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Goals of Project:New and/or improved solutions to the stabilization and volume reduction of nuclear materials processing residues are urgently needed. Mediated electrochemical oxidation / reduction (MEO/R) processes are one such approach for incinerator ash, combustibles, and other solid residues. However, questions remain concerning the mechanisms of these processes, and how they might be optimized. In addition, further research is merited to extend their range of applicability. Recent advances in the study of heterogeneous electron transfer in solid substrates have opened the door for the re-examination of electron transfer processes associated with redox mediated actinide dissolution. We will develop a deeper understanding of the thermodynamic and mechanistic aspects of heterogeneous electron transfer that lie at the heart of these MEO/R processes. We will also develop and test new approaches based on the results of these fundamental studies using actual residue materials. Key aspects of this proposal include: