[en] In this study the variability of greenhouse gases (GHGs) concentrations along lateral and vertical dimensions of the chalk aquifer located in the eastern part of Belgium was examined in order to understand its dependence on hydrogeological and hydrogeochemical conditions. Groundwater samples from 29 wells/piezometers were analyzed for concentrations of nitrous oxide (N2O), carbon dioxide (CO2), methane (CH4), major and minor elements and stable isotopes of nitrate (NO3−), nitrous oxide (N2O), sulfate (SO42−) and boron (B). For lateral investigations, four zones with different environmental settings were identified (southern, central, north-eastern and northern). Groundwater was oversaturated with GHGs with respect to its equilibrium concentrations with the atmosphere in all zones, except the northern one, undersaturated in N2O (0.07 ± 0.08 μgN/L vs. 0.3 μgN/L). Vertical dimension studies showed the decrease in CO2 concentration and significant changes in both isotope signatures and concentration of N2O with depth. The production of N2O could be attributed to a combination of nitrification and denitrification processes occurring at different depths. CO2 concentration is controlled by the process of dissolution of carbonate minerals which constitute aquifer geology. CH4 is produced due to methanogenesis in deeper parts of the aquifer, though its thermogenic origin is also possible. Differences in hydrogeochemical settings and changing intensity of biogeochemical processes across the area and with depth have considerable effect on GHGs concentrations. Thus, before estimating GHGs fluxes at the groundwater–river interface insights obtained from larger-scale investigations are required in order to identify the representative spatial zones which govern GHGs emissions.
H2020 - 642372 - INSPIRATION - INtegrated Spatial PlannIng, land use and soil management Research ActTION
Funders :
CE - Commission Européenne
Funding text :
This project has received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No 675120.
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Bibliography
Aelion, C.M., Höhener, P., Hunkeler, D., Aravena, R., (eds.) Environmental Isotopes in Biodegradation and Bioremediation, 2009, CRC Press.
Anderson, T.R., Groffman, P.M., Kaushal, S.S., Walter, M.T., Shallow groundwater denitrification in riparian zones of a headwater agricultural landscape. J. Environ. Qual. 43:2 (2014), 732–744.
Beaulieu, J.J., Tank, J.L., Hamilton, S.K., Wollheim, W.M., Hall, R.O., Mulholland, P.J., et al. Nitrous oxide emission from denitrification in stream and river networks. Proc. Natl. Acad. Sci. Unit. States Am. 108:1 (2011), 214–219.
Bell, R.A., Darling, W.G., Ward, R.S., Basava-Reddi, L., Halwa, L., Manamsa, K., Dochartaigh, B.Ó., A baseline survey of dissolved methane in aquifers of Great Britain. Sci. Total Environ. 601 (2017), 1803–1813.
Boulvain, F., Pingot, J.L., Une introduction à la géologie de la Wallonie. 2008.
Brouyère, S., Dassargues, A., Hallet, V., Migration of contaminants through the unsaturated zone overlying the Hesbaye chalky aquifer in Belgium: a field investigation. J. Contam. Hydrol. 72:1–4 (2004), 135–164.
Bunnell-Young, D., Rosen, T., Fisher, T.R., Moorshead, T., Koslow, D., Dynamics of nitrate and methane in shallow groundwater following land use conversion from agricultural grain production to conservation easement. Agric. Ecosyst. Environ. 248 (2017), 200–214.
Butterbach-Bahl, K., Well, R., Indirect emissions of nitrous oxide from nitrogen deposition and leaching of agricultural nitrogen. Nitrous Oxide and Climate Change, 2010, Routledge, 166–193.
Casciotti, K.L., Sigman, D.M., Ward, B.B., Linking diversity and stable isotope fractionation in ammonia-oxidizing bacteria. Geomicrobiol. J. 20:4 (2003), 335–353.
Casciotti, K.L., McIlvin, M., Buchwald, C., Oxygen isotopic exchange and fractionation during bacterial ammonia oxidation. Limnol. Oceanogr. 55:2 (2010), 753–762.
Choi, B.Y., Yun, S.T., Mayer, B., Chae, G.T., Kim, K.H., Kim, K., Koh, Y.K., Identification of groundwater recharge sources and processes in a heterogeneous alluvial aquifer: results from multi‐level monitoring of hydrochemistry and environmental isotopes in a riverside agricultural area in Korea. Hydrol. Process. 24:3 (2010), 317–330.
Clagnan, E., Thornton, S.F., Rolfe, S.A., Tuohy, P., Peyton, D., Wells, N.S., Fenton, O., Influence of artificial drainage system design on the nitrogen attenuation potential of gley soils: evidence from hydrochemical and isotope studies under field-scale conditions. J. Environ. Manag. 206 (2018), 1028–1038.
Clough, T.J., Addy, K., Kellogg, D.Q., Nowicki, B.L., Gold, A.J., Groffman, P.M., Dynamics of nitrous oxide in groundwater at the aquatic–terrestrial interface. Glob. Chang. Biol. 13 (2007), 1528–1537.
Currell, M., Banfield, D., Cartwright, I., Cendón, D.I., Geochemical indicators of the origins and evolution of methane in groundwater: Gippsland Basin, Australia. Environ. Sci. Pollut. Control Ser. 24:15 (2017), 13168–13183.
Dautrebande, S., Sohier, C., Modélisation hydrologique des sols et des pratiques agricoles en Région wallonne (Sous-bassins de la Meuse et de l'Escaut). 2004, Faculté des Sciences Agronomiques de Gembloux, Unité d'Hydraulique Agricole.
Denman, S.E., Tomkins, N.W., McSweeney, C.S., Quantitation and diversity analysis of ruminal methanogenic populations in response to the antimethanogenic compound bromochloromethane. FEMS Microbiol. Ecol. 62:3 (2007), 313–322.
Fitts, C.R., Groundwater Science. 2002, Elsevier.
Gamble, A., Babbar-Sebens, M., On the use of multivariate statistical methods for combining in-stream monitoring data and spatial analysis to characterize water quality conditions in the White River Basin, Indiana, USA. Environ. Monit. Assess. 184:2 (2012), 845–875.
Goderniaux, P., Brouyere, S., Blenkinsop, S., Burton, A., Fowler, H.J., Orban, P., Dassargues, A., Modeling climate change impacts on groundwater resources using transient stochastic climatic scenarios. Water Resour. Res., 47(12), 2011.
Hakoun, V., Orban, P., Dassargues, A., Brouyère, S., Factors controlling spatial and temporal patterns of multiple pesticide compounds in groundwater (Hesbaye chalk aquifer, Belgium). Environ. Pollut. 223 (2017), 185–199.
Hasegawa, K., Hanaki, K., Matsuo, T., Hidaka, S., Nitrous oxide from the agricultural water system contaminated with high nitrogen. Chemosphere Global Change Sci. 2:3 (2000), 335–345.
Hérivaux, C., Orban, P., Brouyère, S., Is it worth protecting groundwater from diffuse pollution with agri-environmental schemes? A hydro-economic modeling approach. J. Environ. Manag. 128 (2013), 62–74.
Hiscock, K.M., Bateman, A.S., Mühlherr, I.H., Fukada, T., Dennis, P.F., Indirect emissions of nitrous oxide from regional aquifers in the United Kingdom. Environ. Sci. Technol. 37:16 (2003), 3507–3512.
IPCC, Stocker, T.F., Qin, D., Plattner, G.-K., Tignor, M., Allen, S.K., Boschung, J., Nauels, A., Xia, Y., Bex, V., Midgley, P.M., (eds.) Climate Change 2013: the Physical Science Basis. Contribution of Working Group I to the Fifth Assessment Report of the Intergovernmental Panel on Climate Change, 2013, Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA, 1535, 10.1017/CBO9781107415324.
Iverach, C.P., Beckmann, S., Cendón, D.I., Manefield, M., Kelly, B.F., Biogeochemical constraints on the origin of methane in an alluvial aquifer: evidence for the upward migration of methane from underlying coal measures. Biogeosciences 14:1 (2017), 215–228.
Jahangir, M.M., Khalil, M.I., Johnston, P., Cardenas, L.M., Hatch, D.J., Butler, M., et al. Denitrification potential in subsoils: a mechanism to reduce nitrate leaching to groundwater. Agric. Ecosyst. Environ. 147 (2012), 13–23.
Jahangir, M.M.R., Johnston, P., Barret, M., Khalil, M.I., Groffman, P.M., Boeckx, P., Richards, K.G., Denitrification and indirect N2O emissions in groundwater: hydrologic and biogeochemical influences. J. Contam. Hydrol. 152 (2013), 70–81.
Johnson, M.S., Lehmann, J., Riha, S.J., Krusche, A.V., Richey, J.E., Ometto, J.P.H., Couto, E.G., CO2 efflux from Amazonian headwater streams represents a significant fate for deep soil respiration. Geophys. Res. Lett., 35(17), 2008.
Jurado, A., Borges, A.V., Brouyère, S., Dynamics and emissions of N2O in groundwater: a review. Sci. Total Environ. 584 (2017), 207–218.
Jurado, A., Borges, A.V., Pujades, E., Briers, P., Nikolenko, O., Dassargues, A., Brouyère, S., Dynamics of greenhouse gases in the river–groundwater interface in a gaining river stretch (Triffoy catchment, Belgium). Hydrogeol. J. 26:8 (2018), 2739–2751.
Jurado, A., Borges, A.V., Pujades, E., Hakoun, V., Otten, J., Knöller, K., Brouyère, S., Occurrence of greenhouse gases in the aquifers of the Walloon Region (Belgium). Sci. Total Environ. 619 (2018), 1579–1588.
Kellman, L.M., Hillaire-Marcel, C., Evaluation of nitrogen isotopes as indicators of nitrate contamination sources in an agricultural watershed. Agric. Ecosyst. Environ. 95:1 (2003), 87–102.
Kindler, R., Siemens, J., Kaiser, K., Walmsley, D.C., Bernhofer, C., Buchmann, et al. Dissolved carbon leaching from soil is a crucial component of the net ecosystem carbon balance. Glob. Chang. Biol. 17:2 (2011), 1167–1185.
Knöller, K., Trettin, R., Strauch, G., Sulphur cycling in the drinking water catchment area of Torgau–Mockritz (Germany): insights from hydrochemical and stable isotope investigations. Hydrol. Process. 19:17 (2005), 3445–3465.
Koba, K., Osaka, K., Tobari, Y., Toyoda, S., Ohte, N., Katsuyama, M., et al. Biogeochemistry of nitrous oxide in groundwater in a forested ecosystem elucidated by nitrous oxide isotopomer measurements. Geochem. Cosmochim. Acta 73:11 (2009), 3115–3133.
Krouse, H.R., Mayer, B., Sulphur and oxygen isotopes in sulphate. Environmental Tracers in Subsurface Hydrology, 2000, Springer, Boston, MA, 195–231.
Kroeze, C., Dumont, E., Seitzinger, S.P., New estimates of global emissions of N2O from rivers and estuaries. Environ. Sci. 2:2–3 (2005), 159–165.
Kuzyakov, Y., Larionova, A.A., Root and rhizomicrobial respiration: a review of approaches to estimate respiration by autotrophic and heterotrophic organisms in soil. J. Plant Nutr. Soil Sci. 168:4 (2005), 503–520.
Laini, A., Bartoli, M., Castaldi, S., Viaroli, P., Capri, E., Trevisan, M., Greenhouse gases (CO2, CH4 and N2O) in lowland springs within an agricultural impacted watershed (Po River Plain, northern Italy). Chem. Ecol. 27:2 (2011), 177–187.
Lewicka-Szczebak, D., Augustin, J., Giesemann, A., Well, R., Quantifying N2O reduction to N2 based on N2O isotopocules-validation with independent methods (helium incubation and 15N gas flux method). Biogeosciences, 14(3), 2017, 711.
Li, L., Spoelstra, J., Robertson, W.D., Schiff, S.L., Elgood, R.J., Nitrous oxide as an indicator of nitrogen transformation in a septic system plume. J. Hydrol. 519 (2014), 1882–1894.
MacQuarrie, K.T., Sudicky, E.A., Robertson, W.D., Multicomponent simulation of wastewater-derived nitrogen and carbon in shallow unconfined aquifers: II. Model application to a field site. J. Contam. Hydrol. 47:1 (2001), 85–104.
Macpherson, G.L., CO2 distribution in groundwater and the impact of groundwater extraction on the global C cycle. Chem. Geol. 264:1–4 (2009), 328–336.
Mayer, B., Fritz, P., Prietzel, J., Krouse, H.R., The use of stable sulfur and oxygen isotope ratios for interpreting the mobility of sulfate in aerobic forest soils. Appl. Geochem. 10:2 (1995), 161–173.
Mayer, B., Assessing sources and transformations of sulphate and nitrate in the hydrosphere using isotope techniques. Isotopes in the Water Cycle, 2005, Springer Netherlands, 67–89.
McMahon, P.B., Böhlke, J.K., Regional patterns in the isotopic composition of natural and anthropogenic nitrate in groundwater, High Plains, USA. Environ. Sci. Technol. 40:9 (2006), 2965–2970.
McPhillips, L.E., Creamer, A.E., Rahm, B.G., Walter, M.T., Assessing dissolved methane patterns in central New York groundwater. J. Hydrol.: Reg. Stud. 1 (2014), 57–73.
Michener, R., Lajtha, K., (eds.) Stable Isotopes in Ecology and Environmental Science, 2008, John Wiley & Sons.
Minamikawa, K., Nishimura, S., Sawamoto, T., Nakajima, Y., Yagi, K., Annual emissions of dissolved CO2, CH4, and N2O in the subsurface drainage from three cropping systems. Glob. Chang. Biol. 16:2 (2010), 796–809.
Minamikawa, K., Nishimura, S., Nakajima, Y., Osaka, K.I., Sawamoto, T., Yagi, K., Upward diffusion of nitrous oxide produced by denitrification near shallow groundwater table in the summer: a lysimeter experiment. Soil Sci. Plant Nutr. 57:5 (2011), 719–732.
Minet, E.P., Goodhue, R., Meier-Augenstein, W., Kalin, R.M., Fenton, O., Richards, K.G., Coxon, C.E., Combining stable isotopes with contamination indicators: a method for improved investigation of nitrate sources and dynamics in aquifers with mixed nitrogen inputs. Water Res. 124 (2017), 85–96.
Molofsky, L.J., Connor, J.A., Wylie, A.S., Wagner, T., Farhat, S.K., Evaluation of methane sources in groundwater in northeastern Pennsylvania. Gr. Water 51:3 (2013), 333–349.
Molofsky, L.J., Connor, J.A., McHugh, T.E., Richardson, S.D., Woroszylo, C., Alvarez, P.J., Environmental factors associated with natural methane occurrence in the Appalachian Basin. Gr. Water 54:5 (2016), 656–668.
Moore, C.H., Wade, W.J., Concepts of sequence stratigraphy as applied to carbonate depositional systems. Carbonate Reservoirs: Porosity and Diagenesis in a Sequence Stratigraphic Framework, vol. 67, 2013, Newnes, 19–36.
Morana, C., Darchambeau, F., Roland, F.A.E., Borges, A.V., Muvundja, F., Kelemen, Z., et al. Biogeochemistry of a large and deep tropical lake (Lake Kivu, East Africa: insights from a stable isotope study covering an annual cycle). Biogeosciences 12:16 (2015), 4953–4963.
Mosier, A., Kroeze, C., Nevison, C., Oenema, O., Seitzinger, S., Van Cleemput, O., Closing the global N2O budget: nitrous oxide emissions through the agricultural nitrogen cycle. Nutrient Cycl. Agroecosyst. 52:2–3 (1998), 225–248.
Nikolenko, O., Jurado, A., Borges, A.V., Knӧller, K., Brouyѐre, S., Isotopic composition of nitrogen species in groundwater under agricultural areas: a review. Sci. Total Environ. 621 (2017), 1415–1432.
Orban, P., Batlle-Aguilar, J., Goderniaux, P., Dassargues, A., Brouyère, S., Description of Hydrogeological Conditions in the Geer Sub-catchment and Synthesis of Available Data for Groundwater Modelling. 2006 Deliverable R3.16, AquaTerra (Integrated Project FP6 505428).
Orban, P., Brouyère, S., Batlle-Aguilar, J., Couturier, J., Goderniaux, P., Leroy, M., et al. Regional transport modelling for nitrate trend assessment and forecasting in a chalk aquifer. J. Contam. Hydrol. 118:1–2 (2010), 79–93.
Ostrom, N.E., Pitt, A., Sutka, R., Ostrom, P.H., Grandy, A.S., Huizinga, K.M., Robertson, G.P., Isotopologue effects during N2O reduction in soils and in pure cultures of denitrifiers. J. Geophys. Res.: Biogeosciences, 112(G2), 2007.
Peeters, L., Bacao, R., Lobo, V., Dassargues, A., Exploratory data analysis and clustering of multivariate spatial hydrogeological data by means of GEO3DSOM, a variant of Kohonen's Self-Organizing Map. Hydrol. Earth Syst. Sci. 11:4 (2007), 1309–1321.
Rosamond, M.S., N2O and NO3-In the Grand River: Sources, Production Pathways and Predictability. Doctoral Dissertation, Dissertation. University of Waterloo, 2013.
Sigman, D.M., Casciotti, K.L., Andreani, M., Barford, C., Galanter, M.B.J.K., Böhlke, J.K., A bacterial method for the nitrogen isotopic analysis of nitrate in seawater and freshwater. Anal. Chem. 73:17 (2001), 4145–4153.
Smith, K.A., (eds.) Nitrous Oxide and Climate Change, 2010, Earthscan.
Snider, D.M., Schiff, S.L., Spoelstra, J., 15N/14N and 18O/16O stable isotope ratios of nitrous oxide produced during denitrification in temperate forest soils. Geochem. Cosmochim. Acta 73:4 (2009), 877–888.
Snider, D.M., Venkiteswaran, J.J., Schiff, S.L., Spoelstra, J., Deciphering the oxygen isotope composition of nitrous oxide produced by nitrification. Glob. Chang. Biol. 18:1 (2012), 356–370.
Snider, D.M., Venkiteswaran, J.J., Schiff, S.L., Spoelstra, J., A new mechanistic model of δ18O-N2O formation by denitrification. Geochem. Cosmochim. Acta 112 (2013), 102–115.
Sutka, R.L., Ostrom, N.E., Ostrom, P.H., Breznak, J.A., Gandhi, H., Pitt, A.J., Li, F., Distinguishing nitrous oxide production from nitrification and denitrification on the basis of isotopomer abundances. Appl. Environ. Microbiol. 72:1 (2006), 638–644.
Syakila, A., Kroeze, C., The global nitrous oxide budget revisited. Greenh. Gas Meas. Manag. 1:1 (2011), 17–26.
Tan, K.H., Principles of soil chemistry. 2010, CRC press.
Teh, Y.A., Silver, W.L., Conrad, M.E., Oxygen effects on methane production and oxidation in humid tropical forest soils. Glob. Chang. Biol. 11:8 (2005), 1283–1297.
Toyoda, S., Yoshida, N., Koba, K., Isotopocule analysis of biologically produced nitrous oxide in various environments. Mass Spectrom. Rev. 36:2 (2017), 135–160.
Vesanto, J., Himberg, J., Alhoniemi, E., Parhankangas, J., SOM Toolbox for Matlab 5. 2000, Helsinki University of Technology, Finland, 109.
Vilain, G., Garnier, J., Tallec, G., Tournebize, J., Indirect N2O emissions from shallow groundwater in an agricultural catchment (Seine Basin, France). Biogeochemistry 111 (2012), 253–271.
von der Heide, C., Bӧttcher, J., Deurer, M., Weymann, D., Well, R., 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 (2008), 230–241.
Wassenaar, L.I., Douence, C., Altabet, M.A., Aggarwal, P.K., N and O isotope (δ15Nα, δ15Nβ, δ18O, δ17O) analyses of dissolved NO3− and NO2− by the Cd‐azide reduction method and N2O laser spectrometry. Rapid Commun. Mass Spectrom. 32:3 (2018), 184–194.
Well, R., Eschenbach, W., Flessa, H., von der Heide, C., Weymann, D., Are dual isotope and isotopomer ratios of N2O useful indicators for N2O turnover during denitrification in nitrate-contaminated aquifers?. Geochem. Cosmochim. Acta 90 (2012), 265–282.
Well, R., Flessa, H., Jaradat, F., Toyoda, S., Yoshida, N., Measurement of isotopomer signatures of N2O in groundwater. J. Geophys. Res. Biogeosci., 110(G2), 2005.
Weymann, D., Well, R., Flessa, H., von der Heide, C., Deurer, M., Meyer, K., Walther, W., Groundwater N2O emission factors of nitrate contaminated aquifers as derived from denitrification progress and N2O accumulation. Biogeosciences 5 (2008), 1215–1226.
Whiticar, M.J., Carbon and hydrogen isotope systematics of bacterial formation and oxidation of methane. Chem. Geol. 161:1–3 (1999), 291–314.
Widory, D., Kloppmann, W., Chery, L., Bonnin, J., Rochdi, H., Guinamant, J.L., Nitrate in groundwater: an isotopic multi-tracer approach. J. Contam. Hydrol. 72:1–4 (2004), 165–188.
Wilcock, R.J., Sorrell, B.K., Emissions of greenhouse gases CH4 and N2O from low-gradient streams in agriculturally developed catchments. Water, Air, Soil Pollut. 188:1–4 (2008), 155–170.
Worrall, F., Lancaster, A., The release of CO2 from riverwaters–the contribution of excess CO2 from groundwater. Biogeochemistry 76:2 (2005), 299–317.
Xue, D., Botte, J., De Baets, B., Accoe, F., Nestler, A., Taylor, P., et al. Present limitations and future prospects of stable isotope methods for nitrate source identification in surface-and groundwater. Water Res. 43:5 (2009), 1159–1170.
Yakovlev, V., Vystavna, Y., Diadin, D., Vergeles, Y., Nitrates in springs and rivers of East Ukraine: distribution, contamination and fluxes. Appl. Geochem. 53 (2015), 71–78.
Zou, Y., Hirono, Y., Yanai, Y., Hattori, S., Toyoda, S., Yoshida, N., Isotopomer analysis of nitrous oxide accumulated in soil cultivated with tea (Camellia sinensis) in Shizuoka, central Japan. Soil Biol. Biochem. 77 (2014), 276–291.
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