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

Zhang, Hailong; Han, Peijie; Wu, Danfeng; Du, Congcong; Zhao, Jiafei; Zhang, Kelvin H L; Lin, Jingdong; Wan, Shaolong et al. · Nat Commun · 2023

basic_science · Level V

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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.