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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.
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1 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)
2 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)
3 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)
4 Washington State University, Voiland School of Chemical Engineering and Bioengineering, Pullman, USA (GRID:grid.30064.31) (ISNI:0000 0001 2157 6568)