Abstract
To properly manage nuclear wastes is critical to sustainable utilization of nuclear power and environment health. Here, we show an innovative carbiding strategy for sustainable management of radioactive graphite through digestion of carbon in H2O2. The combined action of intermolecular oxidation of graphite by MoO3 and molybdenum carbiding demonstrates success in gasifying graphite and sequestrating uranium for a simulated uranium-contaminated graphite waste. The carbiding process plays a triple role: (1) converting graphite into atomic carbon digestible in H2O2, (2) generating oxalic ligands in the presence of H2O2 to favor U-precipitation, and (3) delivering oxalic ligands to coordinate to MoVI-oxo anionic species to improve sample batching capacity. We demonstrate > 99% of uranium to be sequestrated for the simulated waste with graphite matrix completely gasifying while no detectable U-migration occurred during operation. This method has further been extended to removal of surface carbon layers for graphite monolith and thus can be used to decontaminate monolithic graphite waste with emission of a minimal amount of secondary waste. We believe this work not only provides a sustainable approach to tackle the managing issue of heavily metal contaminated graphite waste, but also indicates a promising methodology toward surface decontamination for irradiated graphite in general.
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