The trivalent lanthanide-actinide separations are a major challenge in reprocessing of nuclear fuels. To achieve this, commonly organic extractants and solvents are utilized in elaborate processes. Here we report a simple new method that can perform a supportive or alternative role. A nanocrystalline α-zirconium phosphate ion exchanger was utilized for Eu(III)/Am(III) column separation. Comprehensive preliminary studies were done using batch experiments to optimize the final separation conditions. The distribution coefficients for Eu were determined as a function of pH (from 0 to 3) and salinity (Na, Sr). The distribution coefficients for Am were determined as a function of pH, and Eu concentration, from 1:40 to 10,000:1 Eu:Am molar ratio. The exchanger always preferred Eu over Am in our experimental conditions. Separation factors (Eu:Am) of up to 400 were achieved in binary Eu-Am solution in pH 1. The breakthrough capacity was determined in dynamic column conditions using Eu: 0.3 meq∙g−1, which is approximately 4% of the theoretical maximum capacity. Two types of hot column separation tests were conducted: (i) binary load (selective Am elution), and (ii) continuous equimolar binary feed. In both cases separation was achieved. In (i), the majority (82% of the recovered 93%) of Am could be purified from Eu with extremely high 99.999% molar purity, while alternatively even more (95% of the recovered 93%) at a lower purity of 99.7 mol %. In (ii), up to 330 L∙kg−1 of the equimolar solution per mass of the exchanger could be treated with Am purity above 99.5 mol % in the total eluate. Alternatively, up to 630 L∙kg−1 above 95 mol %, or up to 800 L∙kg−1 above 90 mol % purities.
Fields of Science
- 116 Chemical sciences