Self-metathesis of 1-butene to ethene and hexene over molybdenum-based heterogeneous catalysts

被引:3
作者
Guo, Ce [1 ,2 ]
Li, Xiujie [1 ]
Zhu, Xiangxue [1 ]
Chu, Weifeng [1 ,2 ]
Liu, Shenglin [1 ]
Wang, Yuzhong [1 ]
Zeng, Peng [3 ]
Guo, Shujing [4 ]
Xu, Longya [1 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Liaoning, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] China Huanqiu Contracting & Engn Corp, Fushun 113006, Liaoning, Peoples R China
[4] Shaanxi Yanchang Petr Grp Co Ltd, Yanan 716000, Shaanxi, Peoples R China
来源
CHINESE JOURNAL OF CATALYSIS | 2018年 / 39卷 / 01期
基金
中国国家自然科学基金;
关键词
1-Butene; Self-metathesis; Molybdenum; Ethene; Hexene; OLEFIN METATHESIS; CROSS-METATHESIS; OXIDE CATALYSTS; SILICA-ALUMINA; PROPENE; PROPYLENE; MO; CONVERSION; MOLYBDATE; ETHYLENE;
D O I
10.1016/S1872-2067(17)62918-8
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
A novel route involving self-metathesis of 1-butene under mild conditions that gave high yields of ethene and hexene was proposed. The results of thermodynamic analysis revealed that the Gibbs energy of the target Metathesis I reaction (1-butene > ethene + 3-hexene) was much higher than that of the main side Metathesis II (1-butene + 2-butene -> propene + 2-pentene). Suppression of 1-butene double-bond isomerization was the key step to increase the selectivity for the target olefin in the reaction network. The relationship between the catalytic performance and support nature was investigated in detail. On basis of H-2-TPR, UV-Vis spectra and HRTEM results, an alumina (Al2O3) support with large surface area was beneficial for the dispersion of molybdenum (Mo) species. Both suitable acidity and sufficient Mo dispersion were important to selectively promote the self-metathesis reaction of 1-butene. On the optimal 6Mo/Al2O3 catalyst, 1-butene conversion reached 47% and ethene selectivity was as high as 42% on the premise of good catalytic stability (80 degrees C, 1.0 MPa, 3 h(-1)). (C) 2018, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
引用
收藏
页码:37 / 46
页数:10
相关论文
共 33 条
[1]   Mo/γ-Al2O3 catalysts for the oxidative dehydrogenation of propane.: Effect of Mo loading [J].
Abello, MC ;
Gomez, MF ;
Ferretti, O .
APPLIED CATALYSIS A-GENERAL, 2001, 207 (1-2) :421-431
[2]   Recent developments in olefin cross-metathesis [J].
Connon, SJ ;
Blechert, S .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2003, 42 (17) :1900-1923
[3]   One-Pot Aerosol Route to MoO3-SiO2-Al2O3 Catalysts with Ordered Super Microporosity and High Olefin Metathesis Activity [J].
Debecker, Damien P. ;
Stoyanova, Mariana ;
Colbeau-Justin, Frederic ;
Rodemerck, Uwe ;
Boissiere, Cedric ;
Gaigneaux, Eric M. ;
Sanchez, Clement .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2012, 51 (09) :2129-2131
[4]   Opposite effect of Al on the performances of MoO3/SiO2-Al2O3 catalysts in the metathesis and in the partial oxidation of propene [J].
Debecker, Damien P. ;
Hauwaert, Damien ;
Stoyanova, Mariana ;
Barkschat, Axel ;
Rodemerck, Uwe ;
Gaigneaux, Eric M. .
APPLIED CATALYSIS A-GENERAL, 2011, 391 (1-2) :78-85
[5]   Flame-made MoO3/SiO2-Al2O3 metathesis catalysts with highly dispersed and highly active molybdate species [J].
Debecker, Damien P. ;
Schimmoeller, Bjoern ;
Stoyanova, Mariana ;
Poleunis, Claude ;
Bertrand, Patrick ;
Rodemerck, Uwe ;
Gaigneaux, Eric M. .
JOURNAL OF CATALYSIS, 2011, 277 (02) :154-163
[6]   Co2C nanoprisms for syngas conversion to lower olefins with high selectivity [J].
Ding, Yunjie .
CHINESE JOURNAL OF CATALYSIS, 2017, 38 (01) :1-4
[7]  
Gartside R. J., 2004, US Patent, Patent No. [6683019 B2, 6683019B2]
[8]   Properties and metathesis activity of molybdena-alumina, molybdena-silica-alumina and molybdena-silica catalysts - a comparative study [J].
Handzlik, Jaroslaw ;
Ogonowski, Jan ;
Stoch, Jerzy ;
Mikolajczyk, Maciej ;
Michorczyk, Piotr .
APPLIED CATALYSIS A-GENERAL, 2006, 312 (1-2) :213-219
[9]   On the Product Formation in 1-Butene Metathesis over Supported Tungsten Catalysts [J].
Harmse, Liesel ;
van Schalkwyk, Charl ;
van Steen, Eric .
CATALYSIS LETTERS, 2010, 137 (3-4) :123-131
[10]   Metathesis of butene to propene and pentene over WO3/MTS-9 [J].
Hua, Derun ;
Chen, Sheng-Li ;
Yuan, Guimei ;
Wang, Yulong ;
Zhao, Qinfeng ;
Wang, Xuelian ;
Fu, Bo .
MICROPOROUS AND MESOPOROUS MATERIALS, 2011, 143 (2-3) :320-325