Modeling the potential impacts of CO 2 sequestration on shallow groundwater: The fate of trace metals and organic compounds before and after leakage stops

Zheng, Liange; Spycher, Nicolas

doi:10.1002/ghg.1728

Title: Modeling the potential impacts of CO ₂ sequestration on shallow groundwater: The fate of trace metals and organic compounds before and after leakage stops

Journal Article · Thu Sep 28 00:00:00 EDT 2017 · Greenhouse Gases: Science and Technology

DOI:https://doi.org/10.1002/ghg.1728· OSTI ID:1476617

^[1]; Spycher, Nicolas ^[1]

Lawrence Berkeley National Laboratory, Berkeley CA USA

Large-scale deployment of CO₂ geological sequestration requires understanding and assessing the risks of such an operation. One of these risks is the potential contamination of groundwater by CO₂/brine leakage into shallow aquifers. Although our understanding of this issue has improved significantly over the last decade, several questions still need to be better addressed, including the fate of organic constituents, the dominant source of trace metals (are they mainly coming from aquifer sediments, or leaking brine), and whether the trace metals released during the leakage phase recover to background levels if the leakage were to be detected and stopped. In this paper, reactive transport simulations that model the behavior of trace metals and organic compounds in response to the leakage of CO₂ and brine into a shallow aquifer are presented to address these questions. Model results show that the metals and organic compounds brought by the leaking brine form a plume at the bottom of the aquifer because the density of the brine is higher than that of groundwater. In contrast, metals are mobilized by CO₂ over a larger vertical extent because of the spreading of gaseous CO₂ by buoyancy. The concentration of organic contaminants is strongly attenuated by adsorption and degradation, with degradation playing the major role in the modeled scenarios. Although the leaking brine is assumed to contain elevated concentrations of As, Pb, Cd, and Ba, it does not contribute significantly to the contamination of the modeled shallow aquifer by these elements. Once the leakage stops, mobilized organic compounds that undergo degradation vanish, while less degradable compounds linger for a longer time; the dissolved concentrations of trace metals decrease significantly, as a result of re-sorption and reversal of processes leading to Ca-driven cation exchange.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Fossil Energy (FE)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1476617

Journal Information:: Greenhouse Gases: Science and Technology, Vol. 8, Issue 1; ISSN 2152-3878

Publisher:: Society of Chemical Industry, WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 14 works

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References (55)

Developing a robust geochemical and reactive transport model to evaluate possible sources of arsenic at the CO2 sequestration natural analog site in Chimayo, New Mexico Viswanathan, Hari; Dai, Zhenxue; Lopano, Christina International Journal of Greenhouse Gas Control, Vol. 10 https://doi.org/10.1016/j.ijggc.2012.06.007	journal	September 2012
Trace metal modeling of groundwater–gas–rock interactions in a volcanic aquifer: Mount Vesuvius, Southern Italy Aiuppa, Alessandro; Federico, Cinzia; Allard, Patrick Chemical Geology, Vol. 216, Issue 3-4 https://doi.org/10.1016/j.chemgeo.2004.11.017	journal	March 2005
A laboratory study of the initial effects of dissolved carbon dioxide (CO2) on metal release from shallow sediments Varadharajan, Charuleka; Tinnacher, Ruth M.; Pugh, John D. International Journal of Greenhouse Gas Control, Vol. 19 https://doi.org/10.1016/j.ijggc.2013.08.017	journal	November 2013
Metal release from limestones at high partial-pressures of CO2 Wunsch, Assaf; Navarre-Sitchler, Alexis K.; Moore, Joel Chemical Geology, Vol. 363 https://doi.org/10.1016/j.chemgeo.2013.10.036	journal	January 2014
On the mobilization of metals by CO ₂ leakage into shallow aquifers: exploring release mechanisms by modeling field and laboratory experiments Zheng, Liange; Spycher, Nicolas; Varadharajan, Charuleka Greenhouse Gases: Science and Technology, Vol. 5, Issue 4 https://doi.org/10.1002/ghg.1493	journal	April 2015
Key factors for determining groundwater impacts due to leakage from geologic carbon sequestration reservoirs Carroll, Susan A.; Keating, Elizabeth; Mansoor, Kayyum International Journal of Greenhouse Gas Control, Vol. 29 https://doi.org/10.1016/j.ijggc.2014.07.007	journal	October 2014
Goethite adsorption of Cu(II), Pb(II), Cd(II), and Zn(II) in the presence of sulfate: Properties of the ternary complex Swedlund, Peter J.; Webster, Jenny G.; Miskelly, Gordon M. Geochimica et Cosmochimica Acta, Vol. 73, Issue 6 https://doi.org/10.1016/j.gca.2008.12.007	journal	March 2009
Evaluating impacts of CO2 intrusion into an unconsolidated aquifer: I. Experimental data Lawter, Amanda; Qafoku, Nikolla P.; Wang, Guohui International Journal of Greenhouse Gas Control, Vol. 44 https://doi.org/10.1016/j.ijggc.2015.07.009	journal	January 2016
Trace Metal Source Terms in Carbon Sequestration Environments Karamalidis, Athanasios K.; Torres, Sharon G.; Hakala, J. Alexandra Environmental Science & Technology, Vol. 47, Issue 1 https://doi.org/10.1021/es304832m	journal	August 2012
Supercritical extraction of contaminants from soils and sediments Anitescu, G.; Tavlarides, L. L. The Journal of Supercritical Fluids, Vol. 38, Issue 2 https://doi.org/10.1016/j.supflu.2006.03.024	journal	September 2006
Chemical characterisation of produced water from four offshore oil production platforms in the North Sea Røe Utvik, Toril I. Chemosphere, Vol. 39, Issue 15 https://doi.org/10.1016/S0045-6535(99)00171-X	journal	December 1999
Diffusion and adsorption of benzene in Regina clay Donahue, Robert B.; Barbour, S. Lee; Headley, John V. Canadian Geotechnical Journal, Vol. 36, Issue 3 https://doi.org/10.1139/t99-017	journal	October 1999
Potential Impacts of Leakage from Deep CO ₂ Geosequestration on Overlying Freshwater Aquifers Little, Mark G.; Jackson, Robert B. Environmental Science & Technology, Vol. 44, Issue 23 https://doi.org/10.1021/es102235w	journal	December 2010
TOUGHREACT Version 2.0: A simulator for subsurface reactive transport under non-isothermal multiphase flow conditions Xu, Tianfu; Spycher, Nicolas; Sonnenthal, Eric Computers & Geosciences, Vol. 37, Issue 6 https://doi.org/10.1016/j.cageo.2010.10.007	journal	June 2011
Gas-water-rock interactions in Frio Formation following CO2 injection: Implications for the storage of greenhouse gases in sedimentary basins Kharaka, Y. K.; Cole, D. R.; Hovorka, S. D. Geology, Vol. 34, Issue 7 https://doi.org/10.1130/G22357.1	journal	January 2006
Changes in the chemistry of shallow groundwater related to the 2008 injection of CO₂ at the ZERT field site, Bozeman, Montana Kharaka, Yousif K.; Thordsen, James J.; Kakouros, Evangelos Environmental Earth Sciences, Vol. 60, Issue 2, p. 273-284 https://doi.org/10.1007/s12665-009-0401-1	journal	December 2009
Dissolution of a mineral phase in potable aquifers due to CO2 releases from deep formations; effect of dissolution kinetics Wang, Sookyun; Jaffe, Peter R. Energy Conversion and Management, Vol. 45, Issue 18-19 https://doi.org/10.1016/j.enconman.2004.01.002	journal	November 2004
Surface complexation modelling of Cd(II), Cu(II), Ni(II), Pb(II) and Zn(II) adsorption onto kaolinite Gu, Xueyuan; Evans, Les J. Geochimica et Cosmochimica Acta, Vol. 72, Issue 2 https://doi.org/10.1016/j.gca.2007.09.032	journal	January 2008
Evaluating impacts of CO2 intrusion into an unconsolidated aquifer: II. Modeling results Zheng, Liange; Qafoku, Nikolla P.; Lawter, Amanda International Journal of Greenhouse Gas Control, Vol. 44 https://doi.org/10.1016/j.ijggc.2015.07.001	journal	January 2016
Potential risks to freshwater resources as a result of leakage from CO2 geological storage: a batch-reaction experiment Lu, Jiemin; Partin, Judson W.; Hovorka, Susan D. Environmental Earth Sciences, Vol. 60, Issue 2 https://doi.org/10.1007/s12665-009-0382-0	journal	December 2009
Thermoddem: A geochemical database focused on low temperature water/rock interactions and waste materials Blanc, Ph.; Lassin, A.; Piantone, P. Applied Geochemistry, Vol. 27, Issue 10 https://doi.org/10.1016/j.apgeochem.2012.06.002	journal	October 2012
Modeling the impact of carbon dioxide leakage into an unconfined, oxidizing carbonate aquifer Bacon, Diana H.; Qafoku, Nikolla P.; Dai, Zhenxue International Journal of Greenhouse Gas Control, Vol. 44 https://doi.org/10.1016/j.ijggc.2015.04.008	journal	January 2016
Modelling the adsorption of Cd(II), Cu(II), Ni(II), Pb(II), and Zn(II) onto Fithian illite Gu, Xueyuan; Evans, Les J. Journal of Colloid and Interface Science, Vol. 307, Issue 2 https://doi.org/10.1016/j.jcis.2006.11.022	journal	March 2007
Metal Release from Sandstones under Experimentally and Numerically Simulated CO ₂ Leakage Conditions Kirsch, Katie; Navarre-Sitchler, Alexis K.; Wunsch, Assaf Environmental Science & Technology, Vol. 48, Issue 3 https://doi.org/10.1021/es403077b	journal	January 2014
Effect of Dissolved CO ₂ on a Shallow Groundwater System: A Controlled Release Field Experiment Trautz, Robert C.; Pugh, John D.; Varadharajan, Charuleka Environmental Science & Technology, Vol. 47, Issue 1 https://doi.org/10.1021/es301280t	journal	August 2012
ECO2N: A TOUGH2 Fluid Property Module for Mixtures of Water, NaCl,and CO2 Pruess, Karsten https://doi.org/10.2172/877331	report	August 2005
Geochemical Impacts to Groundwater from Geologic Carbon Sequestration: Controls on pH and Inorganic Carbon Concentrations from Reaction Path and Kinetic Modeling Wilkin, Richard T.; DiGiulio, Dominic C. Environmental Science & Technology, Vol. 44, Issue 12 https://doi.org/10.1021/es100559j	journal	June 2010
Geochemical Implications of Gas Leakage associated with Geologic CO ₂ Storage—A Qualitative Review Harvey, Omar R.; Qafoku, Nikolla P.; Cantrell, Kirk J. Environmental Science & Technology, Vol. 47, Issue 1 https://doi.org/10.1021/es3029457	journal	August 2012
Competitive Adsorption of Arsenate and Arsenite on Oxides and Clay Minerals Goldberg, Sabine Soil Science Society of America Journal, Vol. 66, Issue 2 https://doi.org/10.2136/sssaj2002.4130	journal	January 2002
Geochemical modeling of changes in shallow groundwater chemistry observed during the MSU-ZERT CO2 injection experiment Zheng, Liange; Apps, John A.; Spycher, Nicolas International Journal of Greenhouse Gas Control, Vol. 7 https://doi.org/10.1016/j.ijggc.2011.10.003	journal	March 2012
Hydro-geochemical impact of CO2 leakage from geological storage on shallow potable aquifers: A field scale pilot experiment Cahill, Aaron G.; Jakobsen, Rasmus International Journal of Greenhouse Gas Control, Vol. 19 https://doi.org/10.1016/j.ijggc.2013.03.015	journal	November 2013
Biodegradation and transport of benzene, toluene, and xylenes in a simulated aquifer: comparison of modelled and experimental results Jean, Jiin-Shuh; Tsai, Ching-Lang; Ju, Shen-Haw Hydrological Processes, Vol. 16, Issue 16 https://doi.org/10.1002/hyp.1093	journal	January 2002
Review: The potential impact of underground geological storage of carbon dioxide in deep saline aquifers on shallow groundwater resources Lemieux, Jean-Michel Hydrogeology Journal, Vol. 19, Issue 4 https://doi.org/10.1007/s10040-011-0715-4	journal	April 2011
Assessing risk to fresh water resources from long term CO2 injection–laboratory and field studies Smyth, Rebecca C.; Hovorka, Susan D.; Lu, Jiemin Energy Procedia, Vol. 1, Issue 1 https://doi.org/10.1016/j.egypro.2009.01.255	journal	February 2009
Modeling of CO2 Leakage up Through an Abandoned Well from Deep Saline Aquifer to Shallow Fresh Groundwaters Humez, Pauline; Audigane, Pascal; Lions, Julie Transport in Porous Media, Vol. 90, Issue 1 https://doi.org/10.1007/s11242-011-9801-2	journal	August 2011
Correlation of benzene, 1,1,1-trichloroethane, and naphthalene distribution coefficients to the characteristics of aquifer materials with low organic carbon content Larsen, Thomas; Kjeldsen, Peter; Christensen, Thomas H. Chemosphere, Vol. 24, Issue 8 https://doi.org/10.1016/0045-6535(92)90191-S	journal	April 1992
Evaluation of Potential Changes in Groundwater Quality in Response to CO2 Leakage from Deep Geologic Storage Apps, J. A.; Zheng, L.; Zhang, Y. Transport in Porous Media, Vol. 82, Issue 1 https://doi.org/10.1007/s11242-009-9509-8	journal	January 2010
Investigation of the geochemical impact of CO2 on shallow groundwater: design and implementation of a CO2 injection test in Northeast Germany Peter, Anita; Lamert, Hendrik; Beyer, Matthias Environmental Earth Sciences, Vol. 67, Issue 2 https://doi.org/10.1007/s12665-012-1700-5	journal	May 2012
Probabilistic evaluation of shallow groundwater resources at a hypothetical carbon sequestration site Dai, Zhenxue; Keating, Elizabeth; Bacon, Diana Scientific Reports, Vol. 4, Issue 1 https://doi.org/10.1038/srep04006	journal	March 2014
CO2-H2O mixtures in the geological sequestration of CO2. II. Partitioning in chloride brines at 12–100°C and up to 600 bar Spycher, Nicolas; Pruess, Karsten Geochimica et Cosmochimica Acta, Vol. 69, Issue 13 https://doi.org/10.1016/j.gca.2005.01.015	journal	July 2005
On modeling the potential impacts of CO2 sequestration on shallow groundwater: Transport of organics and co-injected H2S by supercritical CO2 to shallow aquifers Zheng, Liange; Spycher, Nicolas; Birkholzer, Jens International Journal of Greenhouse Gas Control, Vol. 14 https://doi.org/10.1016/j.ijggc.2013.01.014	journal	May 2013
Geochemistry, radiocarbon ages, and paleorecharge conditions along a transect in the central High Plains aquifer, southwestern Kansas, USA McMahon, P. B.; Böhlke, J. K.; Christenson, S. C. Applied Geochemistry, Vol. 19, Issue 11 https://doi.org/10.1016/j.apgeochem.2004.05.003	journal	November 2004
Evidence for Very Tight Sequestration of BTEX Compounds in Manufactured Gas Plant Soils Based on Selective Supercritical Fluid Extraction and Soil/Water Partitioning Hawthorne, Steven B.; Miller, David J. Environmental Science & Technology, Vol. 37, Issue 16 https://doi.org/10.1021/es020899f	journal	August 2003
Environmental consequences of potential leaks of CO2 in soil Wei, Yang; Maroto-Valer, Mercedes; Steven, Michael D. Energy Procedia, Vol. 4 https://doi.org/10.1016/j.egypro.2011.02.239	journal	January 2011
Comparison of Arsenic(V) and Arsenic(III) Sorption onto Iron Oxide Minerals: Implications for Arsenic Mobility Dixit, Suvasis; Hering, Janet G. Environmental Science & Technology, Vol. 37, Issue 18 https://doi.org/10.1021/es030309t	journal	September 2003
The impact of CO2 on shallow groundwater chemistry: observations at a natural analog site and implications for carbon sequestration Keating, Elizabeth H.; Fessenden, Julianna; Kanjorski, Nancy Environmental Earth Sciences, Vol. 60, Issue 3 https://doi.org/10.1007/s12665-009-0192-4	journal	June 2009
Applicability of aquifer impact models to support decisions at CO2 sequestration sites Keating, Elizabeth; Bacon, Diana; Carroll, Susan International Journal of Greenhouse Gas Control, Vol. 52 https://doi.org/10.1016/j.ijggc.2016.07.001	journal	September 2016
Impacts of elevated dissolved CO2 on a shallow groundwater system: Reactive transport modeling of a controlled-release field test Zheng, Liange; Spycher, Nicolas; Bianchi, Marco Chemical Geology, Vol. 447 https://doi.org/10.1016/j.chemgeo.2016.10.027	journal	December 2016
Potential chemical impacts of CO2 leakage on underground source of drinking water assessed by quantitative risk analysis Xiao, Ting; McPherson, Brian; Pan, Feng International Journal of Greenhouse Gas Control, Vol. 50 https://doi.org/10.1016/j.ijggc.2016.04.009	journal	July 2016
Potential environmental issues of CO2 storage in deep saline aquifers: Geochemical results from the Frio-I Brine Pilot test, Texas, USA Kharaka, Yousif K.; Thordsen, James J.; Hovorka, Susan D. Applied Geochemistry, Vol. 24, Issue 6 https://doi.org/10.1016/j.apgeochem.2009.02.010	journal	June 2009
TOUGH2 User's Guide Version 2 Pruess, K.; Oldenburg, C.M.; Moridis, G.J. https://doi.org/10.2172/751729 LBNL--43134	report	November 1999
Modeling the adsorption of Cd (II), Cu (II), Ni (II), Pb (II) and Zn (II) onto montmorillonite Gu, Xueyuan; Evans, Les J.; Barabash, Sarah J. Geochimica et Cosmochimica Acta, Vol. 74, Issue 20 https://doi.org/10.1016/j.gca.2010.07.016	journal	October 2010
Single-well push–pull test for assessing potential impacts of CO2 leakage on groundwater quality in a shallow Gulf Coast aquifer in Cranfield, Mississippi Yang, Changbing; Mickler, Patrick J.; Reedy, Robert International Journal of Greenhouse Gas Control, Vol. 18 https://doi.org/10.1016/j.ijggc.2012.12.030	journal	October 2013
Transport of organic contaminants mobilized from coal through sandstone overlying a geological carbon sequestration reservoir Zhong, L.; Cantrell, K. J.; Bacon, D. H. International Journal of Greenhouse Gas Control, Vol. 21 https://doi.org/10.1016/j.ijggc.2013.12.014	journal	February 2014
On mobilization of lead and arsenic in groundwater in response to CO2 leakage from deep geological storage Zheng, Liange; Apps, John A.; Zhang, Yingqi Chemical Geology, Vol. 268, Issue 3-4 https://doi.org/10.1016/j.chemgeo.2009.09.007	journal	November 2009

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