Chlorination of TRU/RE/SrOx in Oxide Spent Nuclear Fuel Using Ammonium Chloride as a Chlorinating Agent

Thermodynamically, TRUOx, REOx, and SrOx can be chlorinated using ammonium chloride (NH4Cl) as a chlorinating agent, whereas uranium oxides (U3O8 and UO2) remain in the oxide form. In the preliminary experiments of this study, U3O8 and CeO2 are reacted separately with NH4Cl at 623 K in a sealed reactor. CeO2 is highly reactive with NH4Cl and becomes chlorinated into CeCl3. The chlorination yield ranges from 96% to 100%. By contrast, U3O8 remains as UO2 even after chlorination. We produced U/REOx- and U/SrOx-simulated fuels to understand the chlorination characteristics of the oxide compounds. Each simulated fuel is chlorinated with NH4Cl, and the products are dissolved in LiCl-KCl salt to separate the oxide compounds from the chloride salt. The oxide compounds precipitate at the bottom. The precipitate and salt phases are sampled and analyzed via X-ray diffraction, scanning electron microscope-energy dispersive spectroscopy, and inductively coupled plasma-optical emission spectroscopy. The analysis results indicate that REOx and SrOx can be easily chlorinated from the simulated fuels; however, only a few of U oxide phases is chlorinated, particularly from the U/SrOx-simulated fuels.