Historically, both the BUTEX (dibutyl carbitol-based) and PUREX (tributyl phosphate-based) processes have been used for uranium recovery and purification. Currently, BUTEX- and PUREX-type extraction processes are being used in series for recovery of isotopically enriched uranium at the Oak Ridge Y-12 Plant. The use of two solvents is predicated on the differing selectivities of each with regard to the contaminant elements present in the uranium source stream. As part of efforts to streamline plant operations in response to decreasing throughput requirements, the Y-12 Development Division is evaluating options for converting the existing two-solvent operation to a single-solvent process. At the request of the Y-12 Development Division, the Robotics and Process Division at the Oak Ridge National Laboratory has undertaken evaluation of solvents for use in a single-solvent recovery process. Initial efforts have been directed toward development of a single-solvent, dibutyl carbitol- or tributyl phosphate-based process that produces a product with purity equal to or exceeding what is currently obtained in the two-cycle, two-solvent operation. The test effort has involved both laboratory equilibrium determinations and engineering-scale process demonstrations in multistage flowsheets using centrifugal solvent extraction contactors. Excellent uranium recovery results have been obtained from both dibutyl carbitol- and tributyl phosphate-based solvent extraction flowsheets. Contaminant rejection performance by the two solvents is similar for many of the elements considered. Extraction of some contaminant elements by tributyl phosphate is significant enough to conclude that the solvent is not as selective for uranium as is dibutyl carbitol. This determination does not necessarily eliminate: tributyl phosphate from consideration for use in a single-solvent process but does indicate a need for effective scrubbing of contaminants from uranium-loaded tributyl phosphate, possibly by partial reflux of the purified, aqueous uranyl nitrate product solution.