Direct observation of DME carbonylation in the different channels of H-MOR zeolite by continuous-flow solid-state NMR spectroscopy

被引:55
作者
He, Ting [1 ]
Ren, Pengju [1 ]
Liu, Xianchun [1 ]
Xu, Shutao [2 ]
Han, Xiuwen [1 ]
Bao, Xinhe [1 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
[2] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Natl Engn Lab Methanol Olefins, Dalian 116023, Peoples R China
关键词
DIMETHYL ETHER CARBONYLATION; ACIDIC ZEOLITES; METHYL ACETATE; SELECTIVE CARBONYLATION; HETEROGENEOUS CATALYSIS; METHANOL; MORDENITE; CONVERSION; SPECIFICITY; MECHANISM;
D O I
10.1039/c5cc07201h
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The dynamic evolution of acetyl intermediates in the two different channels of H-mordenite (H-MOR) zeolite during dimethyl ether (DME) carbonylation is tracked by using in situ solid-state NMR spectroscopy under continuous-flow conditions. Thus, the reaction path via methyl acetate produced over active sites in 8 member ring (MR) channels, followed by diffusion into 12 MR channels, is proposed.
引用
收藏
页码:16868 / 16870
页数:3
相关论文
共 20 条
[1]   Specificity of sites within eight-membered ring zeolite channels for carbonylation of methyls to acetyls [J].
Bhan, Aditya ;
Allian, Ayman D. ;
Sunley, Glenn J. ;
Law, David J. ;
Iglesia, Enrique .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2007, 129 (16) :4919-4924
[2]   Mechanistic differences between methanol and dimethyl ether carbonylation in side pockets and large channels of mordenite [J].
Boronat, Mercedes ;
Martinez, Cristina ;
Corma, Avelino .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2011, 13 (07) :2603-2612
[3]   Enzyme-like Specificity in Zeolites: A Unique Site Position in Mordenite for Selective Carbonylation of Methanol and Dimethyl Ether with CO [J].
Boronat, Mercedes ;
Martinez-Sanchez, Cristina ;
Law, David ;
Corma, Avelino .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (48) :16316-16323
[4]   FORMATION OF SURFACE-BONDED METHOXY GROUPS IN THE SORPTION OF METHANOL AND METHYL-IODIDE ON ZEOLITES STUDIED BY C-13 MAS NMR-SPECTROSCOPY [J].
BOSACEK, V .
JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (41) :10732-10737
[5]   Selective carbonylation of dimethyl ether to methyl acetate catalyzed by acidic zeolites [J].
Cheung, P ;
Bhan, A ;
Sunley, GJ ;
Iglesia, E .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2006, 45 (10) :1617-1620
[6]   Site requirements and elementary steps in dimethyl ether carbonylation catalyzed by acidic zeolites [J].
Cheung, Patricia ;
Bhan, Aditya ;
Sunley, Glenn J. ;
Law, David J. ;
Iglesia, Enrique .
JOURNAL OF CATALYSIS, 2007, 245 (01) :110-123
[7]   A NEW MAS NMR PROBE FOR IN-SITU INVESTIGATIONS OF HYDROCARBON CONVERSION ON SOLID CATALYSTS UNDER CONTINUOUS-FLOW CONDITIONS [J].
HUNGER, M ;
HORVATH, T .
JOURNAL OF THE CHEMICAL SOCIETY-CHEMICAL COMMUNICATIONS, 1995, (14) :1423-1424
[9]   CONVERSION OF METHANOL TO GASOLINE - A NEW MECHANISM FOR FORMATION OF THE 1ST CARBON CARBON BOND [J].
JACKSON, JE ;
BERTSCH, FM .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1990, 112 (25) :9085-9092
[10]   On the reactivity of surface methoxy species in acidic zeolites [J].
Jiang, Yijiao ;
Hunger, Michael ;
Wang, Wei .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2006, 128 (35) :11679-11692