Methane occurrence and origin in Dutch groundwater: from shallow aquifers to deep reservoirs

  • Gilian Schout KWR Water Research Institute, Nieuwegein, the Netherlands https://orcid.org/0000-0002-9066-1499
  • Jasper Griffioen Copernicus Institute of Sustainable Development, Utrecht University, Utrecht, the Netherlands; and TNO Geological Survey of the Netherlands, Utrecht, the Netherlands
  • Niels Hartog KWR Water Research Institute, Nieuwegein, the Netherlands; and Earth Sciences Department, Utrecht University, Utrecht, the Netherlands
  • Hans G.M. Eggenkamp Équipe de Géochimie des Isotopes Stables, Institut de Physique du Globe de Paris, Université de Paris, Paris, France; and ISOLAB BV, Geffen, The Netherlands
  • Dirk Gijsbert Cirkel KWR Water Research Institute, Nieuwegein, the Netherlands
Keywords: Groundwater methane, methane isotopes, deep groundwater, gas migration, stable chloride isotopes, well integrity failure

Abstract

Methane is a common constituent of groundwater with multiple possible origins. Elevated methane concentrations may also result from anthropogenically induced pathways between the deep and shallow subsurface caused by oil and gas production. A baseline characterisation of methane occurrence and origin in the subsurface of the Netherlands was made using a large set of methane concentrations in shallow groundwater (n = 12,219, up to 500 mbgs). Additionally, targeted sampling (n = 40) was carried out in (1) the shallow aquifers at locations where the presence of thermogenic methane was deemed most probable, such as above faults and known gas reservoirs, (2) deep groundwater aquifers below the depth of Neogene and Paleogene marine clays that form the hydrogeological base in the country and (3) geothermal formation waters at 1640–2625 mbgs. Median methane concentrations in shallow aquifers are relatively high from an international perspective (0.2 mg L−1). The highest methane concentrations (up to 120 mg L−1) are attributed to reactive organic matter in Holocene deposits and Pleistocene marine and glacial formations. However, elevated concentrations are also found at greater depth (100–160 m bgs) in Pleistocene aquifers in the eastern and southern inland areas of the Netherlands. Isotopic evidence and gas composition of naturally occurring methane indicate that methane in the targeted samples from shallow aquifers was of biogenic origin, and that methanogenesis predominantly occurs via CO2 reduction. Only trace amounts of methane (<0.2 mg L−1) were observed in the deep groundwater aquifers. A combination of methane and ethane isotopic composition showed that this methane consists of varying fractions of both biogenic and thermogenic origin. Methane in the geothermal reservoirs has an oil associated thermogenic origin. Overall, these findings highlight that future observations of thermogenic methane in Dutch shallow groundwater (post-Paleogene) are most probably linked to anthropogenically induced connections with the deep subsurface.

References

Atkins, M.L., Santos, I.R. & Maher, D.T., 2015. Groundwater methane in a potential coal seam gas extraction region. Journal of Hydrology: Regional Studies 4: 452–471. DOI: 10.1016/j.ejrh.2015.06.022.

Beekman, H.E., Eggenkamp, H.G.M. & Appelo, C.A.J., 2011. An integrated modelling approach to reconstruct complex solute transport mechanisms - Cl and δ37Cl in pore water of sediments from a former brackish lagoon in The Netherlands. Applied Geochemistry 26(3): 257–268. DOI: 10.1016/j.apgeochem.2010.11.026.

Bell, R.A., Darling, W.G., Ward, R.S., Basava-Reddi, L., Halwa, L., Manamsa, K., Dochartaigh, Ó. & BE, 2017. A baseline survey of dissolved methane in aquifers of Great Britain. Science of The Total Environment 601-602: 1803–1813. DOI: 10.1016/j.scitotenv.2017.05.191.

Bense, V.F., Van Balen, R.T. & De Vries, J.J., 2003. The impact of faults on the hydrogeological conditions in the Roer Valley Rift System: An overview. Netherlands Journal of Geosciences - Geologie en Mijnbouw 82(1): 41–54. DOI: 10.1017/S0016774600022782.

Bergen, F.van, Zijp, M., Nelskamp, S. & Kombrink, H., 2013. Shale gas evaluation of the Early Jurassic Posidonia Shale Formation and the Carboniferous Epen Formation in the Netherlands. In: Chatellier, J. & Jarvie, D. (eds): Critical Assessment of Shale Resource Plays: AAPG Memoir 103, Critical Assessment of Shale Resource Plays. AAPG Memoir 103, 24. DOI: 10.1306/134017221H53468.

Bol, J., 1991. Moeras- of brongas. In: Grondboor en Hamer, 150–153.

Buijs, E.A. & Stuurman, R.J., 2003. Herkomst van het brongas in Noord-Holland. Utrecht.

Cesar, J., Mayer, B. & Humez, P., 2021. A novel isotopic approach to distinguish primary microbial and thermogenic gases in shallow subsurface environments. Applied Geochemistry 131: 105048. DOI: 10.1016/j.apgeochem.2021.105048.

Christian, K.M., Lautz, L.K., Hoke, G.D., Siegel, D.I., Lu, Z. & Kessler, J., 2016. Methane occurrence is associated with sodium-rich valley waters in domestic wells overlying the Marcellus shale in New York State. Water Resources Research 52(1): 206–226. DOI: 10.1002/2015WR017805.

Cirkel, G., Hartog, N., De La, B., Gonzalez, L. & Stuyfzand, P., 2015. Methaan in ondiep Nederlands grondwater: verbinding met de diepe ondergrond? H2O-online.Google Scholar

de Gans, W., Beets, D.J. & Centineo, M.C., 2000. Late Saalian and Eemian deposits in the Amsterdam glacial basin. Netherlands Journal of Geosciences 79(2-3): 147–160. DOI: 10.1017/S0016774600021685.

de Vries, J.J., 2007. Groundwater. In: Wong, T.E., Batjes, D.A.J. & Jager, J. de (eds): Geology of the Netherlands. Royal Netherlands Academy of Arts and Sciences (Amsterdam): 354.

Desaulniers, D.E., Kaufmann, R.S., Cherry, J.A. & Bentley, H.W., 1986. 37Cl-35Cl variations in a diffusion-controlled groundwater system. Geochimica et Cosmochimica Acta 50(8): 1757–1764. DOI: 10.1016/0016-7037(86)90137-7.

Dufour, F.C., 1998. Groundwater in the Netherlands: invisible water on which we walk. TNO Geological Survey of the Netherlands (Delft).

Eggenkamp, H., 1994. δ37Cl: the geochemistry of chlorine isotopes. PhD thesis. Utrecht University (Utrecht).

Eggenkamp, H.G.M., Louvat, P., Agrinier, P., Bonifacie, M., Bekker, A., Krupenik, V., Griffioen, J., Horita, J., Brocks, J.J. & Bagheri, R., 2019. The bromine and chlorine isotope composition of primary halite deposits and their significance for the secular isotope composition of seawater. Geochimica et Cosmochimica Acta 264: 13–29. DOI: 10.1016/j.gca.2019.08.005.

Eltschlager, K.K., Hawkins, J.W., Ehler, W.C. & Baldassare, F.J., 2001. Technical Measures for the Investigation and Mitigation of Fugitive Methane Hazards in Areas of Coal Mining. U.S. Dep. Inter. Off. Surf. Min (Pittsburgh, PA).

Etiope, G., Baciu, C.L. & Schoell, M., 2011. Extreme methane deuterium, nitrogen and helium enrichment in natural gas from the Homorod seep (Romania). Chemical Geology 280(1-2): 89–96. DOI: 10.1016/j.chemgeo.2010.10.019.

Etiope, G., Feyzullayev, A. & Baciu, C.L., 2009. Terrestrial methane seeps and mud volcanoes: a global perspective of gas origin. Marine and Petroleum Geology 26(3): 333–344.

Etiope, G. & Ionescu, A., 2015. Low-temperature catalytic CO2 hydrogenation with geological quantities of ruthenium: a possible abiotic CH4 source in chromitite-rich serpentinized rocks. Geofluids 15(3): 438–452. DOI: 10.1111/gfl.12106.

Forde, O.N., Cahill, A.G., Mayer, K.U., Mayer, B., Simister, R.L., Finke, N., Crowe, S.A., Cherry, J.A. & Parker, B.L., 2019. Hydro-biogeochemical impacts of fugitive methane on a shallow unconfined aquifer. Science of The Total Environment 690: 1342–1354. DOI: 10.1016/j.scitotenv.2019.06.322.

Fortuin, N.P.M. & Willemsen, A., 2005. Exsolution of nitrogen and argon by methanogenesis in Dutch ground water. Journal of Hydrology 301(1-4): 1–13.

Godon, A., Jendrzejewski, N., Eggenkamp, H.G.M., Banks, D.A., Ader, M., Coleman, M.L. & Pineau, F., 2004. A cross-calibration of chlorine isotopic measurements and suitability of seawater as the international reference material. Chemical Geology 207(1-2): 1–12.

Griffioen, J., Klaver, G. & Westerhoff, W.E., 2016a. The mineralogy of suspended matter, fresh and Cenozoic sediments in the fluvio-deltaic Rhine-Meuse–Scheldt-Ems area, the Netherlands: An overview and review. Netherlands Journal of Geosciences - Geologie en Mijnbouw 95(1): 23–107. DOI: 10.1017/njg.2015.32.

Griffioen, J., Vermooten, S. & Janssen, G., 2013. Geochemical and palaeohydrological controls on the composition of shallow groundwater in the Netherlands. Applied Geochemistry 39: 129–149. DOI: 10.1016/j.apgeochem.2013.10.005.

Griffioen, J., Verweij, H. & Stuurman, R., 2016b. The composition of groundwater in Palaeogene and older formations in the Netherlands. A synthesis. Netherlands Journal of Geosciences 95(3): 349–372. DOI: 10.1017/njg.2016.19.

Humez, P., Mayer, B., Ing, J., Nightingale, M., Becker, V., Kingston, A., Akbilgic, O. & Taylor, S., 2016. Occurrence and origin of methane in groundwater in Alberta (Canada): gas geochemical and isotopic approaches. Science of The Total Environment 541: 1253–. DOI: 10.1016/j.scitotenv.2015.09.055.

Jackson, R.B., Vengosh, A., Carey, J.W., Davies, R.J., Darrah, T.H., Sullivan, F.O. & Gabrielle, P., 2014. The environmental costs and benefits of fracking. Annual Review of Environment and Resources 39(1): 327–362. DOI: 10.1146/annurev-environ-031113-144051.

Jackson, R.B., Vengosh, A., Darrah, T.H., Warner, N.R., Down, A., Poreda, R.J., Osborn, S.G., Zhao, K. & Karr, J.D., 2013. Increased stray gas abundance in a subset of drinking water wells near Marcellus shale gas extraction. Proceedings of the National Academy of Sciences 110(28): 11250–11251. DOI: 10.1073/pnas.1221635110.

Jager, J.de & Geluk, M.C., 2007. Petroleum Geology. In: Wong, T.E., Batjes, D.A.J. & Jager, J.de (eds): Geology of the Netherlands. Royal Netherlands Academy of Arts and Sciences, 241–264.

Kappelhof, J., Van Breukelen, B.M., Stuyfzand, P.J. & Drijver, B.C., 2006. Methaanwinning uit grondwater om methaanemissie te voorkomen. Haalbaarheidsstudie. IF Technology (Arnhem).

Kang, M., Kanno, C.M., Reid, M.C., Zhang, X., Mauzerall, D.L., Celia, M.A., Chen, Y. & Onstott, T.C., 2014. Direct measurements of methane emissions from abandoned oil and gas wells in Pennsylvania. Proceedings of the National Academy of Sciences 111(51): 18173–18177. DOI: 10.1073/pnas.1408315111.

Kaufmann, R.S. Chlorine in ground water: Stable isotope distribution (PhD Thesis), 1984, 137, The University of Arizona

Kulongoski, J.T., McMahon, P.B., Land, M., Wright, M.T., Johnson, T.A. & Landon, M.K., 2018. Origin of methane and sources of high concentrations in Los Angeles groundwater. Journal of Geophysical Research: Biogeosciences 123(3): 818–831. DOI: 10.1002/2017JG004026.

Lackey, G., Vasylkivska, V.S., Huerta, N.J., King, S. & Dilmore, R.M., 2019. Managing well leakage risks at a geologic carbon storage site with many wells. International Journal of Greenhouse Gas Control 88: 182–194. DOI: 10.1016/j.ijggc.2019.06.011.

Laier, T., Jørgensen, N.O., Buchardt, B., Cederberg, T. & Kuijpers, A., 1992. Accumulation and seepages of biogenic gas in northern Denmark. Continental Shelf Research 12(10): 1173–. DOI: 10.1016/0278-4343(92)90077-W.

Lollar, B.S., Lacrampe-Couloume, G., Slater, G.F., Ward, J., Moser, D.P., Gihring, T.M., Lin, L.H. & Onstott, T.C., 2006. Unravelling abiogenic and biogenic sources of methane in the Earth’s deep subsurface. Chemical Geology 226(3-4): 328–339. DOI: 10.1016/j.chemgeo.2005.09.027.

McIntosh, J.C., Hamilton, S.M., Grasby, S.E. & Osborn, S.G., 2014. Origin, distribution and hydrogeochemical controls on methane occurrences in shallow aquifers, southwestern Ontario. Applied Geochemistry 50: 37–52. DOI: 10.1016/j.apgeochem.2014.08.001.

McMahon, P.B., Belitz, K., Barlow, J.R.B. & Jurgens, B.C., 2017. Methane in aquifers used for public supply in the United States. Applied Geochemistry 84: 337–347. DOI: 10.1016/j.apgeochem.2017.07.014.

Meinardi, C.R., 1994. Groundwater recharge and travel times in the sandy regions of the Netherlands. VU University (Amsterdam).

Mendizabal, I., Stuyfzand, P.J. & Wiersma, A.P., 2011. Hydrochemical system analysis of public supply well fields, to reveal water-quality patterns and define groundwater bodies: the Netherlands. Hydrogeology Journal 19(1): 83–100. DOI: 10.1007/s10040-010-0614-0.

Milkov, A.V., 2010. Methanogenic biodegradation of petroleum in the West Siberian Basin (Russia): significance for formation of giant Cenomanian gas pools. AAPG Bulletin 94(10): 1485–1541. DOI: 10.1306/01051009122 .

Milkov, A.V. & Etiope, G., 2018. Revised genetic diagrams for natural gases based on a global dataset of >20,000 samples. Organic Geochemistry 125: 109–120. DOI: 10.1016/j.orggeochem.2018.09.002.

Ministry for Infrastructure and Environment, Ministry for Econimic Affairs and Climate, 2018, Structuurvisie Ondergrond. Den Haag (Netherlands).

Miyazaki, B., 2009. Well integrity: An overlooked source of risk and liability for underground natural gas storage. Lessons learned from incidents in the USA: Fig. 1. Geological Society, London, Special Publications 313(1): 163–172. DOI: 10.1144/sp313.11.

Molofsky, L.J., Connor, J.a, Farhat, Jr & A.S.W., S.K., 2011. Methane in Pennsylvania water wells unrelated to Marcellus shale fracturing. Oil Gas Journal 5: 54–67.

Molofsky, L.J., Connor, J.A., Wylie, A.S., Wagner, T. & Farhat, S.K., 2013. Evaluation of methane sources in groundwater in Northeastern Pennsylvania. Groundwater 51(3): 333–349.

Molofsky, L.J., Richardson, S.D., Gorody, A.W., Baldassare, F., Black, J.A., McHugh, T.E. & Connor, J.A., 2016. Effect of different sampling methodologies on measured methane concentrations in groundwater samples. Groundwater 54(5): 669–680. DOI: 10.1111/gwat.12415.

Molofsky, L.J., Richardson, S.D., Gorody, A.W., Baldassare, F., Connor, J.A., McHugh, T.E., Smith, A.P., Wylie, A.S. & Wagner, T., 2018. Purging and other sampling variables affecting dissolved methane concentration in water supply wells. Science of The Total Environment 618: 998–1007. DOI: 10.1016/j.scitotenv.2017.09.077.

Mook, W.G. & Plicht, J. Van Der, 1999. Reporting radiocarbon activities and concentrations. Radiocarbon 41(3): 227–239.

Nicot, J.P., Mickler, P., Larson, T., Clara Castro, M., Darvari, R., Uhlman, K. & Costley, R., 2017. Methane occurrences in aquifers overlying the Barnett Shale play with a focus on Parker County, Texas. Groundwater 55(4): 469–481. DOI: 10.1111/gwat.12508

Nisbet, E.G., Manning, M.R., Dlugokencky, E.J., Fisher, R.E., Lowry, D., Michel, S.E., Myhre, C.L., Platt, S.M., Allen, G., Bousquet, P., Brownlow, R., Cain, M., France, J.L., Hermansen, O., Hossaini, R., Jones, A.E., Levin, I., Manning, A.C., Myhre, G., Pyle, J.A., Vaughn, B.H., Warwick, N.J. & White, J.W.C., 2019. Very strong atmospheric methane growth in the 4 Years 2014-2017: implications for the paris agreement. Global Biogeochemical Cycles 33(3): 318–342. DOI: 10.1029/2018GB006009.

NLOG, 2020. Netherlands oil and gas portal [WWW document]. https://www.nlog.nl/ (accessed 1.2.20).

Osborn, S.G., Vengosh, A., Warner, N.R. & Jackson, R.B., 2011. Methane contamination of drinking water accompanying gas-well drilling and hydraulic fracturing. Proceedings of the National Academy of Sciences 108(20): E665–E666. DOI: 10.1073/pnas.1100682108.

Rice, A.K., Lackey, G., Proctor, J. & Singha, K., 2018. Groundwater-quality hazards of methane leakage from hydrocarbon wells: a review of observational and numerical studies and four testable hypotheses. WIREs Water 5(4): e1283.10.1002/wat2.1283.

Schloemer, S., Elbracht, J., Blumenberg, M. & Illing, C.J., 2016. Distribution and origin of dissolved methane, ethane and propane in shallow groundwater of Lower Saxony, Germany. Applied Geochemistry 67: 118–132. DOI: 10.1016/j.apgeochem.2016.02.005.

Schout, G., Griffioen, J., Hassanizadeh, S.M., Cardon de Lichtbuer, G. & Hartog, N., 2019. Occurrence and fate of methane leakage from cut and buried abandoned gas wells in the Netherlands. Science of The Total Environment 659: 773–782. DOI: 10.1016/j.scitotenv.2018.12.339.

Schout, G., Hartog, N., Hassanizadeh, S.M. & Griffioen, J., 2017. Impact of an historic underground gas well blowout on the current methane chemistry in a shallow groundwater system. Proceedings of the National Academy of Sciences 115(2): 296–301. DOI: 10.1073/pnas.1711472115.

Schout, G., Hartog, N., Hassanizadeh, S.M., Helmig, R. & Griffioen, J., 2020. Impact of groundwater flow on methane gas migration and retention in unconsolidated aquifers. Journal of Contaminant Hydrology 230: 103619. DOI: 10.1016/j.jconhyd.2020.103619.

Schroot, B.M., Klaver, G.T. & Schüttenhelm, R.T.E., 2005. Surface and subsurface expressions of gas seepage to the seabed - examples from the Southern North Sea. Marine and Petroleum Geology 22(4): 499–515. DOI: 10.1016/j.marpetgeo.2004.08.007.

Siegel, D.I., Azzolina, N.A., Smith, B.J., Perry, A.E. & Bothun, R.L., 2015. Methane concentrations in water wells unrelated to proximity to existing oil and gas wells in northeastern Pennsylvania. Environmental Science & Technology 49(7): 4106–4112. DOI: 10.1021/es505775c.

Sissingh, W., 2004. Palaeozoic and Mesozoic igneous activity in the Netherlands: a tectonomagmatic review. Netherlands Journal of Geosciences - Geologie en Mijnbouw 83(2): 113–134. DOI: 10.1017/S0016774600020084.

SodM, 2019, De integriteit van onshore putten in Nederland. Den Haag.

Stuyfzand, P.J., Luers, F. & Reijnen, G.K., 1994. Geohydrochemische aspecten van methaan in grondwater in Nederland. H2O 17: 500–506.

ten Veen, J.H., van Gessel, S.F. & den Dulk, M., 2012. Thin- and thick-skinned salt tectonics in the Netherlands; a quantitative approach. Netherlands Journal of Geosciences - Geologie en Mijnbouw 91(4): 447–464. DOI: 10.1017/S0016774600000330.

Ten Veen, J.H., Verweij, H., Donders, T., Geel, K., de Bruin, G., Munsterman, D., Verreussel, R., Daza Cajigal, V., Harding, R. & Cremer, H., 2013. Anatomy of the Ccenozoic Eeridanos Hhydrocarbon Ssystem. Utrecht.

Thielemann, T., Lücke, A., Schleser, G.H. & Littke, R., 2000. Methane exchange between coal-bearing basins and the atmosphere: the Ruhr Basin and the Lower Rhine Embayment, Germany. Organic Geochemistry 31(12): 1387–1408. DOI: 10.1016/S0146-6380(00)00104-2.

TNO, 2018. Inventarisatie aantoonbare effecten voor mens en milieu als gevolg van historische conventionele frackoperaties. Utrecht.

Valstar, J.R. & Goorden, N., 2016. Far-field transport modelling for a repository in the Boom Clay in the Netherlands. Netherlands Journal of Geosciences 95(3): 337–347. DOI: 10.1017/njg.2016.13.

Van Der Kemp, W.J.M., Appelo, C.A.J. & Walraevens, K., 2000. Inverse chemical modeling and radiocarbon dating of palaeogroundwaters: the Tertiary Ledo-Paniselian aquifer in Flanders, Belgium. Water Resources Research 36(5): 1277–1287. DOI: 10.1029/1999WR900357.

van Thienen-Visser, K. & Breunese, J.N., 2015. Induced seismicity of the Groningen gas field: history and recent developments. The Leading Edge 34(6): 664–671. DOI: 10.1190/tle34060664.1.

Vengosh, A., Jackson, R.B., Warner, N., Darrah, T.H. & Kondash, A., 2014. A critical. review of the risks to water resources from unconventional shale gas development and hydraulic fracturing in the United States. Environmental Science & Technology 48(15): 8334–8348. DOI: 10.1021/es405118y.

Verhoef, E., Neeft, E., Grupa, J. & Poley, A. Outline of a disposal concept in clay (2014).

Verweij, J.M., Nelskamp, S.N., Ten Veen, J.H., De Bruin, G., Geel, K. & Donders, T.H., 2018. Generation, migration, entrapment and leakage of microbial gas in the Dutch part of the Southern North Sea Delta. Marine and Petroleum Geology 97: 493–516. DOI: 10.1016/j.marpetgeo.2018.07.034.

Verweij, J.M., Simmelink, H.J., Underschultz, J. & Witmans, N., 2012. Pressure and fluid dynamic characterisation of the Dutch subsurface. Netherlands Journal of Geosciences - Geologie en Mijnbouw 91(4): 465–490. DOI: 10.1017/S0016774600000342.

Warner, N.R., Jackson, R.B., Darrah, T.H., Osborn, S.G., Down, A., Zhao, K., White, A. & Vengosh, A., 2012. Geochemical evidence for possible natural migration of Marcellus Formation brine to shallow aquifers in Pennsylvania. Proceedings of the National Academy of Sciences 109(30): 11961–11966.

Whiticar, M.J., 1999. Carbon and hydrogen isotope systematics of bacterial formation and oxidation of methane. Chemical Geology 161(1-3): 291–314. DOI: 10.1016/s0009-2541(99)00092-3.

Williams, G.M. & Aitkenhead, N., 1991. Lessons from Loscoe: the uncontrolled migration of landfill gas. Quarterly Journal of Engineering Geology 24(2): 191–207. DOI: 10.1144/GSL.QJEG.1991.024.02.03.
Published
2024-11-15
How to Cite
Schout , G., Griffioen , J., Hartog , N., Eggenkamp , H. G., & Cirkel , D. G. (2024). Methane occurrence and origin in Dutch groundwater: from shallow aquifers to deep reservoirs. Netherlands Journal of Geosciences, 103. https://doi.org/10.1017/njg.2024.20
Section
Regular paper