Ab initio mechanism revealing for tricalcium silicate dissolution

Yunjian Li; Hui Pan; Qing Liu; Xing Ming; Zongjin Li

doi:10.1038/s41467-022-28932-2

Ab initio mechanism revealing for tricalcium silicate dissolution

Nat Commun. 2022 Mar 10;13(1):1253. doi: 10.1038/s41467-022-28932-2.

Authors

Yunjian Li¹, Hui Pan^{1

2}, Qing Liu¹, Xing Ming¹, Zongjin Li³

Affiliations

¹ Institute of Applied Physics and Materials Engineering, University of Macau, Macao SAR, 999078, P. R. China.
² Department of Physics and Chemistry, Faculty of Science and Technology, University of Macau, Macao SAR, 999078, P. R. China.
³ Institute of Applied Physics and Materials Engineering, University of Macau, Macao SAR, 999078, P. R. China. zongjinli@um.edu.mo.

Abstract

Dissolution of minerals in water is ubiquitous in nature and industry, especially for the calcium silicate species. However, the behavior of such a complex chemical reaction is still unclear at atomic level. Here, we show that the ab initio molecular dynamics and metadynamics simulations enable quantitative analyses of reaction pathways, thermodynamics and kinetics of the calcium ion dissolution from the tricalcium silicate (Ca₃SiO₅) surface. The calcium sites with different coordination environments lead to different reaction pathways and free energy barriers. The low free energy barriers result in that the detachment of the calcium ion is a ligand exchange and auto-catalytic process. Moreover, the water adsorption, proton exchange and diffusion of water into the surface layer accelerate the leaching of the calcium ion from the surface step by step. The discovery in this work thus would be a landmark for revealing the mechanism of tricalcium silicate hydration.