Silver and Copper Dual Single Atoms Boosting Direct Oxidation of Methane to Methanol via Synergistic Catalysis

Author:

Yu Baiyang12,Cheng Lu34,Dai Sheng3,Jiang Yongjun3,Yang Bing5,Li Hong5,Zhao Yi12,Xu Jing6,Zhang Ying12,Pan Chengsi12,Cao Xiao‐Ming34,Zhu Yongfa7,Lou Yang12ORCID

Affiliation:

1. Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering Jiangnan University Wuxi Jiangsu 214122 China

2. International Joint Research Center for Photoresponsive Molecules and Materials Jiangnan University Wuxi Jiangsu 214122 China

3. Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering East China University of Science and Technology Shanghai 200237 China

4. Centre for Computational Chemistry and Research Institute of Industrial Catalysis East China University of Science and Technology Shanghai 200237 China

5. Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics 457 Zhongshan Road Dalian 116023 China

6. School of Food Science and Technology Jiangnan University Wuxi Jiangsu 214122 China

7. Department of Chemistry Tsinghua University Beijing 100084 China

Abstract

AbstractRationally constructing atom‐precise active sites is highly important to promote their catalytic performance but still challenging. Herein, this work designs and constructs ZSM‐5 supported Cu and Ag dual single atoms as a proof‐of‐concept catalyst (Ag1−Cu1/ZSM‐5 hetero‐SAC (single‐atom catalyst)) to boost direct oxidation of methane (DOM) by H2O2. The Ag1−Cu1/ZSM‐5 hetero‐SAC synthesized via a modified co‐adsorption strategy yields a methanol productivity of 20,115 µmol gcat−1 with 81% selectivity at 70 °C within 30 min, which surpasses most of the state‐of‐the‐art noble metal catalysts. The characterization results prove that the synergistic interaction between silver and copper facilitates the formation of highly reactive surface hydroxyl species to activate the C−H bond as well as the activity, selectivity, and stability of DOM compared with SACs, which is the key to the enhanced catalytic performance. This work believes the atomic‐level design strategy on dual‐single‐atom active sites should pave the way to designing advanced catalysts for methane conversion.

Funder

National Natural Science Foundation of China

Natural Science Foundation of Jiangsu Province

Dalian University of Technology

Fundamental Research Funds for the Central Universities

Publisher

Wiley

Subject

General Physics and Astronomy,General Engineering,Biochemistry, Genetics and Molecular Biology (miscellaneous),General Materials Science,General Chemical Engineering,Medicine (miscellaneous)

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