Abstract

The direct oxidation of methane to methanol (MTM) remains a significant challenge in heterogeneous catalysis due to the high dissociation energy of the C-H bond in methane and the high desorption energy of methanol. In this work, we demonstrate a breakthrough in selective MTM by achieving a high methanol space-time yield of 2678 mmol molCu−1 h−1 with 93% selectivity in a continuous methane-steam reaction at 400 °C. The superior performance is attributed to the confinement effect of 6-membered ring (6MR) voids in SSZ-13 zeolite, which host isolated Cu-OH single sites. Our results provide a deeper understanding of the role of Cu-zeolites in continuous methane-steam to methanol conversion and pave the way for further improvement.

High yields of methanol are difficult to achieve with direct oxidation of methane to methanol. Here the authors report a high methanol space-time yield which is attributed to the confinement effect of 6-membered ring voids and the isolated Cu-OH single sites in SSZ−13 zeolite.

Details

Title
Confined Cu-OH single sites in SSZ-13 zeolite for the direct oxidation of methane to methanol
Author
Zhang, Hailong 1 ; Han, Peijie 2 ; Wu, Danfeng 2 ; Du, Congcong 2   VIAFID ORCID Logo  ; Zhao, Jiafei 2 ; Zhang, Kelvin H. L. 2   VIAFID ORCID Logo  ; Lin, Jingdong 2   VIAFID ORCID Logo  ; Wan, Shaolong 2 ; Huang, Jianyu 3 ; Wang, Shuai 2   VIAFID ORCID Logo  ; Xiong, Haifeng 2   VIAFID ORCID Logo  ; Wang, Yong 4   VIAFID ORCID Logo 

 Xiamen University, State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen, China (GRID:grid.12955.3a) (ISNI:0000 0001 2264 7233); Sichuan University, College of Carbon Neutrality Future Technology, Chengdu, China (GRID:grid.13291.38) (ISNI:0000 0001 0807 1581) 
 Xiamen University, State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen, China (GRID:grid.12955.3a) (ISNI:0000 0001 2264 7233) 
 Yanshan University, Clean Nano Energy Center, State Key Laboratory of Metastable Materials Science and Technology, Qinhuangdao, China (GRID:grid.413012.5) (ISNI:0000 0000 8954 0417) 
 Washington State University, Voiland School of Chemical Engineering and Bioengineering, Pullman, USA (GRID:grid.30064.31) (ISNI:0000 0001 2157 6568) 
Pages
7705
Publication year
2023
Publication date
2023
Publisher
Nature Publishing Group
e-ISSN
20411723
Source type
Scholarly Journal
Language of publication
English
ProQuest document ID
2893290082
Copyright
© The Author(s) 2023. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.