| Institution: | 1. State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005 Fujian, P. R. China
These authors contributed equally to this work.;2. State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005 Fujian, P. R. China;3. Center for Sustainable Catalysis and Engineering, Faculty of Bioscience Engineering, KU Leuven, 3001 Heverlee, Belgium |
| Abstract: | 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. |
