AUTHOR=Tao Yong , Mu Yuandong , Zhang Wenqin , Wang Fazhou 

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

JOURNAL=Frontiers in Materials

VOLUME=7

YEAR=2020

URL=https://www.frontiersin.org/journals/materials/articles/10.3389/fmats.2020.00299

DOI=10.3389/fmats.2020.00299

ISSN=2296-8016

ABSTRACT=<p>γ-Ca<sub>2</sub>SiO<sub>4</sub> as a promising carbonation-activated cementitious material features an attractive capacity of carbon sequestration. Improving the carbonation reactivity of γ-Ca<sub>2</sub>SiO<sub>4</sub> 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-Ca<sub>2</sub>SiO<sub>4</sub> crystal. Ba, P, and F elements are found to decrease the overall binding strength of γ-Ca<sub>2</sub>SiO<sub>4</sub> 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.</p>