甲烷氧化偶联
环己烷
化学
催化作用
选择性
甲烷
光化学
分子间力
联轴节(管道)
氧化还原
能量转换效率
无机化学
材料科学
有机化学
分子
冶金
光电子学
作者
Huizhen Zhang,Wanfu Zhong,Qiaobin Gong,Pengfei Sun,Xiaozhen Fei,Xuejiao Wu,Sha Xu,Qinghong Zhang,Gang Fu,Shunji Xie,Ye Wang
出处
期刊:Angewandte Chemie
[Wiley]
日期:2023-04-22
卷期号:62 (25): e202303405-e202303405
被引量:22
标识
DOI:10.1002/anie.202303405
摘要
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.
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