文献类型：期刊文献

英文题名：Fe-(μ-O)-Zn dual-atom boosting C-C coupling for direct oxidation of methane to acetic acid using O2

作者：Yu, Baiyang[1,2];Li, Wenlong[3,4];Tang, Xuan[3,4];Cheng, Lu[3,4];Zhang, Jiawei[1,2];Yang, Shuobing[1,2];Liu, Fudong[5];Xu, Jing[6];Zhang, Ying[1,2];Pan, Chengsi[1,2];Cao, Xiao-Ming[7];Zhu, Yongfa[8];Lou, Yang[1,2]

机构：[1]Jiangnan Univ, Sch Chem & Mat Engn, Key Lab Synthet & Biol Colloids, Minist Educ, Wuxi, Jiangsu, Peoples R China;[2]Jiangnan Univ, Int Joint Res Ctr Photorespons Mol & Mat, Wuxi, Jiangsu, Peoples R China;[3]East China Univ Sci & Technol, Ctr Computat Chem, Shanghai, Peoples R China;[4]East China Univ Sci & Technol, Res Inst Ind Catalysis, Shanghai, Peoples R China;[5]Univ Calif Riverside, Dept Chem & Environm Engn, Riverside, CA USA;[6]Jiangnan Univ, Sch Food Sci & Technol, Wuxi, Jiangsu, Peoples R China;[7]Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, Shanghai, Peoples R China;[8]Tsinghua Univ, Dept Chem, Beijing, Peoples R China

年份：2025

卷号：16

期号：1

外文期刊名：NATURE COMMUNICATIONS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:001603687300020)】；

基金：This project was supported financially by the National Key R&D Program of China (2021YFB3501900, 2023YFA1507601), National Natural Science Foundation of China (U21A20326, 22172065, 22306063, and 22022302), Natural Science Foundation of Jiangsu Province (BK20211239), and Jiangsu Specially-Appointed Professor (1046010241211400). We thank the Center for High Performance Computing at Shanghai Jiao Tong University for providing the computing resources of the Siyuan-1 cluster. We acknowledge support from Lixia Yan (Analysis and Testing Center of Jiangnan University) for the help with the HRTEM/STEM test.

语种：英文

摘要：Direct oxidation of methane (DOM) into high-value C2+ products using molecular oxygen (O2) is essential for the sustainable production of clean energy and bulk chemicals, but is still challenging due to the difficult C-H activation and uncontrollable C-C coupling process. Herein, we design and construct the Fe-(mu-O)-Zn dual-atom sites by supporting Fe and Zn atoms on ZSM-5 (Fe1-Zn1/ZSM-5), which achieves the DOM by O2 to acetic acid under ambient temperature and pressure. The Fe-(mu-O)-Zn dual-atom sites yield an acetic acid productivity of 3006 mu mol center dot gcat-1 center dot h-1 with 86.8% selectivity (total C2+ products selectivity of 93.0%) for at least 20 hours at 25 oC and atmospheric pressure. The mutual electronic modulation between Fe and Zn shifts the d-band center of Fe 3d in Fe-(mu-O)-Zn dual-atom sites upwards, which promotes the formation and stabilization of highly reactive Fe=O species through O2 photodissociation and thereby enhances the C-H bond activation of CH4. The Fe-(mu-O)-Zn dual-atom reaction sites (spatial distance of 2.7 & Aring;) boost the C-C coupling of key CH3 and HCHO intermediate species, which steadily produce acetic acid and other C2+ oxygenates. This work would broaden the avenue towards the sustainable conversion of methane to value-added C2+ products under ambient temperature and pressure.