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

来源：

CATALYSTS | 2023年 / 13卷 / 07期

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; MORDENITE; ZEOLITES; CONVERSION; 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

页数：11

共 41 条

[11] Methane Activation by a Mononuclear Copper Active Site in the Zeolite Mordenite: Effect of Metal Nuclearity on Reactivity [J].