Abstract

A program based upon thermodynamic values and scouting experiments at Argonne National Laboratory is proposed for development of a pyrochemical head-end treatment of spent nuclear fuels to replace the proposed chopping and leaching operation in the Purex process. The treatment consists of separation of the cladding from the oxide fuel by dissolution into liquid zinc; oxide reduction of uranium and plutonium and dissolution into a zinc--magnesium alloy; separation of alkali, alkaline earth, and rare earth fission products into a molten salt; and, finally, separation and recovery of the plutonium and uranium in the alloy. Uranium and plutonium would be separated from the fuel cladding and selected fission products in a form readily dissolvable in nitric acid. The head-end process could be developed eventually into an optimum method for recovering uranium, plutonium, and selected fission products and for minimizing wastes as compact, stable solids. Developmental expenses are not known clearly, but the potential advantages of the process are impressive.

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