Interfacial mechanisms governing CO₂ mineralization: From reactivity origins of basaltic surfaces to engineering...

CO₂ mineralization offers a permanent and scalable route for carbon storage, and rapid in situ mineralization has been achieved in several field projects. Traditionally attributed to the classical dissolution-precipitation pathway, this process is increasingly recognized to be strongly influenced by CO₂-mineral interfacial reactions, which remain underrepresented in current models. This review synthesizes recent advances on how interfacial reactions accelerate carbonation, from atomic-scale reactivity of nonbridging oxygen (NBO) sites to mesoscopic effects of wettability, water film structure, and nanoconfinement. These reactions promote both metal release and carbonate nucleation by forming surface carbonate complexes that weaken metal-oxygen bonds and lower dehydration barriers. Building on these insights, we propose a multiscale modeling framework integrating ab initio molecular dynamics, surface complexation modeling, and reactive transport modeling to incorporate interfacial pathways into field-scale predictions. We also outline engineering strategies inspired by interfacial chemistry, including highly porous rock with high specific area, high-NBO mineral selection in terms of lithology (e.g., Olivine), CO₂ nanobubble injection, and additive co-injection to tune wettability. By linking interfacial science with reservoir engineering, this review establishes a mechanistic basis for accelerating and optimizing CO₂ mineralization systems.