This paper reports work to further develop a process to chlorinate uranium oxide and cause it to dissolve in a molten salt. The method was first reported by Japanese researchers and involves reaction with ZrCl₄ and Zr. The challenge with this approach is achieving a high concentration of ZrCl₄ in the molten salt due to its high volatility at the required operating temperature (500 °C). Two methods for introducing ZrCl₄ into the molten salt were explored in this study and found to be effective to cause formation of UCl₃. The first method consisted of in-situ reaction of NiCl₂ with zirconium metal in LiCl–KCl eutectic salt. Up to 0.337 wt% zirconium was dissolved in the salt with this method, and 0.386 wt% uranium was measured in the salt after 12 h. After these experiments, particles were cross-sectioned particles and revealed a skeletal ZrO₂ product layer formed around an unreacted UO₂ core. The second method was based on sublimating ZrCl₄ in flowing argon. Using this method, up to 2.56 wt% zirconium was achieved in the salt, and 0.652 wt% uranium was measured in the salt after 2 h. Cyclic voltammetry and open circuit potential electrochemical measurements both confirmed that primarily UCl₃ was formed in the salt mixture.