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
[21]  
Hagen A, 1995, STUD SURF SCI CATAL, V94, P195
[22]   Phosphate modified ZSM-5 for the shape-selective synthesis of para-diethylbenzene: Role of crystal size and acidity [J].
Hodala, Janardhan L. ;
Halgeri, Anand B. ;
Shanbhag, Ganapati V. .
APPLIED CATALYSIS A-GENERAL, 2014, 484 :8-16
[23]   SELECTIVE CONVERSION OF METHANOL INTO AROMATIC-HYDROCARBONS OVER SILVER-EXCHANGED ZSM-5 ZEOLITES [J].
INOUE, Y ;
NAKASHIRO, K ;
ONO, Y .
MICROPOROUS MATERIALS, 1995, 4 (05) :379-383
[24]   SELECTIVE CONVERSION OF PROPANE INTO AROMATICS ON PLATINUM ION-EXCHANGED GALLIUM-SILICATE BIFUNCTIONAL CATALYSTS [J].
INUI, T ;
MAKINO, Y ;
OKAZUMI, F ;
MIYAMOTO, A .
JOURNAL OF THE CHEMICAL SOCIETY-CHEMICAL COMMUNICATIONS, 1986, (07) :571-573
[25]   Zeolites by confined space synthesis -: characterization of the acid sites in nanosized ZSM-5 by ammonia desorption and 27Al/29Si-MAS NMR spectroscopy [J].
Jacobsen, CJH ;
Madsen, C ;
Janssens, TVW ;
Jakobsen, HJ ;
Skibsted, J .
MICROPOROUS AND MESOPOROUS MATERIALS, 2000, 39 (1-2) :393-401
[26]   SAPO-34 and ZSM-5 nanocrystals' size effects on their catalysis of methanol-to-olefin reactions [J].
Jang, Hoi-Gu ;
Min, Hyung-Ki ;
Lee, Jun Kyu ;
Hong, Suk Bong ;
Seo, Gon .
APPLIED CATALYSIS A-GENERAL, 2012, 437 :120-130
[27]   Methanol aromatization over Ga-doped desilicated HZSM-5 [J].
Lai, Po-Chen ;
Chen, Chao-Huang ;
Hsu, His-Yen ;
Lee, Chiou-Hwang ;
Lin, Yu-Chuan .
RSC ADVANCES, 2016, 6 (71) :67361-67371
[28]   THE ROLE OF GALLIUM IN THE CATALYTIC ACTIVITY OF ZEOLITE [SI,GA]-ZSM-5 FOR METHANOL CONVERSION [J].
LALIK, E ;
LIU, XS ;
KLINOWSKI, J .
JOURNAL OF PHYSICAL CHEMISTRY, 1992, 96 (02) :805-809
[29]   The nucleation period for TPA-silicalite-1 crystallization determined by a two-stage varying-temperature synthesis [J].
Li, Q ;
Creaser, D ;
Sterte, J .
MICROPOROUS AND MESOPOROUS MATERIALS, 1999, 31 (1-2) :141-150
[30]   The acidity and catalytic behavior of Mg-ZSM-5 prepared via a solid-state reaction [J].
Li, YG ;
Xie, WH ;
Yong, S .
APPLIED CATALYSIS A-GENERAL, 1997, 150 (02) :231-242