Screening Out Reactivity-Promoting Candidates for γ-Ca₂SiO₄ Carbonation by First-Principles Calculations

γ-Ca₂SiO₄ as a promising carbonation-activated cementitious material features an attractive capacity of carbon sequestration. Improving the carbonation reactivity of γ-Ca₂SiO₄ is of great significance for its practical application. In this paper, first-principles calculations are performed to single out the potential candidates for carbonation activation from a series of dopants. Electronic structure analyses reveal that the carbonation reactivity is related to the reactive site distribution and the binding strength of γ-Ca₂SiO₄ crystal. Ba, P, and F elements are found to decrease the overall binding strength of γ-Ca₂SiO₄ crystal, which benefits the dissolution of ions from the crystal to take part in the carbonation reactions. The theoretical conjectures are validated by designed and previous experiments, which confirms the first-principles-based method to effectively guide our experimental investigation.