Pore-Scale Microenvironments Control Anthropogenic Carbon Mineralization Outcomes in Basalt

Depp, Charles T.; Miller, Quin R. S.; Crum, Jarrod V.; Horner, Jake A.; Schaef, H. Todd

doi:10.1021/acsearthspacechem.2c00165

Pore-Scale Microenvironments Control Anthropogenic Carbon Mineralization Outcomes in Basalt

Journal Article · Tue Nov 29 23:00:00 EST 2022 · ACS Earth and Space Chemistry

DOI:https://doi.org/10.1021/acsearthspacechem.2c00165· OSTI ID:1906315

^[1]; ^[2]; Crum, Jarrod V. ^[2]; Horner, Jake A. ^[2]; ^[2]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Colorado School of Mines, Golden, CO (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Thin sections and hand samples from 50 sidewall cores from the Wallula Basalt Pilot Demonstration, a basaltic carbon sequestration demonstration, provided the opportunity for the in-depth analysis of carbon mineralization induced by the injection of supercritical CO₂. In this study, we used optical petrography and scanning electron microscopy to characterize the physical and chemical characteristics of the basalt components influenced by carbon mineralization reactions from all available hand samples and thin sections within the three CO₂ injection zones and caprock flow interiors. We found extensive carbonate mineralization, mostly in the form of nodules that were shown to be chemically zoned: Ca-dominant in the core regions and Ca-bearing Fe-dominant in the outer regions. Carbonate mineralization also took the form of fracture-filling carbonate cement, and acicular aragonite was also observed. Overall, we clarified the structural and paragenetic relationships between newly formed minerals, identifying a new fibro-palagonite-like, poorly crystalline silicate phase that grew on the carbonate nodules and pore-lining zeolites. Here we observed Fe-dominant carbonate precipitates surrounding acicular aragonite and rhombohedral Ca-carbonate cores, whereas previous studies of these zoned nodules did not observe these structures. A comprehensive accounting of the carbon mineralization products is vital to understand and predict the behavior of supercritical CO₂ in the subsurface given both the diversity of the host rock between and within injection zones, especially considering that the morphology and chemistry of the diverse precipitates are influenced by the pore-scale microenvironments of the basalt.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Workforce Development for Teachers and Scientists (WDTS); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1906315

Report Number(s):: PNNL-SA-173493

Journal Information:: ACS Earth and Space Chemistry, Journal Name: ACS Earth and Space Chemistry Journal Issue: 12 Vol. 6; ISSN 2472-3452

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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