Molecular-level understanding of environmental interfaces using density functional theory modeling

Abstract

The ability to apply existing density functional theory-based modeling techniques to timely research problems in environmental chemistry is demonstrated by an ab initio thermodynamics investigation of stable hydrated oxide surface models and a comparative reactivity study of Pb(II) adsorption on two water-mineral interfaces with a common geometry, but distinct electronic structure. We emphasize the unique considerations required to produce chemically reasonable structural models for hydrated surfaces and surface complex structures, as well as how to use experimental insights to limit the extensive configuration space encountered in complex hydrated models relative to theoretical surface science done under idealized, ultra-high vacuum conditions.