Geochemical modeling of a sustained shallow aquifer CO2 leakage field study and implications for leakage and site monitoring

Abstract A geochemical numerical modeling study was conducted to constrain processes occurring in field and laboratory experiments, simulating CO 2 leakage from geological storage on shallow potable aquifers. A leak was previously physically simulated in a shallow potable aquifer at Vrogum plantation, Western Denmark by injection of 1600 kg of gas phase CO 2 over 72 days. Here, a 1-dimensional reactive transport model was constructed based on field and laboratory results and subsequently used to explore the contributions of various geochemical processes to explain observed results from the carbonate free system. Finite gibbsite derived Al 3+ driven cation exchange is able to explain the majority of water chemistry change observed at Vrogum including: a pulse like effect showing a fast peak and return toward background levels for alkalinity and dissolved ion concentrations; and increasing and persistent acidification via buffering exhaustion. Model processes were supported further by simulation of a batch experiment conducted on the Vrogum glacial sand, employing the same processes and sediment parameters. The fitted reactive transport model was subsequently used to extend predictions and explore various scenarios. Extended predictions suggest the pulse of elevated ions travels with advective flow succeeded by a zone of increasing acidification. Model runs at higher P CO2 (implying greater depths) suggest amplification of effects, i.e., greater peaks and more rapid and severe acidification. Calcite limits acidification, however, induces additional Ca driven ion exchange giving rise to more significant chemistry change. Although a site specific model, results have significant implications for risks posed to water resources from CCS leakage and implementation of MMV programs.

[1]  P. Marker,et al.  Hydrogeochemical and mineralogical effects of sustained CO2 contamination in a shallow sandy aquifer: A field‐scale controlled release experiment , 2014 .

[2]  G. Zyvoloski,et al.  A numerical model for thermo-hydro-mechanical coupling in fractured rock , 1997 .

[3]  John E. McCray,et al.  A quantitative methodology to assess the risks to human health from CO2 leakage into groundwater , 2010 .

[4]  Jens T. Birkholzer,et al.  Geochemical modeling of changes in shallow groundwater chemistry observed during the MSU-ZERT CO2 injection experiment , 2012 .

[5]  Glenn E. Hammond,et al.  Elucidating geochemical response of shallow heterogeneous aquifers to CO2 leakage using high-performance computing: Implications for monitoring of CO2 sequestration , 2013 .

[6]  Jens T. Birkholzer,et al.  On modeling the potential impacts of CO2 sequestration on shallow groundwater: Transport of organics and co-injected H2S by supercritical CO2 to shallow aquifers , 2013 .

[7]  Mohamed Azaroual,et al.  Geochemical and solute transport modelling for CO2 storage, what to expect from it? , 2008 .

[8]  J. O. Reuss,et al.  Chemical processes governing soil and water acidification , 1987, Nature.

[9]  K. Jensen,et al.  Large‐scale dispersion experiments in a sandy aquifer in Denmark: Observed tracer movements and numerical analyses , 1993 .

[10]  Hari S. Viswanathan,et al.  CO2 leakage impacts on shallow groundwater: Field-scale reactive-transport simulations informed by observations at a natural analog site , 2013 .

[11]  R. Jakobsen,et al.  Risks attributable to water quality changes in shallow potable aquifers from geological carbon sequestration leakage into sediments of variable carbonate content , 2013 .

[12]  Jens Birkholzer,et al.  Reactive transport simulations to study groundwater quality changes in response to CO2 leakage from deep geological storage , 2009 .

[13]  M. Parmentier,et al.  Potential impacts of leakage from CO2 geological storage on geochemical processes controlling fresh groundwater quality: A review , 2014 .

[14]  Tarla Rai Peterson,et al.  Controversy in technology innovation: Contrasting media and expert risk perceptions of the alleged leakage at the Weyburn carbon dioxide storage demonstration project , 2013 .

[15]  Tran V. Long,et al.  Surface complexation modeling of groundwater arsenic mobility: Results of a forced gradient experiment in a Red River flood plain aquifer, Vietnam , 2012 .

[16]  Liange Zheng,et al.  Changes in the chemistry of shallow groundwater related to the 2008 injection of CO2 at the ZERT field site, Bozeman, Montana , 2010 .

[17]  D. Postma,et al.  Acidification, Buffering, and Salt Effects in the Unsaturated Zone of a Sandy Aquifer, Klosterhede, Denmark , 1995 .

[18]  F. Morel,et al.  Development of a data base for modelling adsorption of inorganics on iron and aluminum oxides , 1987 .

[19]  Carsten Vogt,et al.  Investigation of the geochemical impact of CO2 on shallow groundwater: design and implementation of a CO2 injection test in Northeast Germany , 2012, Environmental Earth Sciences.

[20]  P. Viet,et al.  Arsenic in groundwater of the Red River floodplain, Vietnam: Controlling geochemical processes and reactive transport modeling , 2007 .

[21]  Rajesh J. Pawar,et al.  The impact of CO2 on shallow groundwater chemistry: observations at a natural analog site and implications for carbon sequestration , 2010 .

[22]  Hari S. Viswanathan,et al.  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 , 2012 .

[23]  P. Audigane,et al.  Modeling of CO2 Leakage up Through an Abandoned Well from Deep Saline Aquifer to Shallow Fresh Groundwaters , 2011 .

[24]  David L. Freyberg,et al.  A natural gradient experiment on solute transport in a sand aquifer: 2. Spatial moments and the advection and dispersion of nonreactive tracers , 1986 .

[25]  M. Bruggenwert,et al.  Survey of experimental information on cation exchange in soil systems , 1979 .

[26]  D. Postma,et al.  The reactivity of iron oxides towards reductive dissolution with ascorbic acid in a shallow sandy aquifer (Rømø, Denmark) , 2006 .

[27]  C.A.J. Appelo,et al.  Reduction of Mn-oxides by ferrous iron in a flow system: column experiment and reactive transport modeling , 2000 .

[28]  S. S. Goldich A Study in Rock-Weathering , 1938, The Journal of Geology.

[29]  H. Sverdrup,et al.  Weathering of primary silicate minerals in the natural soil environment in relation to a chemical weathering model , 1988, Water, Air, and Soil Pollution.

[30]  Rasmus Jakobsen,et al.  Hydro-geochemical impact of CO2 leakage from geological storage on shallow potable aquifers: A field scale pilot experiment , 2012 .

[31]  Karsten Pruess,et al.  TOUGHREACT Version 2.0: A simulator for subsurface reactive transport under non-isothermal multiphase flow conditions , 2011, Comput. Geosci..

[32]  Jean-Michel Lemieux,et al.  Review: The potential impact of underground geological storage of carbon dioxide in deep saline aquifers on shallow groundwater resources , 2011 .

[33]  Jiemin Lu,et al.  Potential risks to freshwater resources as a result of leakage from CO2 geological storage: a batch-reaction experiment , 2010 .

[34]  R. Klusman,et al.  Comparison of surface and near-surface geochemical methods for detection of gas microseepage from carbon dioxide sequestration , 2011 .

[35]  E. Frind,et al.  Large‐Scale Dispersion in a Sandy Aquifer: Simulation of Subsurface Transport of Environmental Tritium , 1996 .

[36]  Liange Zheng,et al.  Effect of dissolved CO2 on a shallow groundwater system: a controlled release field experiment. , 2013, Environmental science & technology.

[37]  R. Wilkin,et al.  Geochemical impacts to groundwater from geologic carbon sequestration: controls on pH and inorganic carbon concentrations from reaction path and kinetic modeling. , 2010, Environmental science & technology.

[38]  David L. Parkhurst,et al.  Description of input and examples for PHREEQC version 3: a computer program for speciation, batch-reaction, one-dimensional transport, and inverse geochemical calculations , 2013 .

[39]  P. Jaffé,et al.  Potential Effect of CO2 Releases from Deep Reservoirs on the Quality of Fresh-Water Aquifers , 2003 .

[40]  J. Matter,et al.  Water–rock interactions during a CO2 injection field-test: Implications on host rock dissolution and alteration effects , 2009 .

[41]  V. Lagneau,et al.  CO2-water-mineral reactions during CO2 leakage: Geochemical and isotopic monitoring of a CO2 injection field test , 2014 .

[42]  Liange Zheng,et al.  A laboratory study of the initial effects of dissolved carbon dioxide (CO2) on metal release from shallow sediments , 2013 .

[43]  G. Bolt,et al.  Thermodynamics of heterovalent cation exchange reactions in a montmorillonite clay , 1968 .

[44]  Yue Hao,et al.  Geochemical detection of carbon dioxide in dilute aquifers , 2009, Geochemical transactions.

[45]  Claus Kjøller,et al.  Groundwater acidification and the mobilization of trace metals in a sandy aquifer. , 2004, Environmental science & technology.