[en] High-Level Waste (HLW) is a waste associated with the dissolution of spent nuclear fuel for the recovery of weapons-grade material. It is the priority problem for the U.S. Department of Energy's Environmental Management Program. Current HLW treatment processes at the Savannah River Site (Aiken, SC) include the use of monosodium titanate. The local structural speciation of sorbed U varied with loading but not for Sr. Sorbed Sr exhibited specific adsorption as partially-hydrated species whereas sorbed U exhibited specific adsorption as monomeric and dimeric U(VI)-carbonate complexes. Sorption proved site specific. These differences in site specificity and sorption mechanism may account for the difficulties associated with predicting Sr and U loading and removal kinetics using MST