Pyrophyllite dissolution at elevated pressure conditions: An ab initio study

The atomistic mechanism of dissolution reactions at mineral fluid interface is essential for understanding the reaction kinetics and adsorption thermodynamic equilibria surfaces. In this study we investigate initial state process on (0 1 0) surface pyrophyllite elevated pressure by applying large-scale ab initio Meta-Dynamics simulations. system setup provides a realistic representation clay edge structure takes into account explicit dynamics solvent molecules. model parameters follow procedure recently tested simulation (1 edge. reveals that single tetrahedral or an octahedral unit from complex multi-step with several intermediates. Typically, each step changes denticity reacting site in step-by-step manner leads, eventually, to leaching ions forming sheets phyllosilicate. rearrangement proton transfer first second coordination shell dissolving play critical role stabilization intermediates net progress reactions. contrast ambient conditions, transition complexes formed during conditions were found have increased number. new insight environment interface.