Separation of Plutonium from Irradiated Fuels and Targets

Spent nuclear fuel from power production reactors contains moderate amounts of transuranium (TRU) actinides and fission products in addition to the still slightly enriched uranium. Originally, nuclear technology was developed to chemically separate and recover fissionable plutonium from irradiated nuclear fuel for military purposes. Military plutonium separations had essentially ceased by the mid-1990s. Reprocessing, however, can serve multiple purposes, and the relative importance has changed over time. In the 1960’s the vision of the introduction of plutonium-fueled fast-neutron breeder reactors drove the civilian separation of plutonium. More recently, reprocessing has been regarded as a means to facilitate the disposal of high-level nuclear waste, and thus requires development of radically different technical approaches. In the last decade or so, the principal reason for reprocessing has shifted to spent power reactor fuel being reprocessed (1) so that unused uranium and plutonium being recycled reduce the volume, gaining some 25% to 30% more energy from the original uranium in the process and thus contributing to energy security and (2) to reduce the volume and radioactivity of the waste by recovering all long-lived actinides and fission products followed by recycling them in fast reactors where they are transmuted to short-lived fission products; this reduces the volume to about 20%, reduces the long-term radioactivity level in the high-level waste, and complicates the possibility of the plutonium being diverted from civil use – thereby increasing the proliferation resistance of the fuel cycle. In general, reprocessing schemes can be divided into two large categories: aqueous/hydrometallurgical systems, and pyrochemical/pyrometallurgical systems. Worldwide processing schemes are dominated by the aqueous (hydrometallurgical) systems. This document provides a historical review of both categories of reprocessing.