The high-level radioactive waste sludge in the underground storage tanks at the Hanford Site contains various chromium solid phases. Dissolution and removal of chromium from tank waste sludges is desirable prior to high-level waste vitrification because increased volume is required to incorporate the residual chromium. Unfortunately, dissolution of chromium from the sludge to form Cr(OH){sub 4}{sup -} through treatment with heated NaOH solution (also used to dissolve aluminum phases and metathesize phosphates to sodium salts) generally has been unsuccessful in tests with both simulated and genuine Hanford waste sludges. Oxidative dissolution of the Cr(III) compounds to form soluble chromate has been proposed as an alternative chromium solid phase dissolution method and results of limited prior testing have been reported. The present systematic tests investigated oxygen gas, hydrogen peroxide, and sodium persulfate oxidants to dissolve Cr(III) under alkaline conditions to form soluble chromate. Permanganate and ozone also were considered for testing but were thought to be of secondary interest because of the insoluble residue (MnO{sub 2} from permanganate) and complex equipment (necessary to generate ozone) implicit with use of these reagents. The oxygen and hydrogen peroxide reagents leave no condensable residue and sodium persulfate only leaves soluble sodium sulfate. Crystalline Cr(OH){sub …

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