Abstract: There are many kinds of unqualified uranium containing materials with large stock. In order to improve the utilization rate of uranium and meet the stable supply of materials needed for fuel element production, uranium recycling is needed. It is introduced that U₃Si₂ powder can be converted into uranium oxides in calcinations process, after which the uranium oxides will react with solid NH₄F to generate UF₄. There are several factors in the producing process such as the amount of fluoride, temperature, reacting time, etc. Thus, the optimal reacting conditions are found. According to all these experiments, it can be inferred that U₃Si₂ powder after calcination and oxidation would react with solid NH₄F or NF₄HF₂ to generate UF₄. The UF₄ products will be up to the standard, meanwhile the amount of UO₂F₂ in UF₄ can be reduced to lowest level if the reacting temperature remained at 500℃ and preserving for 4.5 hours.