The synergic effect between Mo species and acid sites in Mo/HMCM-22 catalysts for methane aromatization

被引:37
作者
Ma, D [1 ]
Zhu, QJ [1 ]
Wu, ZL [1 ]
Zhou, DH [1 ]
Shu, YY [1 ]
Xin, Q [1 ]
Xu, YD [1 ]
Bao, XH [1 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
关键词
D O I
10.1039/b502794b
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
The acid properties of Mo/HMCM-22 catalyst, which is the precursor form of the working catalyst for methane aromatization reaction, and the synergic effect between Mo species and acid sites were studied and characterized by various characterization techniques. It is concluded that Bronsted and Lewis acidities of HMCM-22 are modified due to the introduction of molybdenum. We suggest a monomer of Mo species is formed by the exchange of Mo species with the Bronsted acid sites. On the other hand, coordinate unsaturated sites (CUS) are suggested to be responsible for the formation of newly detected Lewis acid sites. Computer modelling is established and coupling with experimental results, it is then speculated that the effective activation of methane is properly accomplished on Mo species accommodated in the 12 MR supercages of MCM-22 zeolite whereas the Bronsted acid sites in the same channel system play a key role for the formation of benzene. A much more pronounced volcano-typed reactivity curve of the Mo/HMCM-22 catalysts, as compared with that of the Mo/HZSM-5, with respect to Mo loading is found and this can be well understood due to the unique channel structure of MCM-22 zeolite and synergic effect between Mo species and acid sites.
引用
收藏
页码:3102 / 3109
页数:8
相关论文
共 51 条
[11]   MCM-22 - A MOLECULAR-SIEVE WITH 2 INDEPENDENT MULTIDIMENSIONAL CHANNEL SYSTEMS [J].
LEONOWICZ, ME ;
LAWTON, JA ;
LAWTON, SL ;
RUBIN, MK .
SCIENCE, 1994, 264 (5167) :1910-1913
[12]   Raman and X-ray absorption studies of Mo species in Mo/H-ZSM5 catalysts for non-oxidative CH4 reactions [J].
Li, W ;
Meitzner, GD ;
Borry, RW ;
Iglesia, E .
JOURNAL OF CATALYSIS, 2000, 191 (02) :373-383
[13]   Bifunctional catalysis of Mo/HZSM-5 in the dehydroaromatization of methane to benzene and naphthalene XAFS/TG/DTA/MASS/FTIR characterization and supporting effects [J].
Liu, ST ;
Wang, L ;
Ohnishi, R ;
Ichikawa, M .
JOURNAL OF CATALYSIS, 1999, 181 (02) :175-188
[14]  
Liu W, 1999, J CATAL, V185, P386, DOI 10.1006/jcat.1999.2515
[15]   Methane dehydrogenation and aromatization in the absence of oxygen on Mo/HZSM-5: A study on the interaction between Mo species and HZSM-5 by using Al-27 and Si-29 MAS NMR [J].
Liu, W ;
Xu, Y ;
Wong, ST ;
Wang, L ;
Qiu, J ;
Yang, N .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1997, 120 (1-3) :257-265
[16]   A high coking-resistance catalyst for methane aromatization [J].
Lu, Y ;
Ma, D ;
Xu, ZS ;
Tian, ZJ ;
Bao, XH ;
Lin, LW .
CHEMICAL COMMUNICATIONS, 2001, (20) :2048-2049
[17]  
Ma D, 2002, CHEM-EUR J, V8, P4557, DOI 10.1002/1521-3765(20021004)8:19<4557::AID-CHEM4557>3.0.CO
[18]  
2-8
[19]   Methane dehydro-aromatization under nonoxidative conditions over Mo/HZSM-5 catalysts: EPR study of the Mo species on/in the HZSM-5 zeolite [J].
Ma, D ;
Shu, YY ;
Bao, XH ;
Xu, YD .
JOURNAL OF CATALYSIS, 2000, 189 (02) :314-325
[20]   On the induction period of methane aromatization over Mo-based catalysts [J].
Ma, D ;
Shu, YY ;
Cheng, MJ ;
Xu, YD ;
Bao, XH .
JOURNAL OF CATALYSIS, 2000, 194 (01) :105-114