Jarosites (KFe3(SO4)2(OH)6) are examples of minerals that are highly effective scavengers of toxic elements, and are abundant in acid rock drainage systems, acid sulfate soils, metallurgical wastes and other contaminated sites. The K, Fe and S sites can be filled by toxic elements such as Cd, Cu and Zn, but the mechanisms of this incorporation are not well understood.We have used atomistic simulation methods to model the jarosite (102) surface and its interactions with Cd, Zn and Cu, in order to understand the mechanisms by which these potentially toxic elements are incorporated into the K-jarosite structure. Our results suggest that incorporation via a defect complex consisting of an impurity cation at the K site charge balanced by a K vacancy stabilises the (102) surface in the order Cu>Zn>Cd.