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Title: Arsenic mobilization in shallow aquifers due to CO2 intrusion from storage reservoirs

Abstract

We developed an integrated framework of combined batch experiments and reactive transport simulations to quantify water-rock-CO2 interactions and arsenic (As) mobilization responses to CO2 and/or saline water leakage into USDWs. Experimental and simulation results suggest that when CO2 is introduced, pH drops immediately that initiates release of As from clay minerals. Calcite dissolution can increase pH slightly and cause As re-adsorption. Thus, the mineralogy of the USDW is ultimately a determining factor of arsenic fate and transport. Salient results suggest that: (1) As desorption/adsorption from/onto clay minerals is the major reaction controlling its mobilization, and clay minerals could mitigate As mobilization with surface complexation reactions; (2) dissolution of available calcite plays a critical role in buffering pH; (3) high salinity in general hinders As release from minerals; and (4) the magnitude and quantitative uncertainty of As mobilization are predicated on the values of reaction rates and surface area of calcite, adsorption surface areas and equilibrium constants of clay minerals, and cation exchange capacity. Results of this study are intended to improve ability to quantify risks associated with potential leakage of reservoir fluids into shallow aquifers, in particular the possible environmental impacts of As mobilization at carbon sequestration sites.

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [1];  [2];  [3];  [4];  [1];  [4]
+ Show Author Affiliations
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
  3. New Mexico Inst. of Mining and Technology, Socorro, NM (United States)
  4. Univ. of Utah, Salt Lake City, UT (United States)
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1369173
Report Number(s):
LA-UR-16-28763
Journal ID: ISSN 2045-2322
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Earth Sciences; Arsenic mobilization, adsorption/desorption, clay mineral, surface complexation, integrated framework, batch experiment.

Citation Formats

Xiao, Ting, Dai, Zhenxue, Viswanathan, Hari S., Hakala, Alexandra, Cather, Martha, Jia, Wei, Zhang, Yongchao, and McPherson, Brian. Arsenic mobilization in shallow aquifers due to CO2 intrusion from storage reservoirs. United States: N. p., 2017. Web. doi:10.1038/s41598-017-02849-z.
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Xiao, Ting, Dai, Zhenxue, Viswanathan, Hari S., Hakala, Alexandra, Cather, Martha, Jia, Wei, Zhang, Yongchao, & McPherson, Brian. Arsenic mobilization in shallow aquifers due to CO2 intrusion from storage reservoirs. United States. https://doi.org/10.1038/s41598-017-02849-z
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Xiao, Ting, Dai, Zhenxue, Viswanathan, Hari S., Hakala, Alexandra, Cather, Martha, Jia, Wei, Zhang, Yongchao, and McPherson, Brian. Mon . "Arsenic mobilization in shallow aquifers due to CO2 intrusion from storage reservoirs". United States. https://doi.org/10.1038/s41598-017-02849-z. https://www.osti.gov/servlets/purl/1369173.
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@article{osti_1369173,
title = {Arsenic mobilization in shallow aquifers due to CO2 intrusion from storage reservoirs},
author = {Xiao, Ting and Dai, Zhenxue and Viswanathan, Hari S. and Hakala, Alexandra and Cather, Martha and Jia, Wei and Zhang, Yongchao and McPherson, Brian},
abstractNote = {We developed an integrated framework of combined batch experiments and reactive transport simulations to quantify water-rock-CO2 interactions and arsenic (As) mobilization responses to CO2 and/or saline water leakage into USDWs. Experimental and simulation results suggest that when CO2 is introduced, pH drops immediately that initiates release of As from clay minerals. Calcite dissolution can increase pH slightly and cause As re-adsorption. Thus, the mineralogy of the USDW is ultimately a determining factor of arsenic fate and transport. Salient results suggest that: (1) As desorption/adsorption from/onto clay minerals is the major reaction controlling its mobilization, and clay minerals could mitigate As mobilization with surface complexation reactions; (2) dissolution of available calcite plays a critical role in buffering pH; (3) high salinity in general hinders As release from minerals; and (4) the magnitude and quantitative uncertainty of As mobilization are predicated on the values of reaction rates and surface area of calcite, adsorption surface areas and equilibrium constants of clay minerals, and cation exchange capacity. Results of this study are intended to improve ability to quantify risks associated with potential leakage of reservoir fluids into shallow aquifers, in particular the possible environmental impacts of As mobilization at carbon sequestration sites.},
doi = {10.1038/s41598-017-02849-z},
journal = {Scientific Reports},
number = 1,
volume = 7,
place = {United States},
year = {Mon Jun 05 00:00:00 EDT 2017},
month = {Mon Jun 05 00:00:00 EDT 2017}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1038/s41598-017-02849-z
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    Works referencing / citing this record:

    Reactive transport modeling of arsenic mobilization in shallow groundwater: impacts of CO2 and brine leakage
    journal, April 2017

    • Xiao, Ting; Dai, Zhenxue; McPherson, Brian
    • Geomechanics and Geophysics for Geo-Energy and Geo-Resources, Vol. 3, Issue 3
    • DOI: 10.1007/s40948-017-0058-2

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

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