抄録
The fate and transport of Cs in engineered barriers and the environment is controlled by sorptive surface reactions. Strong Cs sorption complexes at the edge of phyllosilicate minerals are known, but an atomistic description of these binding sites remains ambiguous. Pyrophyllite, a non-swelling phyllosilicate, is an ideal analog for the study of phyllosilicate edges as pyrophyllite lacks a permanent structural charge. An atomistic model of the dominant crystallographic edge predicts changes in the interfacial structure as a function of pH. These structural changes at the interface are due to the increased edge surface charge and related to the hydrolysis of the Al. Molecular dynamics simulations of this model identify three strong, inner-sphere Cs sorption sites at the pyrophyllite edge.
