Spent Nuclear Fuel–Waste to Resource, Part 2: Radiolytic Hydrogen Production—A Novel Approach to Sustainably Meeting the World’s Hydrogen Needs from the Nuclear Fuel Cycle

Nuclear cogeneration is increasingly proposed to support decarbonisation, partly via hydrogen (H2) production through electrolysis, thermolysis, or a combination of these, but wide-scale adoption is limited by process inefficiencies, high costs, and concerns around nuclear wastes. Recent work has demonstrated that gamma radiation, sourced from 137Cs, splits water into H2 at high yields with a TiO2 photocatalyst, extrapolating that the world’s spent nuclear fuel (SNF) stockpiles could generate ~60% of world hydrogen demand, worth ~90 billion USD/y. This is achievable using present technology and would valorise SNF, which is commonly viewed as a waste, and decouple H2 production from reactor operations, but would limit operations to open fuel cycles, replacing the cooling ponds therein. By combining advanced separations in SNF recycle, partitioning the high-heat radionuclides (137Cs, 134Cs, and 90Sr) responsible for most SNF radiation, and forming these into dedicated sources for hydro