Innovative deep decontamination of radioactive solid surfaces using microemulsions of deep eutectic solvents in supercritical carbon dioxide

Radioactive solid wastes resulting from the application of nuclear energy pose a risk to the environment, yet traditional decontamination methods generate many secondary wastes. Thus, sustainability-driven innovations are receiving increasing attention to achieve eco-friendly decontamination methods characterized by minimizing secondary waste generation. Here, we proposed a sustainable and pioneering approach to decontaminate radioactive solid wastes using microemulsions of deep eutectic solvents (DESs) in supercritical carbon dioxide (SC-CO2). We also determined the optimal ratios of the additives as follows: prepared DESs with a molar ratio of choline chloride (ChCl) to p-toluenesulfonic acid monohydrate (ptsa) of 1:2, and nonyl phenol polyoxyethylene ether (NP-10) to ChCl:ptsa DESs in a molar ratio of 0.8. Remarkably, after optimization of the decontamination process in terms of pressure, temperature and cleaning time, the radioactivity on the sample surface can be reduced to a level that is reusable in the nuclear field. Detailed analyses provided insights into the intermolecular interactions within the DESs. And the decontamination mechanisms involved the spontaneous evolution of microemulsions with ChCl:ptsa as the core to facilitate the solvation and removal of radioactive contaminants. Additionally, repeated cleaning was proved to be effective for ultra-deep decontamination, with the radioactivity on the sample surface reaching a clearance level and a decontamination efficiency of 99.8%. The DESs-in-CO2 systems successfully decontaminated various materials and simulated radionuclides, even real radioactive metal wastes from the nuclear industry. It was notable that the DESs-in-CO2 systems achieved decontamination efficiencies of more than 95.0% for radioactive contaminants on these solid surfaces. Overall, this innovative approach provided a green alternative to conventional radioactive solids decontamination, meeting the need for sustainable development of nuclear energy.