Highly efficient conversion of methane to formic acid under mild conditions at ZSM-5-confined Fe-sites

作者：Kai-Xin Zhu, Suxia Liang, Xiao-Ju Cui, Rui Huang, Ning-Bo Wan, Lei Hua, Hai-Yang Li, Hongyu Chen, Zhen-Chao Zhao, Guangjin Hou, Mingrun Li, Qi-Ke Jiang, Liang Yu, De-Hui Deng · 发表于：Nano Energy · 年份：2021 · DOI：10.1016/j.nanoen.2020.105718 · 被引用次数：73 · 研究领域：Materials Science

Abstract Production of value-added chemicals from oriented methane conversion under mild conditions is of great significance for utilization of the energy resources, which, however, remains a great challenge due to its difficulty in the selective activation of C–H bond. Herein, we report a highly selective and efficient methane conversion to formic acid on atomically dispersed Fe sites confined in the nano-channels of ZSM-5. The turnover frequency for producing C1 liquid oxygenates reaches 84,200 h−1 with a high selectivity of 91% to formic acid at 80 °C, which outperforms all previously reported catalysts. Electron paramagnetic resonance analysis and density functional theory calculations demonstrate that the ZSM-5-confined Fe-O active centers can facilely dissociate the C–H bonds and catalyze successive oxidation of methane to formic acid via free radical mechanisms under mild conditions. This study opens a new path of engineering the microenvironment of confined Fe sites within nano-channels toward highly selective methane conversion with low energy input.