Lead
(Pb)-containing solids find widespread commercial use in batteries,
piezoelectrics, and as starting materials for synthesis. Here, we
combine density functional theory (DFT) and thermodynamics in a DFT
+ solvent ion model to compare the surface reactivity of Pb oxides
and carbonates, specifically litharge, massicot, and cerussite, in
contact with water. The information provided by this model is used
to delineate structure–property relationships for surfaces
that are able to release Pb as Pb2+. We find that Pb2+ release is dependent on pH and chemical bonding environment
and go on to correlate changes in the surface bonding to key features
of the electronic structure through a projected density of states
analysis. Collectively, our analyses link the atomistic structure
to i) specific electronic states and ii) the thermodynamics of surface
transformations, and the results presented here can be used to guide
synthetic efforts of Pb2+-containing materials in aqueous
media or be used to better understand the initial steps in solid decomposition.
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