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

作者：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 · 发表于：Nature Communications · 年份：2023 · DOI：10.1038/s41467-023-43508-4 · 被引用次数：62 · 研究领域：Catalytic Processes in Materials Science、Catalysis and Oxidation Reactions、Mesoporous Materials and Catalysis

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.