Photo‐driven CH4 conversion to multi‐carbon products and H2 is attractive but challenging, and the development of efficient catalytic systems is critical. Herein, we construct a solar‐energy‐driven redox cycle for combining CH4 conversion and H2 production using iron ions. A photo‐driven iron‐induced reaction system was developed, which is efficient at selective coupling of CH4 as well as conversion of benzene and cyclohexane under mild conditions. For CH4 conversion, 94 % C2 selectivity and a C2H6 formation rate of 8.4 μmol h−1 is achieved. Mechanistic studies reveal that CH4 coupling is induced by hydroxyl radical, which is generated by photo‐driven intermolecular charge migration of an Fe3+ complex. The delicate coordination structure of the [Fe(H2O)5OH]2+ complex ensures selective C−H bond activation and C−C coupling of CH4. The produced Fe2+ can be used to reduce the potential for electrolytic H2 production, and then turns back into Fe3+, forming an energy‐saving and sustainable recyclable system.
The electrochemical process of coupling electrocatalytic CO2 reduction and organic conversion reaction can effectively reduce the reaction overpotential and obtain value‐added chemicals. Moreover, because of the diversity of substrates and the designability of coupling forms, more and more attention has been paid to this field. This review systematically summarizes the research progress of coupling electrolysis in recent years, (1) co‐electrolysis of CO2 and organics at the cathode to obtain specific products with high selectivity, (2) replacing traditional anodic oxygen evolution reaction (OER) with other valuable oxidation reactions to improve energy utilization efficiency and economic benefits of CO2 conversion, (3) in an electrolytic cell without membrane, the cathode and anode jointly transform CO2 and organics to redox products. We hope that the examples and insights on coupling electrolysis introduced in this review can inspire researchers to further explore and innovate in this direction.
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