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Abstract Nature is capable of storing solar energy in chemical bonds via photosynthesis through a series of C–C, C–O and C–N bond-forming reactions starting from CO₂and light. Direct capture of solar energy for organic synthesis is a promising approach. Lead (Pb)-halide perovskite solar cells reach 24.2% power conversion efficiency, rendering perovskite a unique type material for solar energy capture. We argue that photophysical properties of perovskites already proved for photovoltaics, also should be of interest in photoredox organic synthesis. Because the key aspects of these two applications are both relying on charge separation and transfer. Here we demonstrated that perovskites nanocrystals are exceptional candidates as photocatalysts for fundamental organic reactions, for example C–C, C–N and C–O bond-formations. Stability of CsPbBr₃in organic solvents and ease-of-tuning their bandedges garner perovskite a wider scope of organic substrate activations. Our low-cost, easy-to-process, highly-efficient, air-tolerant and bandedge-tunable perovskites may bring new breakthrough in organic chemistry. 

Abstract Metal‐halide perovskites have been explored as photocatalysts for CO₂reduction. We report that perovskite photocatalytic CO₂reduction in organic solvents is likely problematic. Instead, the detected products (i.e., CO) likely result from a photoredox organic transformation involving the solvent. Our observations have been validated using isotopic labeling experiments, band energy analysis, and new control experiments. We designed a typical perovskite photocatalytic setup in organic solvents that led to CO production of up to ≈1000 μmol g⁻¹ h⁻¹. CO₂reduction in organic solvents must be studied with extra care because photoredox organic transformations can produce orders of magnitude higher rate of CO or CH₄than is typical for CO₂reduction routes. Though CO₂reduction is not likely to occur, in situ CO generation is extremely fast. Hence a suitable system can be established for challenging organic reactions that use CO as a feedstock but exploit the solvent as a CO surrogate.