Proceedings of nanoGe Fall Meeting 2018 (NFM18)
DOI: https://doi.org/10.29363/nanoge.nfm.2018.337
Publication date: 6th July 2018
New semiconductor metal oxides capable of driving water-splitting reactions by solar irradiation alone are required for sustainable hydrogen production. Whereas most metal oxides only marginally deliver the photochemical energy to split water molecules, uranium oxides are efficient photoelectrocatalysts due to their absorption properties (Eg ~ 2.0 - 2.6 eV) and easy valence switching among uranium centers that additionally augment the photocatalytic efficiency. Although considered a scarce resource, the abundance of uranium compounds in the environment is manifested in the huge quantities of stored UF6 gas, produced as waste streams in the nuclear fuel enrichment process. Here we demonstrate that thin films of depleted uranium oxide (U3O8) and their bilayers with hematite (a-Fe2O3) are high activity water oxidation catalysts due to electronically coupled phase boundaries. The electronic structure of uranium oxides showed an optimal band edge alignment in U3O8//Fe2O3 bilayers (DFT calculations) resulting in improved charge-transfer at the heterojunction as supported by TAS and XAS measurements. The enhanced photocurrent density of the heterostructures with respect to well-known hematite offers unexplored potential of uranium oxide in artificial photosynthesis.
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