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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.
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页数:10
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