Uraninite [U(IV) dioxide, UO 2 ] and metaschoepite [U(VI) oxide hydrate; (UO 2) 8 O 2 (OH) 12 (H 2 O) 12 or UO 3 •2H 2 O] are the uranium phases most frequently observed in actual K Basin sludge by X-ray diffractometry (XRD). Prior studies with genuine sludge from the K Basins have shown that specific uranium compounds and their alteration may affect the physical and chemical behaviors of products generated from 185°C hydrothermal treatment (Delegard et al. 2007a). The present work was performed to obtain uraninite, prepared by a commercial vendor via anoxic corrosion of uranium metal, oxidize aqueous suspensions of uraninite with dissolved oxygen gas to form metaschoepite, and characterize the uraninite, metaschoepite, and the reaction intermediates. Separate studies also were undertaken to determine if dissolved hydrogen gas is scavenged by metaschoepite to form reduced uranium compounds such as uraninite, ianthinite, or uranium octaoxide. Pure uraninite and metaschoepite compounds were to serve as feed material for further hydrothermal treatment tests that had been planned in accordance with Sludge Treatment Project (STP) corrosion process chemistry follow-on testing (Delegard et al. 2007b). Although most of the planned hydrothermal testing was cancelled in July 2007 (as described in the forward of Delegard et al. 2007b), uranium oxide procurement and lab tests on the preparation of metaschoepite by reaction of uraninite with oxygen, reaction of hydrogen with metaschoepite, and characterization of the various starting, product, and intermediate materials were continued to improve the understanding of uranium oxide chemistry in sludge and to provide well-characterized uranium oxides suited to support study of evolving STP processing alternatives (Sloughter 2007). (a) Testing with well characterized uranium oxide provides better experimental control and is significantly less costly than equivalent testing with the highly radioactive genuine sludge.