Enhancing the Activity of Cu-MOR by Water for Oxidation of Methane to Methanol

被引:3
|
作者
Guan, Xi'an [1 ,2 ,3 ]
Wang, Yehong [1 ]
Liu, Xiumei [1 ]
Du, Hong [1 ]
Guo, Xinwen [2 ]
Zhang, Zongchao [1 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
[2] Dalian Univ Technol, Sch Chem Engn, Penn State Univ Dalian Univ Technol PSU DUT Joint, State Key Lab Fine Chem, Dalian 116023, Peoples R China
[3] Univ Chinese Acad Sci, Sch Chem Engn, Beijing 100039, Peoples R China
基金
中国国家自然科学基金;
关键词
Cu-MOR; water; methane to methanol; ZCu(II)OH; XPS; SELECTIVE ANAEROBIC OXIDATION; CONVERSION; MORDENITE; ZEOLITES; SPECTROSCOPY; STABILITY; CATALYSTS; CU-ZSM-5; SITES; FILMS;
D O I
10.3390/catal13071066
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
As clean energy, methane has huge reserves and great development potential in the future. Copper zeolites are efficient in the oxidation of methane to methanol. Water has been confirmed as a source of oxygen to regenerate the copper-zeolite active sites to enable selective anaerobic oxidation of methane to methanol. In this work, we report that the methanol yield increased from 36 & mu;mol/g (Cu-MOR1) to 92 & mu;mol/g (Cu-MOR1-water) as a result of water enhancing the activity of copper ion-exchange mordenite catalyst. We show for the first time that water could convert inactive copper species into active copper species during catalyst activation. A combination of the XPS, FTIR, and NMR results indicates that water dissociates and then converts ZCu(II)Z into ZCu(II)(OH) (where Z indicates framework O (O-fw) bonded to one isolated Al in a framework T-site, i.e., 1Al) and simultaneously produces a Bronsted acid site during catalyst activation. This finding can be used to tune the state of copper species and design highly active copper-zeolite catalysts for methane oxidation to methanol.
引用
收藏
页数:11
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