Catalytic reduction of U(VI) to U(IV) using hydrogen as the sole reducing agent

Using hydrogen gas as a sole reducing agent to catalyze the reduction of hexavalent uranium to prepare tetravalent uranium can avoid the problem of pollutant poisoning catalysts caused by hydrazine reducing agents. However, research using only hydrogen as the sole reducing agent is very scarce. Herein, catalyst has been developed for catalytic hydrogen reduction to prepare uranium(IV) and a systematic study of the influence of process parameters such as catalyst carrier particle size, temperature, pressure, and acidity on the catalytic hydrogen reduction process for the preparation of uranium(IV) is presented. The effect of catalyst carrier particle size is particularly pronounced due to the differing rates of molecular diffusion. Fine particle-sized catalyst carriers exhibit faster catalytic reaction kinetics. Temperature exhibits an unusual phenomenon in its impact on the reaction process. As temperature increases, the reaction rate decreases, and an upper limit reaction temperature is observed. Furthermore, at excessively high reaction temperatures, an anomalous occurrence of uranium(IV) formation followed by disappearance was observed. Through an analysis of the reaction mechanism, the underlying reasons for this abnormal phenomenon are elucidated. Additionally, this paper also reveals that reaction rates increase with increasing reaction pressure and decrease with decreasing raw material acidity. Process parameters such as reaction temperature, pressure, and acidity exhibit coupled effects on the reaction process. Different reaction upper limit temperatures are observed under varying pressures and raw material acidities.