Multiphase sequestration geochemistry: Model for mineral carbonation

Abstract

Carbonation of formation minerals converts low viscosity supercritical CO2 injected into deep saline reservoirs for geologic sequestration into an immobile form. Until recently the scientific focus of mineralization reactions with reservoir rocks has been those that follow an aqueous-mediated dissolution/precipitation mechanism, driven by the sharp reduction in pH that occurs with CO2 partitioning into the aqueous phase. For sedimentary basin formations the kinetics of aqueous-mediated dissolution/precipitation reactions are sufficiently slow to make the role of mineralization trapping insignificant over a century period. For basaltic saline formations aqueous-phase mineralization progresses at a substantially higher rate, making the role of mineralization trapping significant, if not dominant, over a century period. The overlooked mineralization reactions for both sedimentary and basaltic saline formations, however, are those that occur in liquid or supercritical CO2 phase; where, dissolved water appears to play a catalyst role in the formation of carbonate minerals. A model is proposed in this paper that describes mineral carbonation over sequestration reservoir conditions ranging from dissolved CO2 in aqueous brine to dissolved water in supercritical CO2. The model theory is based on a review of recent experiments directed at understanding the role of water in mineral carbonation reactions of interest in geologic sequestration systems occurring under low water contents.