Uncertainty studies of real anode surface area in computational analysis for molten salt electrorefining

Highlights: → Numerical electrochemo-fluid modeling of pyrochemical electrorefining in cross comparison with 2D and 3D analysis models. → Benchmark study on cell potential of molten LiCl-KCl electrorefining with Mark-IV electrorefiner containing EBR-II spent fuel. → Determination of real anode surface area profile model governing electrorefining performance. → Identification of uncertainty factors in electrorefining causing disagreements between simulation and experiment. → Fully transient performance analysis of 80 hours Mark-IV electrorefining with multi-species multi-reaction 1D model. - Abstract: This study examines how much cell potential changes with five differently assumed real anode surface area cases. Determining real anode surface area is a significant issue to be resolved for precisely modeling molten salt electrorefining. Based on a three-dimensional electrorefining model, calculated cell potentials compare with an experimental cell potential variation over 80 h of operation of the Mark-IV electrorefiner with driver fuel from the Experimental Breeder Reactor II. We succeeded to achieve a good agreement with an overall trend of the experimental data with appropriate selection of a mode for real anode surface area, but there are still local inconsistencies between theoretical calculation and experimental observation. In addition, the results were validated and compared with two-dimensional results to identify possible uncertainty factors that had to be further considered in a computational electrorefining analysis. These uncertainty factors include material properties, heterogeneous material distribution, surface roughness, and current efficiency. Zirconium's abundance and complex behavior have more impact on uncertainty towards the latter period of electrorefining at given batch of fuel. The benchmark results found that anode materials would be dissolved from both axial and radial directions at least for low burn-up metallic fuels after active liquid sodium bonding was dissolved.