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.

γ-的Ca ₂的SiO ₄作为有力的碳化活化胶凝材料设有固碳的一个有吸引力的容量。改善γ-Ca的碳酸化反应₂的SiO ₄是用于其实际应用具有重要的意义。在本文中，进行第一性原理计算以从一系列掺杂剂中选出可能的碳酸化活化候选物。电子结构的分析表明，碳酸化反应性相关的反应性位点的分布和γ-Ca的结合强度₂的SiO ₄晶体。的Ba，P，和F的元素被发现降低γ-Ca的总体结合强度₂的SiO ₄晶体，有利于离子从晶体中溶解，参与碳酸化反应。通过设计和先前的实验验证了理论上的猜想，这证实了基于第一原理的方法可以有效地指导我们的实验研究。