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Photosynthesis is nature's route to convert intermittent solar irradiationinto storable energy, while its use for an industrial energy supply is impairedby low efficiency. Artificial photosynthesis provides a promising alternativefor efficient robust carbon-neutral renewable energy generation. The approachof direct hydrogen generation by photoelectrochemical water splitting utilisescustomised tandem absorber structures to mimic the Z-scheme of naturalphotosynthesis. Here, a combined chemical surface transformation of a tandemstructure and catalyst deposition at ambient temperature yields photocurrentsapproaching the theoretical limit of the absorber and results in asolar-to-hydrogen efficiency of 14%. The potentiostatically assistedphotoelectrode efficiency is 17%. Present benchmarks for integrated systems areclearly exceeded. Details of the in situ interface transformation, theelectronic improvement and chemical passivation are presented. The surfacefunctionalisation procedure is widely applicable and can be preciselycontrolled, allowing further developments of high-efficiency robust hydrogengenerators.

Efficient Direct Solar-to-Hydrogen Conversion by In Situ Interface Transformation of a Tandem Structure