Kinetic Monte Carlo Approach To Study Carbonate Dissolution

Abstract

Reactive properties of carbonate minerals and rocks attract a significant attention with regard to modern environmental and industrial problems, including geologic carbon sequestration, toxic waste utilization, cement clinker production, and the fate of carbonate shell-bearing organisms in acidifying oceans. Despite the ultimate importance of the problem, the number of studies connecting atomistic-scale models to experimental observations is limited. In this work we employ the Kinetic Monte Carlo (KMC) approach to model carbonate dissolution at the nanometer–micron scale range and to access quantitative relationships between the variety of surface reactive sites and experimentally observed spatiotemporal rate variance. The presented KMC model adequately reproduces experimentally observed dissolution patterns and rates. We examine mechanistic and quantitative relationships between site reactivity, atomic step velocity, etch pit evolution dynamics, and macroscopic dissolution rates. The analysis of reactive...