Thermodynamic modelling of CO2 mineralization and experimental verification

Thermodynamics plays a crucial role in understanding complex chemical systems. Given known conditions of temperature, pressure, and composition, thermodynamic calculations can be applied to predict whether a reaction will proceed spontaneously and what the final equilibrium state will be. The thermodynamic method was first applied to cement chemistry by Le Chatelier in the late 19th century to describe hydration as the dissolution of clinker phases, leading to supersaturation and subsequent precipitation of hydration products. Thermodynamic approaches were later applied to cement manufacturing processes, focusing on the chemical reconstitution of raw materials, the release of structural water and CO 2 from precursor minerals, and the reorganization of complex minerals during processing. Since the 1940s, advances in fundamental science and microstructural characterization techniques have significantly enhanced our understanding of the highly disordered phases—including glasses, melts, and gels—which have greatly contributed to the development of structural models of these phases, such as C-S-H, and the establishment of more accurate and systematic thermodynamic databases. Subsequently, the development of computer technologies has led to the creation of a series of open-source Gibbs free energy minimization codes and stimulated the advancement of thermodynamic modeling software.