In Situ Growth of Nanostructured BiVO4-Bi2O3 Mixed-Phase via Non-Equilibrium Deposition Involving Metal Exsolution for Enhanced Photoelectrochemical Water Splitting.

Non-equilibrium deposition is a remarkable method for in situ growth of unique nanostructures and phases for the functionalization of thin films. We introduce a distinctive structure of mixed-phase, composed of BiVO4 and β-Bi2O3, for photoelectrochemical water splitting. The mixed-phase is fabricated via non-equilibrium deposition by adjusted the oxygen partial pressure. According to density functional theory calculations, we find that vanadium exsolution can be facilitated by introducing oxygen vacancies, enabling the fabrication of nanostructured mixed-phase. These unique structures enhance charge migration by increasing the interfacial area and properly aligning the band offset between two crystalline phases. Consequently, the photocurrent density of the nanostructured mixed-phase thin films is about twice that of pristine BiVO4 thin films at 1.23 VRHE. Our work suggests that non-equilibrium deposition provides an innovative route for the structural engineering of photoelectrodes for the understanding of fundamental properties and for improving photocatalytic performance for solar water splitting.

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