Zhang Hailong, Han Peijie, Wu Danfeng, Du Congcong, Zhao Jiafei, Zhang Kelvin H L, Lin Jingdong, Wan Shaolong, Huang Jianyu, Wang Shuai, Xiong Haifeng, Wang Yong
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, 422 South Siming Road, Xiamen, 361005, China.
College of Carbon Neutrality Future Technology, Sichuan University, Chengdu, 610064, China.
Nat Commun. 2023 Nov 24;14(1):7705. doi: 10.1038/s41467-023-43508-4.
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.
由于甲烷中C-H键的高解离能和甲醇的高脱附能，甲烷直接氧化制甲醇（MTM）在多相催化中仍然是一项重大挑战。在这项工作中，我们展示了选择性MTM的一项突破，即在400°C的连续甲烷-蒸汽反应中，实现了2678 mmol molCu-1 h-1的高甲醇时空产率，选择性达93%。这种优异的性能归因于SSZ-13沸石中六元环（6MR）空隙的限域效应，这些空隙容纳了孤立的Cu-OH单中心。我们的结果为深入理解铜沸石在甲烷-蒸汽连续转化为甲醇过程中的作用提供了依据，并为进一步改进铺平了道路。
