Carbonation and self-healing in concrete: Kinetic Monte Carlo simulations of mineralization

Industrial applications of carbonation such as self-healing and carbon capture and storage have been limited, due to a lack of reliable predictive models linking the chemistry of carbonation at the molecular scale to microstructure development and macroscopic properties. This work proposes a coarse-grained Kinetic Monte Carlo (KMC) approach to simulate microstructural evolution of a model cement paste during carbonation, along with evolution of pore solution chemistry and saturation indexes of solid species involved. The simulations predict the effective rate constants for Ca(OH)2 dissolution and CaCO3 precipitation as kCa(OH)2 = 2.20 x 10-5 kg/ m3/s and kCaCO3 = 4.24 x 10-6 kg/m3/s. These values are directly fed to a macroscale reactive transport model to predict carbonate penetration depth. The rate constants from the molecular scale are used in a boundary nucleation and growth model to predict self-healing of cracks. Subsequently these results are compared with experimental data, and provide good agreement. This proposed multiscale approach can help understand and manage the carbonation of both traditional and new concretes, supporting applications in residual lifetime assessment, carbon capture, and self-healing.

Automated summary

This study proposes a coarse-grained Kinetic Monte Carlo approach to simulate the microstructural evolution of cement paste during carbonation and predicts the rate constants for dissolution and precipitation. The results can support applications in self-healing and carbon capture.