The Savannah River Site (SRS) has forty-three remaining very large underground tanks containing significant quantities of nuclear waste generated primarily from cold-war radiochemical separations. All of the tanks eventually must be closed. As part of decommissioning/closing the nuclear waste tanks, even residual quantities of the waste must be removed. Although most sludge can be removed mechanically, chemically cleaning (i.e. decontamination) with oxalic acid is used to aid in the removal of residual quantities. Although oxalic acid works for cleaning the tanks, its downstream impacts are considered detrimental. To better understand and quantify the impacts, detailed models were developed to account for different potential processing strategies for handling the spent oxalic acid nuclear decontamination slurries. Although the results vary, the models show that regardless of the oxalate handling strategies: 1) significant washing to decrease sodium concentration/solids concentration in vitrification feed will be required, and 2) the creation of copious future additions of feed for salt processing will be unavoidable. Using a Theory of Inventive Problem Solving (TRIZ) approach, a modified form of the Chemical Oxidation Reduction Decontamination (CORD) ultraviolet (UV) light was identified as being used with an analogous but already resolved problem that could be adapted to SRS HLW tank cleaning. A novel preliminary process called Enhanced Chemical Cleaning (ECC) was envisioned. Many people have aided me in this research and made this thesis possible. Naming all key people would likely be impossible; therefore, I will probably leave someone out. In advance, please accept my apologies. From my time at High-Level Waste Engineering, I would like to thank Renee Spires, Tommy Caldwell, Mark Mahoney, and Neil Davis. They were the first people to honestly trust my novel TRIZ determination that using oxalic acid to clean the High-Level Waste tanks, tied closely to decomposing the resultant spent acid solution represented the "ideal solution." At Savannah River National Laboratory, Chris Martino and Bill King, who spent considerable time helping me understand much of the oxidation chemistry. At AREVA NP (Lynchburg) Dennis Jones, John Remark, Ray Beatty, and Sarah Evans, all who helped me gain valuable insights. My supervisor Professor Colin Boxall who encouraged me throughout the process. And finally, to my many friends and colleagues that supported me during this research. viii