Gas-solid reaction pathway for chlorination of rare earth and actinide metals using hydrogen and chlorine gas

Hydriding and chlorination of buttons of metallic cerium have been tested as a head-end step to separating metal impurities from actinides. The objective was to achieve complete conversion to chlorides while maintaining high surface area via small particles and open porosity. Hydriding by reaction with 100% H-2 gas at 573 K was successful at reducing cm-scale metal buttons into small particles/fragments. This step was followed by reaction with flowing 99.5% anhydrous Cl-2 gas at temperatures ranging from 423 to 573 K for 60 min. In experiments reported here, up to 92% conversion to cerium chloride was achieved from reacting with the anhydrous chlorine gas. The final chloride product has high porosity coupled with small particle sizes (microns to 1600 mu m), which makes it suitable for subsequent purification processes. Higher chlorine concentrations in the gas favor higher conversion to chloride. The optimal temperature to achieve high chlorination is 523 K. Oxygen is a minor impurity in the chlorine gas which appears to prevent complete chlorination from being achieved. (C) 2020 Elsevier B.V. All rights reserved.