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Abstract
The partitioning of the long‐lived α‐emitters and the high‐yield fission products from dissolved used nuclear fuel is a key component of processes envisioned for the safe recycling of used nuclear fuel and the disposition of high‐level waste. These future processes will likely be based on aqueous solvent‐extraction technologies for light‐water reactor fuel and consist of four main components for the sequential separation of uranium, fission products, group trivalent actinides, and lanthanides, and then trivalent actinides from lanthanides. Since the solvent systems will be in contact with highly radioactive solutions, they must be robust toward radiolytic degradation in an irradiated mixed organic/aqueous acidic environment, with the formation of only benign degradation products. Therefore, an understanding of their radiation chemistry is important to the design of a practical system. In the first paper in this series, we reviewed the radiation chemistry of irradiated aqueous nitric acid and the tributyl phosphate ligand for uranium extraction in the first step of these extractions. In the second, we reviewed the radiation chemistry of the ligands proposed for use in the extraction of cesium and strontium fission products. Here, we review the radiation chemistry of the ligands that might be used for the group extraction of the lanthanides and actinides. This includes traditional organophosphorus reagents such as CMPO and HDEHP, as well as novel reagents such as the amides and diamides currently being investigated.