DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

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

Abstract

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 andmore » 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.« less

Authors:
ORCiD logo [1];  [1]
  1. Lawrence Berkeley National Laboratory, Berkeley CA USA
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Fossil Energy (FE)
OSTI Identifier:
1476617
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Greenhouse Gases: Science and Technology
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2152-3878
Publisher:
Society of Chemical Industry, Wiley
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 54 ENVIRONMENTAL SCIENCES

Citation Formats

Zheng, Liange, and Spycher, Nicolas. Modeling the potential impacts of CO 2 sequestration on shallow groundwater: The fate of trace metals and organic compounds before and after leakage stops. United States: N. p., 2017. Web. doi:10.1002/ghg.1728.
Zheng, Liange, & Spycher, Nicolas. Modeling the potential impacts of CO 2 sequestration on shallow groundwater: The fate of trace metals and organic compounds before and after leakage stops. United States. https://doi.org/10.1002/ghg.1728
Zheng, Liange, and Spycher, Nicolas. Thu . "Modeling the potential impacts of CO 2 sequestration on shallow groundwater: The fate of trace metals and organic compounds before and after leakage stops". United States. https://doi.org/10.1002/ghg.1728. https://www.osti.gov/servlets/purl/1476617.
@article{osti_1476617,
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},
author = {Zheng, Liange and Spycher, Nicolas},
abstractNote = {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.},
doi = {10.1002/ghg.1728},
journal = {Greenhouse Gases: Science and Technology},
number = 1,
volume = 8,
place = {United States},
year = {Thu Sep 28 00:00:00 EDT 2017},
month = {Thu Sep 28 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 14 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

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
journal, September 2012

  • Viswanathan, Hari; Dai, Zhenxue; Lopano, Christina
  • International Journal of Greenhouse Gas Control, Vol. 10
  • DOI: 10.1016/j.ijggc.2012.06.007

Trace metal modeling of groundwater–gas–rock interactions in a volcanic aquifer: Mount Vesuvius, Southern Italy
journal, March 2005


A laboratory study of the initial effects of dissolved carbon dioxide (CO2) on metal release from shallow sediments
journal, November 2013

  • Varadharajan, Charuleka; Tinnacher, Ruth M.; Pugh, John D.
  • International Journal of Greenhouse Gas Control, Vol. 19
  • DOI: 10.1016/j.ijggc.2013.08.017

Metal release from limestones at high partial-pressures of CO2
journal, January 2014


On the mobilization of metals by CO 2 leakage into shallow aquifers: exploring release mechanisms by modeling field and laboratory experiments
journal, April 2015

  • Zheng, Liange; Spycher, Nicolas; Varadharajan, Charuleka
  • Greenhouse Gases: Science and Technology, Vol. 5, Issue 4
  • DOI: 10.1002/ghg.1493

Key factors for determining groundwater impacts due to leakage from geologic carbon sequestration reservoirs
journal, October 2014

  • Carroll, Susan A.; Keating, Elizabeth; Mansoor, Kayyum
  • International Journal of Greenhouse Gas Control, Vol. 29
  • DOI: 10.1016/j.ijggc.2014.07.007

Goethite adsorption of Cu(II), Pb(II), Cd(II), and Zn(II) in the presence of sulfate: Properties of the ternary complex
journal, March 2009

  • Swedlund, Peter J.; Webster, Jenny G.; Miskelly, Gordon M.
  • Geochimica et Cosmochimica Acta, Vol. 73, Issue 6
  • DOI: 10.1016/j.gca.2008.12.007

Evaluating impacts of CO2 intrusion into an unconsolidated aquifer: I. Experimental data
journal, January 2016

  • Lawter, Amanda; Qafoku, Nikolla P.; Wang, Guohui
  • International Journal of Greenhouse Gas Control, Vol. 44
  • DOI: 10.1016/j.ijggc.2015.07.009

Trace Metal Source Terms in Carbon Sequestration Environments
journal, August 2012

  • Karamalidis, Athanasios K.; Torres, Sharon G.; Hakala, J. Alexandra
  • Environmental Science & Technology, Vol. 47, Issue 1
  • DOI: 10.1021/es304832m

Supercritical extraction of contaminants from soils and sediments
journal, September 2006


Diffusion and adsorption of benzene in Regina clay
journal, October 1999

  • Donahue, Robert B.; Barbour, S. Lee; Headley, John V.
  • Canadian Geotechnical Journal, Vol. 36, Issue 3
  • DOI: 10.1139/t99-017

Potential Impacts of Leakage from Deep CO 2 Geosequestration on Overlying Freshwater Aquifers
journal, December 2010

  • Little, Mark G.; Jackson, Robert B.
  • Environmental Science & Technology, Vol. 44, Issue 23
  • DOI: 10.1021/es102235w

TOUGHREACT Version 2.0: A simulator for subsurface reactive transport under non-isothermal multiphase flow conditions
journal, June 2011


Changes in the chemistry of shallow groundwater related to the 2008 injection of CO2 at the ZERT field site, Bozeman, Montana
journal, December 2009

  • Kharaka, Yousif K.; Thordsen, James J.; Kakouros, Evangelos
  • Environmental Earth Sciences, Vol. 60, Issue 2, p. 273-284
  • DOI: 10.1007/s12665-009-0401-1

Dissolution of a mineral phase in potable aquifers due to CO2 releases from deep formations; effect of dissolution kinetics
journal, November 2004


Surface complexation modelling of Cd(II), Cu(II), Ni(II), Pb(II) and Zn(II) adsorption onto kaolinite
journal, January 2008


Evaluating impacts of CO2 intrusion into an unconsolidated aquifer: II. Modeling results
journal, January 2016

  • Zheng, Liange; Qafoku, Nikolla P.; Lawter, Amanda
  • International Journal of Greenhouse Gas Control, Vol. 44
  • DOI: 10.1016/j.ijggc.2015.07.001

Potential risks to freshwater resources as a result of leakage from CO2 geological storage: a batch-reaction experiment
journal, December 2009

  • Lu, Jiemin; Partin, Judson W.; Hovorka, Susan D.
  • Environmental Earth Sciences, Vol. 60, Issue 2
  • DOI: 10.1007/s12665-009-0382-0

Thermoddem: A geochemical database focused on low temperature water/rock interactions and waste materials
journal, October 2012


Modeling the impact of carbon dioxide leakage into an unconfined, oxidizing carbonate aquifer
journal, January 2016

  • Bacon, Diana H.; Qafoku, Nikolla P.; Dai, Zhenxue
  • International Journal of Greenhouse Gas Control, Vol. 44
  • DOI: 10.1016/j.ijggc.2015.04.008

Modelling the adsorption of Cd(II), Cu(II), Ni(II), Pb(II), and Zn(II) onto Fithian illite
journal, March 2007


Metal Release from Sandstones under Experimentally and Numerically Simulated CO 2 Leakage Conditions
journal, January 2014

  • Kirsch, Katie; Navarre-Sitchler, Alexis K.; Wunsch, Assaf
  • Environmental Science & Technology, Vol. 48, Issue 3
  • DOI: 10.1021/es403077b

Effect of Dissolved CO 2 on a Shallow Groundwater System: A Controlled Release Field Experiment
journal, August 2012

  • Trautz, Robert C.; Pugh, John D.; Varadharajan, Charuleka
  • Environmental Science & Technology, Vol. 47, Issue 1
  • DOI: 10.1021/es301280t

Geochemical Impacts to Groundwater from Geologic Carbon Sequestration: Controls on pH and Inorganic Carbon Concentrations from Reaction Path and Kinetic Modeling
journal, June 2010

  • Wilkin, Richard T.; DiGiulio, Dominic C.
  • Environmental Science & Technology, Vol. 44, Issue 12
  • DOI: 10.1021/es100559j

Geochemical Implications of Gas Leakage associated with Geologic CO 2 Storage—A Qualitative Review
journal, August 2012

  • Harvey, Omar R.; Qafoku, Nikolla P.; Cantrell, Kirk J.
  • Environmental Science & Technology, Vol. 47, Issue 1
  • DOI: 10.1021/es3029457

Competitive Adsorption of Arsenate and Arsenite on Oxides and Clay Minerals
journal, January 2002


Geochemical modeling of changes in shallow groundwater chemistry observed during the MSU-ZERT CO2 injection experiment
journal, March 2012

  • Zheng, Liange; Apps, John A.; Spycher, Nicolas
  • International Journal of Greenhouse Gas Control, Vol. 7
  • DOI: 10.1016/j.ijggc.2011.10.003

Hydro-geochemical impact of CO2 leakage from geological storage on shallow potable aquifers: A field scale pilot experiment
journal, November 2013


Biodegradation and transport of benzene, toluene, and xylenes in a simulated aquifer: comparison of modelled and experimental results
journal, January 2002

  • Jean, Jiin-Shuh; Tsai, Ching-Lang; Ju, Shen-Haw
  • Hydrological Processes, Vol. 16, Issue 16
  • DOI: 10.1002/hyp.1093

Assessing risk to fresh water resources from long term CO2 injection–laboratory and field studies
journal, February 2009


Modeling of CO2 Leakage up Through an Abandoned Well from Deep Saline Aquifer to Shallow Fresh Groundwaters
journal, August 2011


Evaluation of Potential Changes in Groundwater Quality in Response to CO2 Leakage from Deep Geologic Storage
journal, January 2010


Investigation of the geochemical impact of CO2 on shallow groundwater: design and implementation of a CO2 injection test in Northeast Germany
journal, May 2012

  • Peter, Anita; Lamert, Hendrik; Beyer, Matthias
  • Environmental Earth Sciences, Vol. 67, Issue 2
  • DOI: 10.1007/s12665-012-1700-5

Probabilistic evaluation of shallow groundwater resources at a hypothetical carbon sequestration site
journal, March 2014

  • Dai, Zhenxue; Keating, Elizabeth; Bacon, Diana
  • Scientific Reports, Vol. 4, Issue 1
  • DOI: 10.1038/srep04006

CO2-H2O mixtures in the geological sequestration of CO2. II. Partitioning in chloride brines at 12–100°C and up to 600 bar
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
journal, May 2013

  • Zheng, Liange; Spycher, Nicolas; Birkholzer, Jens
  • International Journal of Greenhouse Gas Control, Vol. 14
  • DOI: 10.1016/j.ijggc.2013.01.014

Geochemistry, radiocarbon ages, and paleorecharge conditions along a transect in the central High Plains aquifer, southwestern Kansas, USA
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
journal, August 2003

  • Hawthorne, Steven B.; Miller, David J.
  • Environmental Science & Technology, Vol. 37, Issue 16
  • DOI: 10.1021/es020899f

Environmental consequences of potential leaks of CO2 in soil
journal, January 2011


Comparison of Arsenic(V) and Arsenic(III) Sorption onto Iron Oxide Minerals:  Implications for Arsenic Mobility
journal, September 2003

  • Dixit, Suvasis; Hering, Janet G.
  • Environmental Science & Technology, Vol. 37, Issue 18
  • DOI: 10.1021/es030309t

The impact of CO2 on shallow groundwater chemistry: observations at a natural analog site and implications for carbon sequestration
journal, June 2009

  • Keating, Elizabeth H.; Fessenden, Julianna; Kanjorski, Nancy
  • Environmental Earth Sciences, Vol. 60, Issue 3
  • DOI: 10.1007/s12665-009-0192-4

Applicability of aquifer impact models to support decisions at CO2 sequestration sites
journal, September 2016

  • Keating, Elizabeth; Bacon, Diana; Carroll, Susan
  • International Journal of Greenhouse Gas Control, Vol. 52
  • DOI: 10.1016/j.ijggc.2016.07.001

Impacts of elevated dissolved CO2 on a shallow groundwater system: Reactive transport modeling of a controlled-release field test
journal, December 2016


Potential chemical impacts of CO2 leakage on underground source of drinking water assessed by quantitative risk analysis
journal, July 2016


Potential environmental issues of CO2 storage in deep saline aquifers: Geochemical results from the Frio-I Brine Pilot test, Texas, USA
journal, June 2009


TOUGH2 User's Guide Version 2
report, November 1999

  • Pruess, K.; Oldenburg, C.M.; Moridis, G.J.
  • LBNL--43134
  • DOI: 10.2172/751729

Modeling the adsorption of Cd (II), Cu (II), Ni (II), Pb (II) and Zn (II) onto montmorillonite
journal, October 2010

  • Gu, Xueyuan; Evans, Les J.; Barabash, Sarah J.
  • Geochimica et Cosmochimica Acta, Vol. 74, Issue 20
  • DOI: 10.1016/j.gca.2010.07.016

Single-well push–pull test for assessing potential impacts of CO2 leakage on groundwater quality in a shallow Gulf Coast aquifer in Cranfield, Mississippi
journal, October 2013

  • Yang, Changbing; Mickler, Patrick J.; Reedy, Robert
  • International Journal of Greenhouse Gas Control, Vol. 18
  • DOI: 10.1016/j.ijggc.2012.12.030

Transport of organic contaminants mobilized from coal through sandstone overlying a geological carbon sequestration reservoir
journal, February 2014


On mobilization of lead and arsenic in groundwater in response to CO2 leakage from deep geological storage
journal, November 2009