Non‐<i>C2</i>‐Symmetric Complexant for Minor Actinide Separation of Actinides from Lanthanides

Advancements in the separation of the minor actinides (An) from the neutron-poisoning post fission lanthanides (Ln) via the partitioning and transmutation strategy are vital toward closure of the nuclear fuel cycle, decreasing dependence on fossil fuels, and minimizing the environmental impact of energy production. Recent advancements in complexant-based separations strategies have realized substantive gains in ease of synthetic access, process-relevant diluent solubility, in addition to stability in strongly acidic environments. As purposeful exploration of chemoselective chelating agents moves forward, rapid, selective, and reversible actinide binding are at the forefront. In this work, the utility of a non-C2-symmetric, bis-1,2,4-triazinylpyridine (BTP)-type complexant for the selective extraction of ²⁴¹Am³⁺ over ^154-152Eu³⁺ from simulated high-level waste is reported. High separation factors (SFs) in 1-octanol:kerosene 50:50 (v/v), equilibration within 15 minutes of contact time, decomplexation with dilute acid only, and recyclability of a discrete complexant for additional extractions were achieved. Separations, spectroscopic, and DFT calculation data supporting the observed experimental results are disclosed herein.