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

被引:15
作者
Zhang, Hailong [1 ,2 ]
Han, Peijie [1 ]
Wu, Danfeng [1 ]
Du, Congcong [1 ]
Zhao, Jiafei [1 ]
Zhang, Kelvin H. L. [1 ]
Lin, Jingdong [1 ]
Wan, Shaolong [1 ]
Huang, Jianyu [3 ]
Wang, Shuai [1 ]
Xiong, Haifeng [1 ]
Wang, Yong [4 ]
机构
[1] Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces, 422 South Siming Rd, Xiamen 361005, Peoples R China
[2] Sichuan Univ, Coll Carbon Neutral Future Technol, Chengdu 610064, Peoples R China
[3] Yanshan Univ, Clean Nano Energy Ctr, State Key Lab Metastable Mat Sci & Technol, Qinhuangdao 066004, Peoples R China
[4] Washington State Univ, Voiland Sch Chem Engn & Bioengn, Pullman, WA 99164 USA
基金
中国国家自然科学基金;
关键词
INITIO MOLECULAR-DYNAMICS; TOTAL-ENERGY CALCULATIONS; ACTIVE-SITES; DIRECT CONVERSION; CRYSTAL-STRUCTURE; CU/SSZ-13; INSIGHTS; CATALYST; TRANSITION; CU-SSZ-13;
D O I
10.1038/s41467-023-43508-4
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
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 degrees 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.
引用
收藏
页数:10
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