Photo‐Driven Iron‐Induced Non‐Oxidative Coupling of Methane to Ethane
Huizhen Zhang, Wanfu Zhong, Qiaobin Gong, Pengfei Sun, Xiaozhen Fei, Xuejiao Wu, Sha Xu, Qinghong Zhang, Gang Fu, Shunji Xie, Ye Wang
Abstract
Abstract Photo‐driven CH 4 conversion to multi‐carbon products and H 2 is attractive but challenging, and the development of efficient catalytic systems is critical. Herein, we construct a solar‐energy‐driven redox cycle for combining CH 4 conversion and H 2 production using iron ions. A photo‐driven iron‐induced reaction system was developed, which is efficient at selective coupling of CH 4 as well as conversion of benzene and cyclohexane under mild conditions. For CH 4 conversion, 94 % C 2 selectivity and a C 2 H 6 formation rate of 8.4 μmol h −1 is achieved. Mechanistic studies reveal that CH 4 coupling is induced by hydroxyl radical, which is generated by photo‐driven intermolecular charge migration of an Fe 3+ complex. The delicate coordination structure of the [Fe(H 2 O) 5 OH] 2+ complex ensures selective C−H bond activation and C−C coupling of CH 4 . The produced Fe 2+ can be used to reduce the potential for electrolytic H 2 production, and then turns back into Fe 3+ , forming an energy‐saving and sustainable recyclable system.