Influence of crystal size on the catalytic performance of H-ZSM-5 and Zn/H-ZSM-5 in the conversion of methanol to aromatics

被引:163
作者
Niu, Xianjun [1 ,2 ,3 ]
Gao, Jie [1 ,3 ]
Wang, Kai [1 ,3 ]
Miao, Qing [1 ,3 ]
Dong, Mei [1 ]
Wang, Guofu [1 ]
Fan, Weibin [1 ]
Qin, Zhangfeng [1 ]
Wang, Jianguo [1 ]
机构
[1] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, POB 165, Taiyuan 030001, Shanxi, Peoples R China
[2] Jinzhong Univ, Coll Chem & Chem Engn, Jinzhong 030619, Shanxi, Peoples R China
[3] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
基金
中国国家自然科学基金;
关键词
Methanol to aromatics; H-ZSM-5; Zn/H-ZSM-5; Crystal size; Zinc species; EXCHANGED ZSM-5 ZEOLITES; CONFINED SPACE SYNTHESIS; TO-OLEFIN REACTIONS; ACID SITES; SELECTIVE CONVERSION; PROPANE AROMATIZATION; HZSM-5; ZEOLITES; LOWER ALKANES; HYDROCARBONS; ZN;
D O I
10.1016/j.fuproc.2016.12.006
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
H-ZSM-5 zeolites with a uniform crystal size from 0.25 to 2 pm were obtained by adding colloidal silicalite-1 seed in the synthesis gel; with H-ZSM-5 as the support, Zn/H-ZSM-5 was prepared by incipient wet impregnation. The influence of crystal size on the state of Zn species and its relation to the catalytic performance of Zn/H-ZSM-5 in the conversion of methanol to aromatics (MTA) was then investigated. The results illustrated that the state of Zn species and catalytic performance of Zn/H-ZSM-5 are closely related to the crystal size, though the crystal size has little influence on the overall acidity. There exist mainly two types of zinc species, viz., ZnO and ZnOH+; Zn/H-ZSM-5 with smaller crystal size is provided with more ZnOH+ species. The selectivity to aromatics and catalyst stability can be improved greatly by using small crystal Zn/H-ZSM-5. A good linear correlation is observed between the amount of ZnOH+ species and the selectivity to aromatics, suggesting that ZnOH+ species plays an important role in enhancing the dehydrogenation of alkanes and aromatization bf alkenes to aromatics. As a result, small crystal Zn/H-ZSM-5 with large portion of ZnOH+ species exhibits high selectivity to aromatics and long lifetime in MTA. (C) 2016 Elsevier B.V. All rights reserved.
引用
收藏
页码:99 / 107
页数:9
相关论文
共 61 条
[1]   Structure-deactivation relationship for ZSM-5 catalysts governed by framework defects [J].
Barbera, Katia ;
Bonino, Francesca ;
Bordiga, Silvia ;
Janssens, Ton V. W. ;
Beato, Pablo .
JOURNAL OF CATALYSIS, 2011, 280 (02) :196-205
[2]   Zinc promoted H-ZSM-5 catalysts for conversion of propane to aromatics .2. Nature of the active sites and their activation [J].
Berndt, H ;
Lietz, G ;
Volter, J .
APPLIED CATALYSIS A-GENERAL, 1996, 146 (02) :365-379
[3]   Structure and density of active Zn species in Zn/H-ZSM5 propane aromatization catalysts [J].
Biscardi, JA ;
Meitzner, GD ;
Iglesia, E .
JOURNAL OF CATALYSIS, 1998, 179 (01) :192-202
[4]   Methanol to gasoline over zeolite H-ZSM-5: Improved catalyst performance by treatment with NaOH [J].
Bjorgen, Morten ;
Joensen, Finn ;
Holm, Martin Spangsberg ;
Olsbye, Unni ;
Lillerud, Karl-Petter ;
Svelle, Stian .
APPLIED CATALYSIS A-GENERAL, 2008, 345 (01) :43-50
[5]   CONVERSION OF METHANOL AND OTHER O-COMPOUNDS TO HYDROCARBONS OVER ZEOLITE CATALYSTS [J].
CHANG, CD ;
SILVESTRI, AJ .
JOURNAL OF CATALYSIS, 1977, 47 (02) :249-259
[6]  
Chen J, 2001, CHINESE J CATAL+, V22, P229
[7]   ZnO clusters encapsulated inside micropores of zeolites studied by UV Raman and laser-induced luminescence spectroscopies [J].
Chen, J ;
Feng, ZC ;
Ying, PL ;
Li, C .
JOURNAL OF PHYSICAL CHEMISTRY B, 2004, 108 (34) :12669-12676
[8]  
Chen J., 2000, CHINESE J CATAL, V21, P125
[9]   PARA-DIRECTED AROMATIC REACTIONS OVER SHAPE-SELECTIVE MOLECULAR-SIEVE ZEOLITE CATALYSTS [J].
CHEN, NY ;
KAEDING, WW ;
DWYER, FG .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1979, 101 (22) :6783-6784
[10]   METHANOL-TO-AROMATICS CONVERSION OVER H-GALLOSILICATE (MFI) - INFLUENCE OF SI/GA RATIO, DEGREE OF H+ EXCHANGE, PRETREATMENT CONDITIONS, AND POISONING OF STRONG ACID SITES [J].
CHOUDHARY, VR ;
KINAGE, AK .
ZEOLITES, 1995, 15 (08) :732-738