Switchable All Inorganic Halide Perovskite Nanocrystalline Photoelectrodes for Solar‐Driven Organic Transformations

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All inorganic halide perovskite nanocrystals (NCs) are considered as fascinating materials for a wide range of optoelectronic applications encompassing photovoltaics, lasing, sensing, and photocatalysis due to their outstanding optoelectronic properties. Herein, it is demonstrated that the photoelectrochemical behavior of CsPbBr 3 NC films can be tailored through engineering the selective contacts and accepting species in the electrolyte. This concept has been successfully applied to the photoelectrochemical oxidation of benzyl alcohol (BzOH) to benzyl aldehyde (BzCHO) and the reverse photoelectrochemical reduction of BzCHO to BzOH, demonstrating that CsPbBr 3 NCs activate both reactions with photocurrents up to 40 μA cm −2 toward BzCHO production and 5 μA cm −2 for the reverse reaction at 0.15 V versus normal hydrogen electrode. The obtained results highlight the huge potential and versatility of halide perovskite NCs for photoelectrocatalytic applications, validating the implementation of these materials for a wide range of solar‐driven complex organic transformations, and emphasizing the urgent need for stabilization strategies to move beyond the proof‐of‐concept stage to relevant technological developments.