References

Biogeosciences

1726-4189

Copernicus Publications

Göttingen, Germany

10.5194/bg-10-1013-2013

Predicting the denitrification capacity of sandy aquifers from shorter-term incubation experiments and sediment properties

Eschenbach

¹ ² Well

Soil Science of Temperate Ecosystems, Büsgen-Institute, Büsgenweg 2, 37077 Göttingen, Germany

Johann Heinrich von Thünen-Institut, Federal Research Institute for Rural Areas, Forestry and Fisheries, Thünen Institute of Climate-Smart Agriculture, Bundesallee 50, 38116 Braunschweig, Germany

13 02 2013

10 2 1013 1035

2013

This work is licensed under the Creative Commons Attribution 3.0 Unported License. To view a copy of this licence, visit https://creativecommons.org/licenses/by/3.0/

This article is available from https://bg.copernicus.org/articles/10/1013/2013/bg-10-1013-2013.html

The full text article is available as a PDF file from https://bg.copernicus.org/articles/10/1013/2013/bg-10-1013-2013.pdf

Knowledge about the spatial variability of denitrification rates and the lifetime of denitrification in nitrate-contaminated aquifers is crucial to predict the development of groundwater quality. Therefore, regression models were derived to estimate the measured cumulative denitrification of aquifer sediments after one year of incubation from initial denitrification rates and several sediment parameters, namely total sulphur, total organic carbon, extractable sulphate, extractable dissolved organic carbon, hot water soluble organic carbon and potassium permanganate labile organic carbon. For this purpose, we incubated aquifer material from two sandy Pleistocene aquifers in Northern Germany under anaerobic conditions in the laboratory using the 15N tracer technique. The measured amount of denitrification ranged from 0.19 to 56.2 mg N kg−1 yr−1. The laboratory incubations exhibited high differences between non-sulphidic and sulphidic aquifer material in both aquifers with respect to all investigated sediment parameters. Denitrification rates and the estimated lifetime of denitrification were higher in the sulphidic samples. For these samples, the cumulative denitrification measured during one year of incubation (Dcum(365)) exhibited distinct linear regressions with the stock of reduced compounds in the investigated aquifer samples. Dcum(365) was predictable from sediment variables within a range of uncertainty of 0.5 to 2 (calculated Dcum(365)/measured Dcum(365)) for aquifer material with a Dcum(365) > 20 mg N kg−1 yr−1. Predictions were poor for samples with lower Dcum(365), such as samples from the NO3− bearing groundwater zone, which includes the non-sulphidic samples, from the upper part of both aquifers where denitrification is not sufficient to protect groundwater from anthropogenic NO3− input. Calculation of Dcum(365) from initial denitrification rates was only successful for samples from the NO3−-bearing zone, whereas a lag-phase of denitrification in samples from deeper zones of NO3− free groundwater caused imprecise predictions. In our study, Dcum(365) of two sandy Pleistocene aquifers was predictable using a combination of short-term incubations and analysis of sediment parameters. Moreover, the protective lifetime of denitrification sufficient to remove NO3− from groundwater in the investigated aquifers is limited, which demonstrates the need to minimise anthropogenic NO3− input.

References 1

Addy, K., Kellogg, D. Q., Gold, A. J., Groffman, P. M., Ferendo, G., and Sawyer, C.: In situ pushpull method to determine ground water denitrification in riparian zones, J. Environ. Qual., 31, 1017–1024, 2002.

Balesdent, J.: The significance of organic separates to carbon dynamics and its modeling in some cultivated soils, Eur. J. Soil Sci., 47, 485–493, <a href="http://dx.doi.org/10.1111/j.1365-2389.1996.tb01848.x">https://doi.org/10.1111/j.1365-2389.1996.tb01848.x</a>, 1996.

Behm, R.: Untersuchung zur Bestimmung der leicht umsetzbaren N- und C-Anteile im Hei{ß}wasserextrakt des Bodens-Kurzmitteilung, Arch. Acker. Pfl. Boden., 32, 333–335, 1988.

Bergmann, A.: Hydrogeochemische Untersuchungen anoxischer Redoxprozesse in tiefen Porengrundwasserleitern der Niederrheiniscchen Bucht – im Umfeld des Tagebaus Garzweiler I, Bochumer geol. geotechn. Arb. 51, 59. Abb., 27. Tab., Bochum, Germany, 167 pp., 1999.

Böttcher, J., Strebel, O., Voerkelius, S., and Schmidt, H. L.: Using isotope fractionation of Nitrate nitrogen and nitrate oxygen for evaluation of microbial denitrification in a sandy aquifer, J. Hydrol., 114, 413–424, 1990.

Böttcher, J., Strebel, O., and Duijnisveld, W. H. M.: Reply (to a comment of Scott F. Korom), Water Resour. Res., 27, 3275–3278, 1991.

Böttcher, J., Strebel, O., and Kölle, W.: Redox conditions and microbial sulfur reactions in the Fuhrberger Feld sandy aquifer, in: Progress in Hydrogeochemistry, edited by: Matthess, G., Frimmel, F. H., Hirsch, P., Schulz, H. D., and Usdowski, E., Springer, Berlin and Heidelberg, 219–226, 1992.

Bouraoui, F., Grizzetti, B., and Aloe, A.: Nutrient Discharge from Rivers to Seas for Year 2000, Joint Research Centre Scientific and technical Reports, 77 pp., 2009.

Chodak, M., Khanna, P., and Beese, F.: Hot water extractable C and N in relation to microbiological properties of soils under beech forests, Biol. Fert. Soils, 39, 123–130, <a href="http://dx.doi.org/10.1007/s00374-003-0688-0">https://doi.org/10.1007/s00374-003-0688-0</a>, 2003.

Dalton, H. and Brand-Hardy, R.: Nitrogen: the essential public enemy, J. Appl. Ecol., 40, 71– 781, 2003.

Defra: Post-Conciliation Partial Regulatory Impact Assessment – Groundwater Proposals Under Article 17 of the Water Framework Directive. Draft final report, Department for Environment, Food and Rural Affairs, London, 2006.

Eusterhues, K., Rumpel, C., and Kogel-Knabner, I.: Organo-mineral associations in Sandy acid forest soils: importance of specific surface area, iron oxides and micropores, Eur. J. Soil Sci., 56, 753–763, <a href="http://dx.doi.org/10.1111/j.1365-2389.2005.00710.x">https://doi.org/10.1111/j.1365-2389.2005.00710.x</a>, 2005.

Frind, E. O., Duynisveld, W. H. M., Strebel, O., and Böttcher, J.: Modeling of multicomponent transport with microbial transformation in groundwater – the Fuhrberg case, Water Resour. Res., 26, 1707–1719, 1990.

Galloway, J. N., Dentener, F. J., Capone, D. G., Boyer, E. W., Howarth, R. W., Seitzinger, S. P., Asner, G. P., Cleveland, C. C., Green, P. A., Holland, E. A., Karl, D. M., Michaels, A. F., Porter, J. H., Townsend, A. R., and Vorosmarty, C. J.: Nitrogen cycles: past, present, and future, Biogeochemistry, 70, 153–226, 2004.

Green, C. T., Puckett, L. J., Bohlke, J. K., Bekins, B. A., Phillips, S. P., Kauffman, L. J., Denver, J. M., and Johnson, H. M.: Limited occurrence of denitrification in four shallow aquifers in agricultural areas of the United States, J. Environ. Qual., 37, 994–1009, <a href="http://dx.doi.org/10.2134/jeq2006.0419">https://doi.org/10.2134/jeq2006.0419</a>, 2008.

Green, C. T., Bohlke, J. K., Bekins, B. A., and Phillips, S. P.: Mixing effects on apparent reaction rates and isotope fractionation during denitrification in a heterogeneous aquifer, Water Resour. Res., 46, W08525, <a href="http://dx.doi.org/10.1029/2009wr008903">https://doi.org/10.1029/2009wr008903</a>, 2010.

Griebler, C. and Lueders, T.: Microbial biodiversity in groundwater ecosystems, Freshwater Biol., 54, 649–677, <a href="http://dx.doi.org/10.1111/j.1365-2427.2008.02013.x">https://doi.org/10.1111/j.1365-2427.2008.02013.x</a>, 2009.

Groffman, P. M., Altabet, M. A., Bohlke, J. K., Butterbach-Bahl, K., David, M. B., Firestone, M. K., Giblin, A. E., Kana, T. M., Nielsen, L. P., and Voytek, M. A.: Methods for measuring denitrification: diverse approaches to a difficult problem, Ecol. Appl., 16, 2091–2122, 2006.

Hansen, C.: Entwicklung und Anwendung hydrogeochemischer Stoffflussmodelle zur Modellierung der Grund- und Rohwasserqualität in Gewinnungsanlagen – Fallbeispiel Fuhrberger Feld, Clausthaler Geowissenschaften, 4: XII, Dissertation Univ. of Clausthal, Clausthal-Zellerfeld, Germany, 246 pp., 2005.

Hartog, N., Van Bergen, P. F., De Leeuw, J. W., and Griffioen, J.: Reactivity of organic Matter in aquifer sediments: geological and geochemical controls, Geochim. Cosmochim. Ac., 68, 1281–1292, <a href="http://dx.doi.org/10.1016/j.gca.2003.09.004">https://doi.org/10.1016/j.gca.2003.09.004</a>, 2004.

Houben, G.: Modellansätze zur Prognose der langfristigen Entwicklung der Grundwasserqualität – Fallbeispiel Bourtanger Moor (Emsland), Aachener Geowissenschaftliche Beiträge 36, Aachen, Germany, 213 pp., 2000.

Howar, M.: Geologische 3-D-Untergrundmodellierung im Bereich Gro{ß}enkneten/Ahlhorn., unpubl. Expertise: Insight, Geologische Softwaresysteme GmbH, Köln, Germany, 11 pp., 2005.

Khanna, P. K., Prenzel, J., Meiwes, K. J., Ulrich, B., and Matzner, E.: Dynamics of sulfate retention by acid forest soils in an acidic deposition environment, Soil Sci. Soc. Am. J., 51, 446–452, 1987.

Köhler, K., Duynisveld, W. H. M., and Böttcher, J.: Nitrogen fertilization and nitrate leaching into groundwater on arable sandy soils, J. Plant Nutr. Soil Sc., 169, 185–195, <a href="http://dx.doi.org/10.1002/jpln.200521765">https://doi.org/10.1002/jpln.200521765</a>, 2006.

Kölbelboelke, J., Anders, E. M., and Nehrkorn, A.: Microbial communities in the saturated groundwater environment, 2. Diversity of bacterial communities in a pleistocene sand aquifer and their invitro activities, Microb. Ecol., 16, 31–48, <a href="http://dx.doi.org/10.1007/bf02097403">https://doi.org/10.1007/bf02097403</a>, 1988.

Kölle, W., Werner, P., Strebel, O., and Böttcher, J.: Denitrification by pyrite in a reducing aquifer, Vom Wasser, 61, 125–147, 1983.

Kölle, W., Strebel, O., and Böttcher, J.: Formation of sulfate by microbial denitrification in a Reducing aquifer, Water Supp., 3, 35–40, 1985.

Konrad, C.: Methoden zur Bestimmung des Umsatzes von Stickstoff für drei pleistozäne Grundwasserleiter Norddeutschlands, 161 pp., 2007.

Korom, S. F.: Modeling of multicomponent transport with microbial transformation in groundwater – the Fuhrberg case – comment, Water Resour. Res., 27, 3271–3274, 1991.

Korom, S. F.: Natural denitrification in the saturated zone – a review, Water Resour. Res., 28, 1657–1668, 1992.

Korom, S. F., Schlag, A. J., Schuh, W. M., and Schlag, A. K.: In situ mesocosms: denitrification in the Elk Valley aquifer, Ground Water Monit. R., 25, 79–89, 2005.

Korom, S. F., Schuh, W. M., Tesfay, T., and Spencer, E. J.: Aquifer denitrification and in situ mesocosms: modeling electron donor contributions and measuring rates, J. Hydrol., 432/433, 112–126, <a href="http://dx.doi.org/10.1016/j.jhydrol.2012.02.023">https://doi.org/10.1016/j.jhydrol.2012.02.023</a>, 2012.

Law, G. T. W., Geissler, A., Boothman, C., Burke, I. T., Livens, F. R., Lloyd, J. R., and Morris, K.: Role of nitrate in conditioning aquifer sediments for technetium bioreduction, Environ. Sci. Technol., 44, 150–155, <a href="http://dx.doi.org/10.1021/es9010866">https://doi.org/10.1021/es9010866</a>, 2010.

Manderscheid, B., Schweisser, T., Lischeid, G., Alewell, C., and Matzner, E.: Sulfate pools in the weathered substrata of a forested catchment, Soil Sci. Soc. Am. J., 64, 1078–1082, 2000.

McMahon, P. B., Bohlke, J. K., and Christenson, S. C.: Geochemistry, radiocarbon ages, and paleorecharge conditions along a transect in the Central High Plains aquifer, Southwestern Kansas, USA, Appl. Geochem., 19, 1655–1686, <a href="http://dx.doi.org/10.1016/j.apgeochem.2004.05.003">https://doi.org/10.1016/j.apgeochem.2004.05.003</a>, 2004.

Mehranfar, O.: Laboruntersuchungen zum langfristigen Denitrifikationspotential im oberflächennahen Grundwasser hydromorpher Mineralböden Nordwestdeutschlands, 128 pp., 2003.

Nordstrom, D. K.: The effect of sulfate on aluminum concentrations in natural-waters – some stability relations in the system Al2O3-SO3-H2O at 298-K, Geochim. Cosmochim. Ac., 46, 681–692, <a href="http://dx.doi.org/10.1016/0016-7037(82)90168-5">https://doi.org/10.1016/0016-7037(82)90168-5</a>, 1982.

Renger, M., Strebel, O., Wessolek, G., and Duynisveld, W. H. M.: Evapotranspiration and groundwater recharge – a case-study for different climate, crop patterns, soil properties and groundwater depth conditions, Z. Pflanz. Bodenkunde, 149, 371–381, <a href="http://dx.doi.org/10.1002/jpln.19861490403">https://doi.org/10.1002/jpln.19861490403</a>, 1986.

Rivett, M. O., Buss, S. R., Morgan, P., Smith, J. W. N., and Bemment, C. D.: Nitrate attenuation in groundwater: a review of biogeochemical controlling processes, Water Res., 42, 4215–4232, <a href="http://dx.doi.org/10.1016/j.watres.2008.07.020">https://doi.org/10.1016/j.watres.2008.07.020</a>, 2008.

Santoro, A. E., Boehm, A. B., and Francis, C. A.: Denitrifier community composition along a nitrate and salinity gradient in a coastal aquifer, Appl. Environ. Microb., 72, 2102–2109, <a href="http://dx.doi.org/10.1128/aem.72.3.2102-2109.2006">https://doi.org/10.1128/aem.72.3.2102-2109.2006</a>, 2006.

Schlichting, E., Blume, H. P., and Stahr, K.: Bodenkundliches Praktikum, Blackwell Wissenschaft, Berlin, Germany, 295 pp., 1995.

Schuchert, A.: Zielflächenidentifikation für Grundwasserschutzma{ß}nahmen, Eine GIS-Datenanalyse im Wasserschutzgebiet Gro{ß}enkneten, Landkreis Oldenburg, Diploma thesis, Institute for Geography, University of Bremen, Germany, 2007.

Seitzinger, S., Harrison, J. A., Bohlke, J. K., Bouwman, A. F., Lowrance, R., Peterson, B., Tobias, C., and Van Drecht, G.: Denitrification across landscapes and waterscapes: a synthesis, Ecol. Appl., 16, 2064–2090, 2006.

Sparling, G., Vojvodic-Vukovic, M., and Schipper, L. A.: Hot-water-soluble C as a simple measure of labile soil organic matter: the relationship with microbial biomass C, Soil Biol. Biochem., 30, 1469–1472, <a href="http://dx.doi.org/10.1016/S0038-0717(98)00040-6">https://doi.org/10.1016/S0038-0717(98)00040-6</a>, 1998.

Strebel, O., Böttcher, J., and Duijnisveld, W. H. M.: Identifizierung und Quantifizierung von Stoffumsetzungen in einem Sand-Aquifer (Beispiel Fuhrberger Feld), DVGW Schriftenr. Wasser, 73, 55–73, 1992.

Tesoriero, A. J. and Puckett, L. J.: O2 reduction and denitrification rates in shallow aquifers, Water Resour. Res., 47, W12522, <a href="http://dx.doi.org/10.1029/2011wr010471">https://doi.org/10.1029/2011wr010471</a>, 2011.

Trudell, M. R., Gillham, R. W., and Cherry, J. A.: An insitu study of the occurrence and rate of denitrification in a shallow unconfined sand aquifer, J. Hydrol., 83, 251–268, 1986.

Ulrich, B.: Natural and anthropogenic components of soil acidification, Z. Pflanz. Bodenkunde, 149, 702–717, <a href="http://dx.doi.org/10.1002/jpln.19861490607">https://doi.org/10.1002/jpln.19861490607</a>, 1986.

van Berk, W., Kübeck, C., Steding, T., van Straaten, L., and Wilde, S.: Vorstudie zur Hydrogeologie im Wassergewinnungsgebiet Gro{ß}enkneten, 55 pp., 2005.

Vitousek, P. M., Aber, J. D., Howarth, R. W., Likens, G. E., Matson, P. A., Schindler, D. W., Schlesinger, W. H., and Tilman, G. D.: Human alteration of the global nitrogen cycle: Sources and consequences, Ecol. Appl., 7, 737–750, 1997.

von der Heide, C., Böttcher, J., Deurer, M., Weymann, D., Well, R., and Duijnisveld, W. H. M.: Spatial variability of N2O concentrations and of denitrification-related factors in the surficial groundwater of a catchment in Northern Germany, J. Hydrol., 360, 230– 241, <a href="http://dx.doi.org/10.1016/j.jhydrol.2008.07.034">https://doi.org/10.1016/j.jhydrol.2008.07.034</a>, 2008.

von der Heide, C., Böttcher, J., Deurer, M., Duijnisveld, W. H. M., Weymann, D., and Well, R.: Spatial and temporal variability of N2O in the surface groundwater: a detailed analysis from a sandy aquifer in Northern Germany, Nutr. Cycl. Agroecosys., 87, 33–47, <a href="http://dx.doi.org/10.1007/s10705-009-9310-7">https://doi.org/10.1007/s10705-009-9310-7</a>, 2010.

Wall, L. G., Tank, J. L., Royer, T. V., and Bernot, M. J.: Spatial and temporal variability in sediment denitrification within an agriculturally influenced reservoir, Biogeochemistry, 76, 85–111, <a href="http://dx.doi.org/10.1007/s10533-005-2199-6">https://doi.org/10.1007/s10533-005-2199-6</a>, 2005.

Weiss, R. F.: Solubility of nitrogen, oxygen and argon in water and seawater, Deep-Sea Res., 17, 721–735, 1970.

Weiss, R. F. and Price, B. A.: Nitrous-oxide solubility in water and seawater, Mar. Chem., 8, 347–359, 1980.

Well, R. and Myrold, D. D.: Laboratory evaluation of a new method for in situ measurement of denitrification in water-saturated soils, Soil Biol. Biochem., 31, 1109–1119, 1999.

Well, R., Augustin, J., Meyer, K., and Myrold, D. D.: Comparison of field and laboratory measurement of denitrification and N2O production in the saturated zone of hydromorphic soils, Soil Biol. Biochem., 35, 783–799, <a href="http://dx.doi.org/10.1016/s0038- 0717(03)00106-8">https://doi.org/10.1016/s0038- 0717(03)00106-8</a>, 2003.

Well, R., Höper, H., Mehranfar, O., and Meyer, K.: Denitrification in the saturated zone of hydromorphic soils-laboratory measurement, regulating factors and stochastic modeling, Soil Biol. Biochem., 37, 1822–1836, <a href="http://dx.doi.org/10.1016/j.soilbio.2005.02.014">https://doi.org/10.1016/j.soilbio.2005.02.014</a>, 2005.

Well, R., Eschenbach, W., Flessa, H., von der Heide, C., and Weymann, D.: Are dual isotope and isotopomer ratios of N2O useful indicators for N2O turnover during denitrification in nitrate-contaminated aquifers?, Geochim. Cosmochim. Ac., 90, 265–282, 2012.

Wessolek, G., Renger, M., Strebel, O., and Sponagel, H.: Einflu{ß} von Boden und Grundwasserflurabstand auf die jährliche Grundwasserneubildung unter Acker, Grünland und Nadelwald., Z. Kulturtech. Flurber., 26, 130–137, 1985.

Weymann, D., Well, R., Flessa, H., von der Heide, C., Deurer, M., Meyer, K., Konrad, C., and Walther, W.: Groundwater N2O emission factors of nitrate-contaminated aquifers as derived from denitrification progress and N2O accumulation, Biogeosciences, 5, 1215–1226, <a href="http://dx.doi.org/10.5194/bg-5-1215-2008">https://doi.org/10.5194/bg-5-1215-2008</a>, 2008.

Weymann, D., Well, R., von der Heide, C., Böttcher, J., Flessa, H., and Duijnisveld, W. H. M.: Recovery of groundwater N2O at the soil surface and its contribution to total N2O emissions, Nutr. Cycl. Agroecosys., 85, 299–312, <a href="http://dx.doi.org/10.1007/s10705-009-9269-4">https://doi.org/10.1007/s10705-009-9269-4</a>, 2009.

Weymann, D., Geistlinger, H., Well, R., von der Heide, C., and Flessa, H.: Kinetics of N2O production and reduction in a nitrate-contaminated aquifer inferred from laboratory incubation experiments, Biogeosciences, 7, 1953–1972, <a href="http://dx.doi.org/10.5194/bg-7-1953-2010">https://doi.org/10.5194/bg-7-1953-2010</a>, 2010.

Wirth, K.: Hydrogeologisches Gutachten zur Bemessung und Gliederung der Trinkwasserschutzgebiete für die Fassungen Hagel, Sage und Baumweg, Wasserwerk Gro{ß}enkneten (OOWV), Beratungsbüro für Hydrogeologie (Hrsg.), Göttingen, Germany, 18 pp., 1990.