06.png"/>

      </fig>

      <fig id="FA3" specific-use="star"><label>Figure A3</label><caption><p id="d2e6504">The base-10 logarithm of the area-normalized dissolution rate of forsterite determined for geometric surfaces from <xref ref-type="bibr" rid="bib1.bibx36" id="text.70"/> as a function of temperature and pH.</p></caption>
        <graphic xlink:href="https://bg.copernicus.org/articles/23/3279/2026/bg-23-3279-2026-f07.png"/>

      </fig>

      <fig id="FA4" specific-use="star"><label>Figure A4</label><caption><p id="d2e6519">Annual maximum mixed layer depth in the GFDL ESM2M model. Mixed layer depth is defined as the depth where density increases by 0.03 <inline-formula><mml:math id="M357" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">kg</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> relative to the surface. It is calculated as the annual maximum of monthly mixed layer depth, averaged over the period 2016-2025 and over five ensemble members. Global average annual maximum mixed layer depth is 123 <inline-formula><mml:math id="M358" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>.</p></caption>
        <graphic xlink:href="https://bg.copernicus.org/articles/23/3279/2026/bg-23-3279-2026-f08.png"/>

      </fig>

      <fig id="FA5" specific-use="star"><label>Figure A5</label><caption><p id="d2e6554">Global mean vertical distribution of additional alkalinity relative to that for surface alkalinity addition over time for the uniform and exponential PSDs with mean volume diameters of 1.7, 2.6, and 3.4 <inline-formula><mml:math id="M359" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> (panels <bold>a</bold>–<bold>e</bold>). We do not show the alkalinity difference for the uniform particle profile with <inline-formula><mml:math id="M360" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M361" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 1.7 <inline-formula><mml:math id="M362" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, as differences are minor. Panel <bold>(f)</bold> shows the alkalinity difference in the eastern and central equatorial Pacific (<inline-formula><mml:math id="M363" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>8 to 8° N, <inline-formula><mml:math id="M364" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>190 to <inline-formula><mml:math id="M365" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>85° E) for the uniform case with <inline-formula><mml:math id="M366" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M367" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 2.6 <inline-formula><mml:math id="M368" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>.</p></caption>
        <graphic xlink:href="https://bg.copernicus.org/articles/23/3279/2026/bg-23-3279-2026-f09.png"/>

      </fig>

      <fig id="FA6" specific-use="star"><label>Figure A6</label><caption><p id="d2e6655">Numerical simulation used to test the influence of variations in temperature and pH (on the total scale) along the water column on the alkalinity release profile. Panel <bold>(a)</bold> shows two exemplary temporal mean profiles, one from the Southern Ocean (<inline-formula><mml:math id="M369" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>57.5° N, 177.5° E) in blue and one from the subtropical Atlantic (20.9° N, <inline-formula><mml:math id="M370" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>58.5° E) in red. Light vertical lines in panel <bold>(a)</bold> show mean temperature and pH over the upper 300 <inline-formula><mml:math id="M371" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>. Under the idealized dissolution profile approach (Sect. <xref ref-type="sec" rid="Ch1.S2.SS3"/>), particles with a diameter of 1.7 <inline-formula><mml:math id="M372" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> in the subtropical Atlantic column and particles with a diameter of 2.6 <inline-formula><mml:math id="M373" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> in the Southern Ocean column both penetrate down to 300 <inline-formula><mml:math id="M374" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> (penetration depth <inline-formula><mml:math id="M375" display="inline"><mml:mrow><mml:msub><mml:mi>z</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> of 300 <inline-formula><mml:math id="M376" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>). The numerical alkalinity release profiles with explicit vertical temperature and pH profiles are shown in panel <bold>(b)</bold>. Panel <bold>(c)</bold> shows the penetration depth with explicit temperature and pH profiles for particles with diameter <inline-formula><mml:math id="M377" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M378" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 2.6 <inline-formula><mml:math id="M379" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> globally, and panel <bold>(d)</bold> shows the difference to the penetration depth assuming mean temperature and pH (Fig. <xref ref-type="fig" rid="F2"/>b). Regions where the water column is shallower than the penetration depth are left blank as they do not allow a direct comparison. Panel <bold>(e)</bold> shows the fraction dissolved in the annual maximum mixed layer with explicit temperature and pH profiles and panel <bold>(f)</bold> shows the difference to the dissolved fraction assuming mean temperature and pH  (Fig. <xref ref-type="fig" rid="F2"/>e).</p></caption>
        <graphic xlink:href="https://bg.copernicus.org/articles/23/3279/2026/bg-23-3279-2026-f10.png"/>

      </fig>

<fig id="FA7"><label>Figure A7</label><caption><p id="d2e6790"><bold>(a)</bold> Discretized sieve-based particle size distribution from <xref ref-type="bibr" rid="bib1.bibx34" id="text.71"/> compared to the exponential particle size distributions from this study for mean volume diameters of 1.7 and 3.4 <inline-formula><mml:math id="M380" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, respectively. The PSDs are plotted on a log-log scale as that from <xref ref-type="bibr" rid="bib1.bibx34" id="text.72"/> spans many orders of magnitudes in particle volume, with its near-linear evolution resembling a heavy-tailed power-law distribution. <bold>(b)</bold> Cumulative alkalinity release over the upper 500 <inline-formula><mml:math id="M381" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> assuming <inline-formula><mml:math id="M382" display="inline"><mml:mi>T</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M383" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 25 <inline-formula><mml:math id="M384" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">°</mml:mi><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula> and pH <inline-formula><mml:math id="M385" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 8.2.</p></caption>
        
        <graphic xlink:href="https://bg.copernicus.org/articles/23/3279/2026/bg-23-3279-2026-f11.png"/>

      </fig>

      <fig id="FA8"><label>Figure A8</label><caption><p id="d2e6865">Global-mean pH difference along the water column between OAE and the baseline simulation without OAE, for <bold>(a)</bold> the exponential PSD with mean volume diameter of 3.4 <inline-formula><mml:math id="M386" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> and <bold>(b)</bold> surface alkalinity addition. The pH change is on the total scale and averaged over the period 2026–2200. Panel <bold>(c)</bold> shows the pH difference between the exponential PSD with mean volume diameter of 3.4 <inline-formula><mml:math id="M387" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> and surface alkalinity addition. Panel <bold>(d)</bold> shows the total change in pH from the baseline <inline-formula><mml:math id="M388" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> emissions and OAE with the exponential PSD relative to the pre-industrial state.</p></caption>
        
        <graphic xlink:href="https://bg.copernicus.org/articles/23/3279/2026/bg-23-3279-2026-f12.png"/>

      </fig>


</app>
  </app-group><notes notes-type="codedataavailability"><title>Code and data availability</title>

      <p id="d2e6926">The code used for this study and the analyzed simulation data are available under the Zenodo repository <uri>https://zenodo.org/records/19944254</uri> <xref ref-type="bibr" rid="bib1.bibx4" id="paren.73"/>.</p>
  </notes><notes notes-type="authorcontribution"><title>Author contributions</title>

      <p id="d2e6938">The concept of the study and the methodology for the dissolution profiles were developed by F.A.B. U.H.E. and F.A.B. implemented the dissolution profile in the Earth system model. F.A.B. conducted the simulations with subsurface alkalinity addition and the baseline simulations without OAE. H.G. conducted the simulations with surface alkalinity addition. F.A.B., U.H.E., H.G., and T.F jointly worked on the interpretation of the results. The initial draft was written by F.A.B., and U.H.E., H.G., and T.F. provided feedback and revised the text.</p>
  </notes><notes notes-type="competinginterests"><title>Competing interests</title>

      <p id="d2e6944">The contact author has declared that none of the authors has any competing interests.</p>
  </notes><notes notes-type="disclaimer"><title>Disclaimer</title>

      <p id="d2e6950">Publisher's note: Copernicus Publications remains neutral with regard to jurisdictional claims made in the text, published maps, institutional affiliations, or any other geographical representation in this paper. The authors bear the ultimate responsibility for providing appropriate place names. Views expressed in the text are those of the authors and do not necessarily reflect the views of the publisher.</p>
  </notes><ack><title>Acknowledgements</title><p id="d2e6956">The authors also thank the CSCS Swiss National Supercomputing Centre for computing resources (project number s1328). We thank both reviewers, the editor as well as Thomas Studer for their valuable comments on the manuscript.</p></ack><notes notes-type="financialsupport"><title>Financial support</title>

      <p id="d2e6961">This study was supported by the Bloom Foundation.</p>
  </notes><notes notes-type="reviewstatement"><title>Review statement</title>

      <p id="d2e6967">This paper was edited by Mathilde Hagens and reviewed by two anonymous referees.</p>
  </notes><ref-list>
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