Carbon mineralization pathways in interfacial adsorbed water nanofilms

Youzi, Mehrdad; Stapper, Julian L.; Zare, Siavash; Schaef, Herbert Todd; Bowden, Mark E.; Rosso, Kevin M.; Miller, Quin R. S.; Abdolhosseini Qomi, Mohammad Javad

doi:10.1038/s43247-025-02436-5

Title: Carbon mineralization pathways in interfacial adsorbed water nanofilms

Journal Article · Thu Jun 19 00:00:00 UTC 2025 · Communications Earth & Environment

DOI: https://doi.org/10.1038/s43247-025-02436-5 · OSTI ID:2570945

^[1]; Stapper, Julian L. ^[1];

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Univ. of California, Irvine, CA (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Carbon mineralization in humidified carbon dioxide offers a promising route to mitigate anthropogenic emissions in a world stressed by water security. Despite its technological importance, our understanding of carbonation in water-poor environments lags, as traditional dissolution-precipitation pathways struggle to explain the adsorbed water nanofilm-mediated reactivity. Here, we utilize in operando X-ray diffraction (XRD) and advanced molecular simulations to investigate nanoconfined reactions driving forsterite carbonation, the magnesium-rich olivine. By examining magnesium ion dissolution and transport in atomistic simulations of the forsterite-water-carbon dioxide interface and comparing these with the in operando XRD activation energies, we identify both processes as rate-limiting at saturation. Our simulations reveal a mechanistic view of interfacial carbonation, where dissolution and precipitation are mediated by anomalous quasi two-dimensional diffusion. The transport process involves intermittent diffusive hopping in the desorbed state, separated by crawling events that are spatially short but temporally long. This understanding transcends carbon mineralization, with implications for understanding the transport of contaminants in geosystems, the design of multifunctional materials, water desalination, and molecular recognition systems.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Univ. of California, Irvine, CA (United States)

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

Grant/Contract Number:: SC0022301

OSTI ID:: 2570945

Report Number(s):: PNNL-SA--205260

Journal Information:: Communications Earth & Environment, Journal Name: Communications Earth & Environment Journal Issue: 1 Vol. 6; ISSN 2662-4435

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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