Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

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

Abstract

The dissolution of CO2 in water leads to a pH decrease and a carbonate content increase in affected groundwater, which in turn can drive the mobilization of metals from sediments. The mechanisms of metal release postulated in various field and laboratory studies often differ. Drawing primarily on previously published results, we examine contrasting metal mobilization behaviors at two field tests and in one laboratory study, to investigate whether the same mechanisms could explain metal releases in these different experiments. Numerical modeling of the two field tests reveals that fast Ca-driven cation exchange (from calcite dissolution) can explain the release of most major and trace metal cations at both sites, and their parallel concentration trends. The dissolution of other minerals reacting more slowly (superimposed on cation exchange) also contributes to metal release over longer time frames, but can be masked by fast ambient groundwater velocities. Therefore, the magnitude and extent of mobilization depends not only on metal-mineral associations and sediment pH buffering characteristics, but also on groundwater flow rates, thus on the residence time of CO2-impacted groundwater relative to the rates of metal-release reactions. Sequential leaching laboratory tests modeled using the same metal-release concept as postulated from field experiments show thatmore » both field and laboratory data can be explained by the same processes. Finally, the reversibility of metal release upon CO2 degassing by de-pressurization is also explored using simple geochemical models, and shows that the sequestration of metals by resorption and re-precipitation upon CO2 exsolution is quite plausible and may warrant further attention.« less

Authors:
 [1];  [1];  [1];  [1];  [2];  [3];  [1];  [1];  [4]
+ Show Author Affiliations
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Southern Company Services, Birmingham AL (United States)
  3. British Geological Survey, Keyworth, Nottingham (United Kingdom)
  4. Electric Power Research Inst., Palo Alto CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Fossil Energy (FE)
OSTI Identifier:
1512097
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Greenhouse Gases: Science and Technology
Additional Journal Information:
Journal Volume: 5; Journal Issue: 4; Journal ID: ISSN 2152-3878
Publisher:
Society of Chemical Industry, Wiley
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; groundwater; carbonic acid; leak; CO 2 sequestration; CCS; CCUS

Citation Formats

Zheng, Liange, Spycher, Nicolas, Varadharajan, Charuleka, Tinnacher, Ruth M., Pugh, John D., Bianchi, Marco, Birkholzer, Jens, Nico, Peter S., and Trautz, Robert C. On the mobilization of metals by CO 2 leakage into shallow aquifers: exploring release mechanisms by modeling field and laboratory experiments. United States: N. p., 2015. Web. doi:10.1002/ghg.1493.
Copy to clipboard
Zheng, Liange, Spycher, Nicolas, Varadharajan, Charuleka, Tinnacher, Ruth M., Pugh, John D., Bianchi, Marco, Birkholzer, Jens, Nico, Peter S., & Trautz, Robert C. On the mobilization of metals by CO 2 leakage into shallow aquifers: exploring release mechanisms by modeling field and laboratory experiments. United States. https://doi.org/10.1002/ghg.1493
Copy to clipboard
Zheng, Liange, Spycher, Nicolas, Varadharajan, Charuleka, Tinnacher, Ruth M., Pugh, John D., Bianchi, Marco, Birkholzer, Jens, Nico, Peter S., and Trautz, Robert C. Thu . "On the mobilization of metals by CO 2 leakage into shallow aquifers: exploring release mechanisms by modeling field and laboratory experiments". United States. https://doi.org/10.1002/ghg.1493. https://www.osti.gov/servlets/purl/1512097.
Copy to clipboard
@article{osti_1512097,
title = {On the mobilization of metals by CO 2 leakage into shallow aquifers: exploring release mechanisms by modeling field and laboratory experiments},
author = {Zheng, Liange and Spycher, Nicolas and Varadharajan, Charuleka and Tinnacher, Ruth M. and Pugh, John D. and Bianchi, Marco and Birkholzer, Jens and Nico, Peter S. and Trautz, Robert C.},
abstractNote = {The dissolution of CO2 in water leads to a pH decrease and a carbonate content increase in affected groundwater, which in turn can drive the mobilization of metals from sediments. The mechanisms of metal release postulated in various field and laboratory studies often differ. Drawing primarily on previously published results, we examine contrasting metal mobilization behaviors at two field tests and in one laboratory study, to investigate whether the same mechanisms could explain metal releases in these different experiments. Numerical modeling of the two field tests reveals that fast Ca-driven cation exchange (from calcite dissolution) can explain the release of most major and trace metal cations at both sites, and their parallel concentration trends. The dissolution of other minerals reacting more slowly (superimposed on cation exchange) also contributes to metal release over longer time frames, but can be masked by fast ambient groundwater velocities. Therefore, the magnitude and extent of mobilization depends not only on metal-mineral associations and sediment pH buffering characteristics, but also on groundwater flow rates, thus on the residence time of CO2-impacted groundwater relative to the rates of metal-release reactions. Sequential leaching laboratory tests modeled using the same metal-release concept as postulated from field experiments show that both field and laboratory data can be explained by the same processes. Finally, the reversibility of metal release upon CO2 degassing by de-pressurization is also explored using simple geochemical models, and shows that the sequestration of metals by resorption and re-precipitation upon CO2 exsolution is quite plausible and may warrant further attention.},
doi = {10.1002/ghg.1493},
journal = {Greenhouse Gases: Science and Technology},
number = 4,
volume = 5,
place = {United States},
year = {Thu Apr 23 00:00:00 EDT 2015},
month = {Thu Apr 23 00:00:00 EDT 2015}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1002/ghg.1493
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 26 works
Citation information provided by
Web of Science

Figures / Tables:

Figure 1 Figure 1: pH (left) and breakthrough of Ca, Sr, Mn, Ba, Cr, and Fe at about 5 m from a carbonated groundwater injection well; model predictions (lines) compared to observations (symbols) (data reported in Trautz et al).
All figures and tables (10 total)
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

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

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

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

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

Inorganic species in geologic fluids: Correlations among standard molal thermodynamic properties of aqueous ions and hydroxide complexes
journal, March 1997

Inducing a CO2 Leak into a Shallow Aquifer (CO2FieldLab Eurogia+ Project): Monitoring the CO2 Plume in Groundwaters
journal, January 2013

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

Chemical evolution and mineral deposition in boiling hydrothermal systems
journal, February 1985

Surface Complexation of Ferrous Iron and Carbonate on Ferrihydrite and the Mobilization of Arsenic
journal, July 2002

  • Appelo, C. A. J.; Van Der Weiden, M. J. J.; Tournassat, C.
  • Environmental Science & Technology, Vol. 36, Issue 14
  • DOI: 10.1021/es010130n

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

Evolution of the chemistry of Fe bearing waters during CO2 degassing
journal, December 2012

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

Large-scale impact of CO2 storage in deep saline aquifers: A sensitivity study on pressure response in stratified systems
journal, March 2009

  • Birkholzer, J.; Zhou, Q.; Tsang, C.
  • International Journal of Greenhouse Gas Control, Vol. 3, Issue 2
  • DOI: 10.1016/j.ijggc.2008.08.002

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

A shallow subsurface controlled release facility in Bozeman, Montana, USA, for testing near surface CO2 detection techniques and transport models
journal, December 2009

  • Spangler, Lee H.; Dobeck, Laura M.; Repasky, Kevin S.
  • Environmental Earth Sciences, Vol. 60, Issue 2, p. 227-239
  • DOI: 10.1007/s12665-009-0400-2

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

Surface catalysis of uranium(VI) reduction by iron(II)
journal, October 1999

  • Liger, Emmanuelle; Charlet, Laurent; Van Cappellen, Philippe
  • Geochimica et Cosmochimica Acta, Vol. 63, Issue 19-20
  • DOI: 10.1016/S0016-7037(99)00265-3

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

Reactive transport modeling of plug-flow reactor experiments: quartz and tuff dissolution at 240°C
journal, August 1998

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

In situ feldspar dissolution rates in an aquifer
journal, March 2005

Chemical Composition of Bottled Mineral Water
journal, April 1989

  • Allen, Herbert E.; Halley-Henderson, Mary Ann; Hass, Charles N.
  • Archives of Environmental Health: An International Journal, Vol. 44, Issue 2
  • DOI: 10.1080/00039896.1989.9934383

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

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

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

A compilation of rate parameters of water-mineral interaction kinetics for application to geochemical modeling
report, January 2004

  • Palandri, James L.; Kharaka, Yousif K.
  • U.S. Geological Survey (USGS)
  • DOI: 10.3133/ofr20041068

Chemical weathering rate laws and global geochemical cycles
journal, May 1994

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

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

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
    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

    CO 2 Leakage-Induced Contamination in Shallow Potable Aquifer and Associated Health Risk Assessment
    journal, January 2018

      Sort by:
      [ × clear filter / sort ]

      Figures / Tables found in this record:

      Figure 1 (p. 8)figure
      Figure 2 (p. 9)figure
      Figure 3 (p. 11)figure
      Figure 4 (p. 12)figure
      Figure 5 (p. 12)figure
      Figure 6 (p. 14)figure
      Figure 7 (p. 15)figure
      Table A1 (p. 17)table
      Table A2 (p. 18)table
      Table A3 (p. 18)table
        [ × clear filter / sort ]
        Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.

        Similar Records in DOE PAGES and OSTI.GOV collections: