This work explores novel heterostructured uranium oxide materials for solar energy conversion through photoelectrochemical water splitting. Uranium oxides, with band-gap energies of 1.8-3.2 eV and favorable electrical and catalytic properties driven by the valence dynamics of uranium cations, show promise as electrode materials. Despite being considered scarce, large quantities of depleted uranium (e.g., 700,000 tons of UF6 in the USA) are stored as waste from nuclear fuel enrichment, posing environmental hazards due to potential release of toxic compounds. Although uranium oxides possess intriguing electronic and structural properties, they have not been extensively studied for energy applications due to limited synthetic accessibility. This research synthesizes various uranium metal-organic precursors and investigates their use in gas phase deposition techniques for uranium oxide coatings. Findings reveal that the phase composition of the resulting CVD deposits is significantly influenced by the oxidation state of uranium and ligand configuration. The thin films produced are assessed as potential photoelectrodes in water splitting setups, highlighting the largely unexplored potential of UOx compounds in (photo)chemical energy conversion. This effort is supplemented by ab-initio DFT calculations to elucidate processes related to water splitting reactions and examines the impact of the U:O ratio on band gap energies and thermo
