Synthesis of eutectic UCl3–NaCl–KCl and UCl3–NaCl by chlorination of uranium metal with ZnCl2
摘要
Candidate fuel mixtures for molten chloride fast reactors require a high concentration (> 30 mol%) of UCl3 to form a eutectic mixture with a sufficiently low melting point. This work describes a novel way of producing the ternary UCl3–NaCl–KCl eutectic and the binary UCl3–NaCl eutectic by chlorinating uranium metal with ZnCl2 starting with a low melting point molten ZnCl2–NaCl–KCl mixture and ZnCl2–NaCl mixture. This method produces the desired salt after complete reaction of the ZnCl2. The three synthesis runs described here resulted in two near-eutectic mixtures of UCl3–NaCl–KCl with UCl3 concentrations of 31 and 35 mol % with Na/K mol ratios of 2.33 and 2.37 as well as one near-eutectic mixture of UCl3–NaCl with 32 mol % UCl3. It is shown that the ternary synthesis can be performed entirely in the liquid phase below 550 °C and results in a salt with a melting point between 468–482 °C. The binary synthesis can be performed below 575 °C and results in a salt with a melting point of 527 °C. The Zn byproduct of this reaction is readily removed by distillation above 450 °C and has a final concentration less than 0.1 wt% in the final salt product. When a U–Zr pellet is used instead of pure U for chlorinating, ZrCl4 is first formed in the melt which either vaporizes out or later reacts with excess U to form UCl3. The final ZrCl4 content in the salt is easily reduced to less than 0.01 wt %.