General project objectives. This project seeks a fundamental understanding and major improvement in cesium separation from high-level waste by cesium-selective calixcrown extractants. Systems of particular interest involve novel solvent-extraction systems containing specific members of the calyx(4)arene-crown-6 family, alcohol solvating agents, and alkylamines. Questions being addressed pertain to cesium binding strength, extraction selectivity, cesium stripping, and extractant solubility. Enhanced properties in this regard will specifically benefit cleanup projects funded by the USDOE Office of Environmental Management to treat and dispose of high-level radioactive wastes currently stored in underground tanks at the Savannah River Site (SRS), the Hanford site, and the Idaho National Environmental and Engineering Laboratory. The most direct beneficiary will be the SRS Salt Processing Project, which has recently identified the Caustic-Side Solvent Extraction (CSSX) process employing a calixcrown as its preferred technology for cesium removal from SRS high level tank waste. This technology owes its development in part to fundamental results obtained in this program.