A theoretical model is used to analyze the transport of U and Zr in electro
refining of irradiated binary Experimental Breeder Reactor-II fuel, A limit
ing-current hypothesis is advanced to explain the observed dissolution of Z
r in the presence of U at high, intermediate, and low cell voltages. The in
ternal diffusion model predicts the existence of a critical current and a c
ritical voltage for Zr oxidation. Experimental results are presented for a
test designed and run based on optimum conditions determined from the model
to dissolve U expediently while retaining Zr in the anode baskets. A simpl
e model of kinetic exchange reactions between salt-phase U and Cd-phase Zr
is formulated to explain the measured electrodeposition of Zr on the solid
cathode. It is shown that the Zr content of the deposit is overpredicted if
the pool is considered isolated and grossly underpredicted if the salt pha
se is equilibrated instantaneously with the Cd pool. Finally, the aspects o
f anodic current efficiency and cathodic collection efficiency are discusse
d taking into account shorting between the dissolution baskets and the Cd p
ool, multiple oxidation stares of Zr, and the exchange reactions between th
e fuel and UCl3 prior to electrotransport.