Experimental Study of Porosity Changes in Shale Caprocks Exposed to Carbon Dioxide-Saturated Brine II: Insights from Aqueous Geochemistry

Miller, Quin R. S.; Wang, Xiuyu; Kaszuba, John P.; Mouzakis, Katherine M.; Navarre-Sitchler, Alexis K.; Alvarado, Vladimir; McCray, John E.; Rother, Gernot; Bañuelos, José Leobardo; Heath, Jason E.

doi:10.1089/ees.2015.0592

Title: Experimental Study of Porosity Changes in Shale Caprocks Exposed to Carbon Dioxide-Saturated Brine II: Insights from Aqueous Geochemistry

Journal Article · Mon Jul 18 00:00:00 EDT 2016 · Environmental Engineering Science

DOI:https://doi.org/10.1089/ees.2015.0592· OSTI ID:1328308

Miller, Quin R. S. ^[1]; Wang, Xiuyu ^[1]; Kaszuba, John P. ^[2]; Mouzakis, Katherine M. ^[3]; Navarre-Sitchler, Alexis K. ^[3]; Alvarado, Vladimir ^[4]; McCray, John E. ^[5]; Rother, Gernot ^[6]; Bañuelos, José Leobardo ^[6]; Heath, Jason E. ^[7]

Univ. of Wyoming, Laramie, WY (United States). Dept. of Geology and Geophysics
Univ. of Wyoming, Laramie, WY (United States). Dept. of Geology and Geophysics; Univ. of Wyoming, Laramie, WY (United States). School of Energy Resources
Colorado School of Mines, Golden, CO (United States). Dept. of Geology and Geological Engineering and Hydrologic Sciences and Engineering Program
Univ. of Wyoming, Laramie, WY (United States). Dept. of Chemical Engineering
Colorado School of Mines, Golden, CO (United States). Civil and Environmental Engineering
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Dept. of Geomechanics

Laboratory experiments evaluated two shale caprock formations, the Gothic Shale and Marine Tuscaloosa Formation, at conditions relevant to carbon dioxide (CO₂) sequestration. Both rocks were exposed to CO₂-saturated brines at 160°C and 15 MPa for ~45 days. Baseline experiments for both rocks were pressurized with argon to 15 MPa for ~35 days. Varying concentrations of iron, aqueous silica, sulfate, and initial pH decreases coincide with enhanced carbonate and silicate dissolution due to reaction between CO₂-saturated brine and shale. Saturation indices were calculated and activity diagrams were constructed to gain insights into sulfate, silicate, and carbonate mineral stabilities. We found that upon exposure to CO₂-saturated brines, the Marine Tuscaloosa Formation appeared to be more reactive than the Gothic Shale. Evolution of aqueous geochemistry in the experiments is consistent with mineral precipitation and dissolution reactions that affect porosity. Finally, this study highlights the importance of tracking fluid chemistry to clarify downhole physicochemical responses to CO₂ injection and subsequent changes in sealing capacity in CO₂ storage and utilization projects.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Nanoscale Control of Geologic CO2 (NCGC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; AC02-05CH11231

OSTI ID:: 1328308

Journal Information:: Environmental Engineering Science, Journal Name: Environmental Engineering Science; ISSN 1092-8758

Publisher:: Mary Ann Liebert, Inc.Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 22 works

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