Dehydrogenation of methylcyclohexane to toluene over partially reduced Mo-SiO2 catalysts

被引:57
作者
Boufaden, N. [1 ]
Akkari, R. [1 ]
Pawelec, B. [2 ]
Fierro, J. L. G. [2 ]
Zina, M. Said [1 ]
Ghorbel, A. [1 ]
机构
[1] Univ Tunis El Manar, Fac Sci Tunis, Dept Chim, Lab Chim Mat & Catalyse, Tunis 2092, Tunisia
[2] CSIC, Inst Catalisis & Petroleoquim, E-28049 Madrid, Spain
关键词
Methylcyclohexane dehydrogenation; Silica-supported Mo catalysts; Catalyst characterization; HYDROGEN STORAGE; AB-INITIO; RAMAN; MCH; NI; CONDENSATION; SPECTROSCOPY; CYCLOHEXANE; ADSORPTION; MO;
D O I
10.1016/j.apcata.2015.05.026
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
Dehydrogenation of methylcyclohexane (MCH) has been carried out on a variety of partially reduced Mo(x) SiO2 (x: Mo/Si molar ratio x 100) catalysts differing by the molybdenum loading and which were prepared by sol-gel method. The objective was to maximize hydrogen production by monitoring the selectivity toward toluene formation. The MCH dehydrogenation was carried out in a down-flow reactor at 673 K and 2.2 MPa of total hydrogen pressure. The effect of Mo molar loading on the structure of the catalysts was studied by N-2 physisorption, TPR, XRD, UV vis DRS, NH3-TPD, XPS and TEM techniques. From the activity tests, it was concluded that Mo I 0 SiO2 catalyst, with Mo molar ratio of 10, exhibited the highest activity and the largest yield of toluene thanks to the existence of a good compromise between reduced Mo species and bulk MoO3. An increase of the molybdenum loading from 10 to 15 (molar ratio) led to: (i), the formation of non-active MoO3 phase; (ii), a low stable molybdenum species during on-stream operation; and (iii), a large coke formation due to an increase of the catalyst acidity. (C) 2015 Elsevier B.V. All rights reserved.
引用
收藏
页码:329 / 339
页数:11
相关论文
共 46 条
[1]   Hydrogen storage in liquid organic hydride: Selectivity of MCH dehydrogenation over monometallic and bimetallic Pt catalysts [J].
Alhumaidan, Faisal ;
Tsakiris, Dimos ;
Cresswell, David ;
Garforth, Arthur .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2013, 38 (32) :14010-14026
[2]   Kinetic Model of the Dehydrogenation of Methylcyclohexane over Monometallic and Bimetallic Pt Catalysts [J].
Alhumaidan, Faisal ;
Cresswell, David ;
Garforth, Arthur .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2011, 50 (05) :2509-2522
[3]   Sol-Gel Synthesis of MoO3/SiO2 Composite for Catalytic Application in Condensation of Anisole with Paraformaldehyde [J].
Amrute, Amol P. ;
Bordoloi, Ankur ;
Lucas, Nishita ;
Palraj, K. ;
Halligudi, S. B. .
CATALYSIS LETTERS, 2008, 126 (3-4) :286-292
[4]   Lattice vibrational modes in synthetic tremolite-Sr-tremolite and tremolite-richterite solid solutions [J].
Andrut, M ;
Gottschalk, M ;
Melzer, S ;
Najorka, J .
PHYSICS AND CHEMISTRY OF MINERALS, 2000, 27 (05) :301-309
[5]  
Aoudjit F., 2008, THESIS U MHAMMAD BOU
[6]   Investigation of a molybdenum-containing silica catalyst synthesized by the sol-gel process in heterogeneous catalytic esterification reactions using methanol and ethanol [J].
Bail, Alesandro ;
dos Santos, Vannia Cristina ;
de Freitas, Marianne Roque ;
Ramos, Luiz Pereira ;
Schreiner, Wido Herwig ;
Ricci, Gustavo Pimenta ;
Ciuffi, Katia Jorge ;
Nakagaki, Shirley .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2013, 130 :314-324
[7]   Catalytic reactions of methylcyclohexane (MCH) on partially reduced MoO3 [J].
Belatel, H ;
Al-Kandari, H ;
Al-Khorafi, F ;
Katrib, A ;
Garin, F .
APPLIED CATALYSIS A-GENERAL, 2004, 275 (1-2) :141-147
[8]   Dehydrogenation of cyclohexane over Ni based catalysts supported on activated carbon using spray-pulsed reactor and enhancement in activity by addition of a small amount of Pt [J].
Biniwale, RB ;
Kariya, N ;
Ichikawa, M .
CATALYSIS LETTERS, 2005, 105 (1-2) :83-87
[9]   Transesterification of diethyl oxalate with phenol using MoO3/SiO2 catalyst [J].
Biradar, AV ;
Umbarkar, SB ;
Dongare, MK .
APPLIED CATALYSIS A-GENERAL, 2005, 285 (1-2) :190-195
[10]   Synthesis of tinidazole by condensation-oxidation sequence using MoO3/SiO2 bifunctional catalyst [J].
Chandorkar, J. G. ;
Umbarkar, S. B. ;
Rode, C. V. ;
Kotwal, V. B. ;
Dongare, M. K. .
CATALYSIS COMMUNICATIONS, 2007, 8 (10) :1550-1555