The pre‐acidification triggers and enhances carbon mineralization in dicalcium silicate

Abstract The mineral carbonation under the natural chemical weathering reaction is one of the significant geochemical processes. The underlying mineral carbonation reaction mechanism remains unclear on the electronic scale. This work illustrates how pre‐acidification treatments create solvation structures that encourage carbon mineralization in β‐C 2 S (100) and γ‐C 2 S (010) by well‐defined ab initio molecular dynamics and well‐tempered metadynamics approaches. The results indicate that the , generated during CO 2 pre‐acidification, exhibits distinct behavior on the β‐C 2 S (100) and γ‐C 2 S (010) surfaces, which directly affects the formation of carbonate complex. In the β‐C 2 S (100)/H 2 O‐ system, the is dissociated by the surface O atoms (O s ), which subsequently form carbonate complexes through interactions with adjacent H 2 O molecules and the surface Ca atoms. However, following dissociation, the resulting CO 3 2− interacts with adjacent H 2 O molecules to form a stable solvation structure on the γ‐C 2 S (010) surface. This promotes the carbonation reaction in the γ‐C 2 S (010)/H 2 O‐ system. This work paves the way to understand the mechanism of mineral carbonation on the electronic scale and offers valuable insights into the process of geological evolution.