The technology of pyrochemical processing of mixed nitride uranium-plutonium spent fuel, realizable at the experimental and demonstration energy complex of the site of the Siberian Chemical Plant, includes several operations with the ultimate goal of isolating the target fission products. It’s planned to use the electrofining of the products of the previous stage, metallized spent nuclear fuel, аs the penultimate stage of processing. It’s necessary to determine the processes and technological modes of electrolytic refining of alloys modeling the product of this stage of the processing module to implement electrolytic refining. This paper presents the results of electrofining of model alloys (simulating the raw materials of the stage of electrofining processing) on an enlarged laboratory electrolyzer. The initial parameters of uranium refining processes in melts based on 3LiCl–2KCl–UCl3 were determined earlier. The basic parameters of refining were the use of electrolyte 3LiCl–2KCl–UCl3 (10.1 wt % UCl3) and conducting experiments at 550°C. Uranium alloys containing palladium and neodymium were prepared by direct fusion of uranium metal, PdAP-1 grade palladium metal powders and neodymium metal (99.99%) in a medium of high-purity argon (99.998%). The data obtained showed that at a temperature of 550°C, cathode precipitates are typical dendritic forms of alpha-uranium in rhombic syngony with a tendency to needle formation with an increase in cathode current density. An increase in the company time and cathode current density leads to a decrease in the current output due to short-circuiting of the electrodes with cathode sediment needles or metal shedding from the cathode. The modes of the cathode process have been experimentally refined as a result of electrofining. When electrofining alloys U–Pd(1.59 wt %), U–Pd(1.62 wt %), U–Pd(1.54 wt %), U–Pd(1.58 wt %)–Nd(5.64 wt %), U–Pd(1.84 wt %)–Nd(6.49 wt %), U–Pd(1.79 wt %)–Nd(6.54 wt %), uranium cathode precipitates were obtained, which were subjected to chemical analysis, which showed the high purity of the resulting metallic uranium, as well as the absence of metallic palladium and molybdenum in it. The palladium purification coefficient exceeds 5000, the neodymium purification coefficient exceeds 1000, which meets the requirements for purification from fission products at this stage of pyrochemical processing of spent fuel. Palladium accumulates in anode slime, while the bulk of neodymium passes into the molten electrolyte.