Exploring the Hydration Kinetics of Alternative Cements using Density Functional Theory and Molecular Dynamics

Cement production accounts for nearly 8% of global CO2 emissions, motivating the development of low carbon alternatives to ordinary portland cement. Calcium sulfoaluminate (CSA) cements containing ye'elimite (Ca4[Al6O12]SO4) offer a promising pathway to reduce emissions while maintaining comparable performance. However, the atomic scale mechanisms governing their hydration remain an active area of investigation. In this work we combine density functional theory (DFT), molecular dynamics (MD), and machine learned interatomic potentials (MLIPs) to investigate the surface properties and hydration behavior of ye'elimite. Using the MLIPs we will enable large scale MD simulations that explore surface relaxation, water structuring, and early hydration dynamics. This work establishes a computational framework for understanding and optimizing hydration in next generation low carbon cement systems.