Molecular-scale mechanisms of CO2 mineralization in nanoscale interfacial water films

Abdolhosseini Qomi, Mohammad Javad; Miller, Quin R. S.; Zare, Siavash; Schaef, Herbert T.; Kaszuba, John P.; Rosso, Kevin M.

doi:10.1038/s41570-022-00418-1

Molecular-scale mechanisms of CO₂ mineralization in nanoscale interfacial water films

Journal Article · Tue Aug 30 00:00:00 EDT 2022 · Nature Reviews Chemistry

DOI:https://doi.org/10.1038/s41570-022-00418-1· OSTI ID:1889464

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Univ. of California, Irvine, CA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Univ. of Wyoming, Laramie, WY (United States)

The calamitous impacts of untethered carbon emission from fossil-fuel-burning energy infrastructure calls for accelerated development of large-scale CO₂ capture, utilization, and storage technologies that are underpinned by fundamental understanding of molecular-level chemical processes. In the subsurface, rocks rich in divalent metals can react with CO₂, permanently sequestering it in the form of stable metal carbonate minerals, with the CO₂-H₂O composition of the post-injection pore fluid acting as a primary control variable. Herein, we compare mechanistic reaction pathways for aqueous-mediated carbonation with carbon mineralization occurring in nanoscale adsorbed water films. In the extreme of pores filled with a CO₂-dominant fluid, carbonation reactions are confined to nanometer-thick water films coating mineral surfaces, which enable metal cation release, transport, nucleation, and crystallization of metal carbonate minerals. Though seemingly counterintuitive, laboratory studies have demonstrated facile carbonation rates in these low water environments, which in recent years has begun to be better understood in mechanistic detail. The overarching objective of this review is to delineate the unique underlying molecular-scale reaction mechanisms that govern CO₂ mineralization in these reactive and dynamic quasi-2D interfaces. Here. we highlight the importance of understanding unique properties in thin water films, such as how water dielectric properties, and consequently ion solvation/hydration behavior, can change under nanoconfinement. We conclude by identifying important frontiers for future work and opportunities to exploit these fundamental chemical insights for decarbonization technologies in the 21st century.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC05-76RL01830; SC0022301

OSTI ID:: 1889464

Report Number(s):: PNNL-SA-169144

Journal Information:: Nature Reviews Chemistry, Journal Name: Nature Reviews Chemistry Journal Issue: 9 Vol. 6; ISSN 2397-3358

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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