Molecular mechanisms of CO2 mineralization on wetting nanoscale surfaces using molecular simulations and metadynamics

Xinping Zhu, Yong Tao (), Romain Dupuis, Yining Gao, Chi-Sun Poon, Katerina Ioannidou () and Roland J-M Pellenq ()
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Xinping Zhu: Université de Montpellier, Laboratoire de Mécanique et Génie Civil (LMGC), CNRS
Yong Tao: The Hong Kong Polytechnic University, Department of Civil and Environmental Engineering & Research Centre for Resources Engineering Towards Carbon Neutrality
Romain Dupuis: Université de Montpellier, Laboratoire de Mécanique et Génie Civil (LMGC), CNRS
Yining Gao: The Hong Kong Polytechnic University, Department of Civil and Environmental Engineering & Research Centre for Resources Engineering Towards Carbon Neutrality
Chi-Sun Poon: The Hong Kong Polytechnic University, Department of Civil and Environmental Engineering & Research Centre for Resources Engineering Towards Carbon Neutrality
Katerina Ioannidou: Université de Montpellier, Laboratoire de Mécanique et Génie Civil (LMGC), CNRS
Roland J-M Pellenq: Université de Montpellier, Institut Européen des Membranes (IEM), CNRS

Nature Communications, 2025, vol. 16, issue 1, 1-14

Abstract: Abstract Carbonatable minerals on earth have significant potential to act as gigatonne-scale CO2 sinks. Many carbon removal managements rely on CO2 mineralization on wetting mineral surfaces. Realizing their carbon removal potential requires a fundamental understanding of the atomic-scale mechanisms of mineral carbonation. This study employs reactive/non-reactive molecular simulations and well-tempered metadynamics to elucidate the complete interfacial CO2 mineralization pathways within a portlandite mesopore adsorbed with a nanometric water film. Here we reveal quantitatively, for the first time, a global CO2 mineralization spectrum describing the local molecular environment and the thermodynamics of the five critical steps: water adsorption, calcium dissolution, CO2 adsorption, CO2 speciation, and CaCO3 ion pairing. We identify kinks as the primary reactive sites for surface dissolution and demonstrate how the water film’s acid-base environment modulates these processes, creating an energetically favorable reaction loop for sustained CO2 mineralization. We uncover that quasi-neutral to slightly basic conditions optimize mineralization efficiency by balancing the opposing effects of pH on calcium dissolution and CO2 speciation.

Date: 2025
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DOI: 10.1038/s41467-025-65794-w

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