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Abstract Semi‐artificial photoelectrochemistry can combine state‐of‐the‐art photovoltaic light‐absorbers with enzymes evolved for selective fuel‐forming reactions such as CO 2 reduction, but the overall performance of such hybrid systems has been limited to date. Here, the electrolyte constituents were first tuned to establish an optimal local environment for a W‐formate dehydrogenase to perform electrocatalysis. The CO 2 reductase was then interfaced with a triple cation lead mixed‐halide perovskite through a hierarchically structured porous TiO 2 scaffold to produce an integrated photocathode achieving a photocurrent density of −5 mA cm −2 at 0.4 V vs. the reversible hydrogen electrode during simulated solar light irradiation. Finally, the combination with a water‐oxidizing BiVO 4 photoanode produced a bias‐free integrated biophotoelectrochemical tandem device (semi‐artificial leaf) with a solar CO 2 ‐to‐formate energy conversion efficiency of 0.8 %.
Moore et al. (Thu,) studied this question.