Interests in molten salt reactor (MSR) using a fast spectrum (FS) have been increased not only for having a high power density but for burning the high-level waste generated from nuclear power plants. For developing the FS-MSR technologies, chloride-based fuels are considered due to the advantage of higher solubility of actinides and lanthanides over fluoride-based salts. Despite significant progress in development of MSR technology, the manufacturing technology for production of the fuel is still insufficiently understood. One of the option to prepare the MSR fuel is to use products from pyroprocessing where oxide form of spent nuclear fuel is reduced into metal form and useful elements can be collected via electrochemical methods in molten salt system at high temperature. In order to chlorinate the products into chloride form, previous study used NH4Cl to chlorinate U metal into UCl3 in an airtight reactor. It was found that the U metal was completely chlorinated into chloride forms; however, impurities generated by the reaction of NH4Cl and reactor wall were found in the product. Therefore, in this work, the air tight reactor was re-deigned to avoid the reaction of reactor wall by insertion of Al2O3 crucible inside of the reactor. In addition, the reactor size was increased to produce UCl3 over 100 g. Using the newly designed reactor, U metal chlorination experiments using NH4Cl chlorinating agent were performed to confirm the optimal experimental conditions. The detailed results will be further discussed.

The effect of Li2O addition on precipitation behavior of uranium in LiCl-KCl-UCl3 has been investigated in this study. 99.99% LiCl-KCl eutectic salt is mixed with 10wt% UCl3 chips at 550°C in the Pyrex tube in argon atmosphere glove box, with 10 ppm O2 and 1 ppm H2O. Then, Li2O chunks are added in mixed LiCl-KCl-UCl3 and the system has been cooled down to room temperature for 10 hours to form enough UO2 particles in the salt. The solid salt has been taken out from the glove box, and cut into three sections (top, middle and bottom) by low-speed saw for further microscopic analysis. Three pieces of solid salt are dissolved in deionized water at room temperature and the solution is filtered by a filter paper to collect non-dissolved particles. The filter paper with particles is baked in vacuum oven at 120°C for 6 hours to evaporate remaining moisture from the filter paper. Further analysis was performed for the powder remaining on the filter paper, and periphery of the powder (cake) on the filter paper. Scanning electron microscopy (SEM), electron diffraction spectroscopy (EDS), and X-ray powder diffraction (XRD) are adopted to analysis the characteristic of the particles. From SEM analysis, the powders are consisted of small particles which have 5 to 10 m diameter, and EDS analysis shows they are likely UO2 with 23 at. % of uranium and 77 at. % oxygen. Cake is also analyzed by SEM and EDS, and needle like structures are widely observed on the particle. The length of needle is distributed from 5 to 20 m, and it has 6 to 10 at. % of chlorine, which are not fully dissolved into deionized water at room temperature. From XRD analysis, the particles show the peak position of UO2, and the result is well matched with the SEM-EDS results. We are planning to add more Li2O in the system for fully reacting uranium in UCl3, and compare the results to find the effect of Li2O concentration on UO2 precipitation.