Confined Cu-OH single sites in SSZ-13 zeolite for the direct oxidation of methane to methanol

Hailong Zhang; Peijie Han; Danfeng Wu; Congcong Du; Jiafei Zhao; Kelvin H L Zhang; Jingdong Lin; Shaolong Wan; Jianyu Huang; Shuai Wang; Haifeng Xiong; Yong Wang

doi:10.1038/s41467-023-43508-4

Confined Cu-OH single sites in SSZ-13 zeolite for the direct oxidation of methane to methanol

Nat Commun. 2023 Nov 24;14(1):7705. doi: 10.1038/s41467-023-43508-4.

Authors

Hailong Zhang^{1

2}, Peijie Han¹, Danfeng Wu¹, Congcong Du¹, Jiafei Zhao¹, Kelvin H L Zhang¹, Jingdong Lin¹, Shaolong Wan¹, Jianyu Huang³, Shuai Wang⁴, Haifeng Xiong⁵, Yong Wang⁶

Affiliations

¹ State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, 422 South Siming Road, Xiamen, 361005, China.
² College of Carbon Neutrality Future Technology, Sichuan University, Chengdu, 610064, China.
³ Clean Nano Energy Center, State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao, 066004, China.
⁴ State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, 422 South Siming Road, Xiamen, 361005, China. [email protected].
⁵ State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, 422 South Siming Road, Xiamen, 361005, China. [email protected].
⁶ Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, WA, 99164, USA. [email protected].

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.

Grants and funding

22072118/National Natural Science Foundation of China (National Science Foundation of China)