The photoelectrochemical production of fuels, exemplified by light‐driven water splitting to hydrogen and oxygen, offers a sustainable option to offset dependence on fossil fuels. A low‐cost, efficient, and stable photoelectrochemical approach to solar fuels remains elusive but using similar materials and photoelectrodes for chemical production or biomass conversion offers an appealing alternative. This work reports a facile method for fabricating pristine (undoped) BiVO4 photoanodes to carry out TEMPO‐mediated benzyl alcohol oxidation to benzaldehyde in organic media (TEMPO=2,2,6,6‐tetramethylpiperidinyl‐N‐oxyl). The best performing BiVO4 photoanode studied here gave a faradaic efficiency (FE) of 85±5% for benzaldehyde formation in the presence of TEMPO and pyridine during a 2.5‐hour reaction. Compared with direct electrocatalytic conversion under the same conditions, light capture and conversion by the BiVO4 surface decreased the required applied bias by 46 %. To our knowledge, this is the first report of visible light assisted, TEMPO‐mediated benzyl alcohol oxidation using pristine BiVO4 photoanodes in organic media.

If generated from water using renewable energy, hydrogen could serve as a carbon-zero, environmentally benign fuel to meet the needs of modern society. Photoelectrochemical cells integrate the absorption and conversion of solar energy and chemical catalysis for the generation of high value products. Tandem photoelectrochemical devices have demonstrated impressive solar-to-hydrogen conversion efficiencies but have not become economically relevant due to high production cost. Dye-sensitized solar cells, those based on a monolayer of molecular dye adsorbed to a high surface area, optically transparent semiconductor electrode, offer a possible route to realizing tandem photochemical systems for H2 production by water photolysis with lower overall material and processing costs. This review addresses the design and materials important to the development of tandem dye-sensitized photoelectrochemical cells for solar H2 production and highlights current published reports detailing systems capable of spontaneous H2 formation from water using only dye-sensitized interfaces for light capture.

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