Carbonates are important minerals that are essential to life on Earth, regulating the carbon dioxide balance in the atmosphere. Understanding how carbonate surfaces transform and change as a function of pH is critical for a multitude of reasons, both natural and synthetic. Here we combine first-principles DFT and experimentally determined thermodynamics to better understand the surface transformations that cause carbonate mineral dissolution for a wide variety of conditions. We investigate the thermodynamics of aqueous surface exchange and bicarbonate release of CaCO3, SrCO3, BaCO3, and PbCO3 minerals and link this to an analysis of their electronic structures. While the outcomes of our study can be related to periodic trends and previously published dissolution studies, our modeling efforts can also help explain the behavior of carbonates in a wealth of applications and be used to form better experimental controls to further develop technologies based on carbonate materials.

Delineating the thermodynamics of carbonate dissolution in aqueous media by combining first-principles and experiments

ACS Spring 2022

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