Direct Synthesis of Ethanol from Dimethyl Ether and Syngas over Combined H-Mordenite and Cu/ZnO Catalysts

被引:146
作者
Li, Xingang [1 ,2 ]
San, Xiaoguang [4 ]
Zhang, Yi [3 ]
Ichii, Takashi [4 ]
Meng, Ming [1 ,2 ]
Tan, Yisheng [5 ]
Tsubaki, Noritatsu [4 ]
机构
[1] Tianjin Univ, Sch Chem Engn, Tianjin Key Lab Appl Catalysis Sci & Technol, Tianjin 300072, Peoples R China
[2] Tianjin Univ, Inst Technol, Tianjin 300072, Peoples R China
[3] Beijing Univ Chem Technol, Res Ctr, Minist Educ High Grav Engn & Technol, Beijing 100029M, Peoples R China
[4] Toyama Univ, Sch Engn, Dept Appl Chem, Toyama 9308555, Japan
[5] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China
基金
中国国家自然科学基金;
关键词
alcohols; carbonylation; ethers; heterogeneous; catalysis; hydrogenation; TEMPERATURE METHANOL SYNTHESIS; CARBON BOND FORMATION; ACIDIC ZEOLITES; HIGHER ALCOHOLS; SYNTHESIS GAS; SELECTIVE CARBONYLATION; METHYL ACETATE; ETHYL-ACETATE; COPPER; PHASE;
D O I
10.1002/cssc.201000109
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Ethanol was directly synthesized from dimethyl ether (DME) and syngas with the combined H-Mordenite and Cu/ZnO catalysts that were separately loaded in a dual-catalyst bed reactor Methyl acetate (MA) was formed by DME carbonylation over the H Mordenite catalyst Thereafter ethanol and methanol were produced by MA hydrogenation over the Cu/ZnO catalyst With the reactant gas containing 1 0% DME the optimized temperature for the reaction was at 493 K to reach 100% conversion In the products the yield of methanol and ethanol could reach 463% and 422%, respectively with a small amount of MA ethyl acetate and CO(2) This process is environmentally friendly as the main byproduct methanol can be recycled to DME by a dehydration reaction In contrast for the physically mixed catalysts, the low conversion of DME and high selectivity of methanol were observed
引用
收藏
页码:1192 / 1199
页数:8
相关论文
共 45 条
[1]   CATALYTIC HYDROGENOLYSIS OF ESTERS - A COMPARATIVE-STUDY OF THE REACTIONS OF SIMPLE FORMATES AND ACETATES OVER COPPER ON SILICA [J].
AGARWAL, AK ;
CANT, NW ;
WAINWRIGHT, MS ;
TRIMM, DL .
JOURNAL OF MOLECULAR CATALYSIS, 1987, 43 (01) :79-92
[2]  
ARVELA PM, 2007, ENERG FUEL, V21, P30
[3]   Specificity of sites within eight-membered ring zeolite channels for carbonylation of methyls to acetyls [J].
Bhan, Aditya ;
Allian, Ayman D. ;
Sunley, Glenn J. ;
Law, David J. ;
Iglesia, Enrique .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2007, 129 (16) :4919-4924
[4]  
Blasco T., 2007, ANGEW CHEM-GER EDIT, V119, P4012
[5]   Carbonylation of methanol on metal-acid zeolites:: Evidence for a mechanism involving a multisite active center [J].
Blasco, Teresa ;
Boronat, Mercedes ;
Concepcion, Patricia ;
Corma, Avelino ;
Law, David ;
Vidal-Moya, Jose Alejandro .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2007, 46 (21) :3938-3941
[6]   Enzyme-like Specificity in Zeolites: A Unique Site Position in Mordenite for Selective Carbonylation of Methanol and Dimethyl Ether with CO [J].
Boronat, Mercedes ;
Martinez-Sanchez, Cristina ;
Law, David ;
Corma, Avelino .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (48) :16316-16323
[7]  
BRADLEY MW, 1983, Patent No. 8303409
[8]   INVESTIGATION OF THE SYNTHESIS OF OXYGENATES FROM CARBON-MONOXIDE HYDROGEN MIXTURES ON SUPPORTED RHODIUM CATALYSTS [J].
BURCH, R ;
PETCH, MI .
APPLIED CATALYSIS A-GENERAL, 1992, 88 (01) :39-60
[9]  
CALVERLEY EM, 1992, STUD SURF SCI CATAL, V73, P111
[10]   Selective carbonylation of dimethyl ether to methyl acetate catalyzed by acidic zeolites [J].
Cheung, P ;
Bhan, A ;
Sunley, GJ ;
Iglesia, E .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2006, 45 (10) :1617-1620