Ethanol steam reforming for hydrogen generation over structured catalysts

被引:57
作者
Lopez, Eduardo [1 ,2 ]
Divins, Nuria J. [1 ,3 ]
Anzola, Andres [2 ]
Schbib, Susana [2 ]
Borio, Daniel [2 ]
Llorca, Jordi [1 ,3 ]
机构
[1] Univ Politecn Cataluna, Inst Tecn Energet, E-08028 Barcelona, Spain
[2] Planta Piloto Ingn Quim CONICET UNS, RA-8000 Bahia Blanca, Buenos Aires, Argentina
[3] Univ Politecn Cataluna, Ctr Res Nanoengn, E-08028 Barcelona, Spain
关键词
Hydrogen; Ethanol reforming; Monolith; Structured catalyst; Wall reactor; BIO-ETHANOL; PRODUCE HYDROGEN; FUEL; OXIDATION; NI; CO;
D O I
10.1016/j.ijhydene.2013.01.174
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
The present paper reports on the preparation, characterization and reaction evaluation of structured catalysts toward hydrogen generation via ethanol steam reforming. To these ends, 400 cpsi cordierite monoliths were functionalized with Rh-Pd/CeO2 catalyst. SEM, TEM and XRD showed a uniform and well-covering CeO2 layer where Rh-Pd nanoparticles of less than 0.5 nm were anchored. The functionalized monoliths were successfully tested for synthesis gas production from ethanol steam reforming. Realistic operating conditions were selected, including temperatures between 500 and 950 K, pressures from 1 to 6 bar, undiluted ethanol:water molar ratios 1:4-1:8 (i.e., 2 <= S/C <= 4) and a wide range of feed loads. Appropriate activity and hydrogen selectivity were verified for the catalytic system, with ca. complete ethanol conversion at T > 700 K and a minor, or even negligible, generation of by-products (acetaldehyde, acetone, ethane, ethylene). Operating at 950 K and 1.5 bar, a H-2 yield of 3.4 mol hydrogen per mol ethanol in feed was achieved for a liquid feed load of 0.22 mu l(liq)/(mg(cat) min) (S/C = 3), with 8.1% of CH4 and 8.2% of CO on dry basis. Kinetic parameters of a phenomenological set of reaction rate equations were fitted against experimental data, considering ethanol decomposition (methane formation) with subsequent methane steam reforming to both CO and CO2 and water-gas shift reaction. Copyright (c) 2013, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
引用
收藏
页码:4418 / 4428
页数:11
相关论文
共 25 条
[1]   Surface-structure sensitivity of CO oxidation over polycrystalline ceria powders [J].
Aneggi, E ;
Llorca, J ;
Boaro, M ;
Trovarelli, A .
JOURNAL OF CATALYSIS, 2005, 234 (01) :88-95
[2]   Low temperature catalytic steam reforming of ethanol. 2. Preliminary kinetic investigation of Pt/CeO2 catalysts [J].
Ciambelli, P. ;
Palma, V. ;
Ruggiero, A. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2010, 96 (1-2) :190-197
[3]   Mechanistic Aspects of the Ethanol Steam Reforming Reaction for Hydrogen Production on Pt, Ni, and PtNi Catalysts Supported on γ-Al2O3 [J].
Cruz Sanchez-Sanchez, Maria ;
Navarro Yerga, Rufino M. ;
Kondarides, Dimitris I. ;
Verykios, Xenophon E. ;
Fierro, Jose Luis G. .
JOURNAL OF PHYSICAL CHEMISTRY A, 2010, 114 (11) :3873-3882
[4]  
Cybulski A.J. Moulijn., 1998, Structured Catalysts and Reactors
[5]   Hydrogen production by ethanol reforming over Rh/CeO2-ZrO2 catalysts [J].
Diagne, C ;
Idriss, H ;
Kiennemann, A .
CATALYSIS COMMUNICATIONS, 2002, 3 (12) :565-571
[6]  
Elnashaie S, 1993, MODELING SIMULATION
[7]   Bio-ethanol, a suitable fuel to produce hydrogen for a molten carbonate fuel cell [J].
Frusteri, Francesco ;
Freni, Salvatore .
JOURNAL OF POWER SOURCES, 2007, 173 (01) :200-209
[8]   Kinetic study of ethanol reforming in a microreactor [J].
Goerke, O. ;
Pfeifer, P. ;
Schubert, K. .
APPLIED CATALYSIS A-GENERAL, 2009, 360 (02) :232-241
[9]   Ethanol Steam Reforming over Rh(1%)MgAl2O4/Al2O3: A Kinetic Study [J].
Graschinsky, Cecilia ;
Laborde, Miguel ;
Amadeo, Norma ;
Le Valant, Anthony ;
Bion, Nicolas ;
Epron, Florence ;
Duprez, Daniel .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2010, 49 (24) :12383-12389
[10]   A Phenomenological Study of the Metal-Oxide Interface: The Role of Catalysis in Hydrogen Production from Renewable Resources [J].
Idriss, Hicham ;
Scott, Morgan ;
Llorca, Jordi ;
Chan, Sze C. ;
Chiu, William ;
Sheng, Po-Yo ;
Yee, Anna ;
Blackford, Mark A. ;
Pas, Steve J. ;
Hill, Anita J. ;
Alamgir, Faisal M. ;
Rettew, Robert ;
Petersburg, Cole ;
Senanayake, Sanjaya D. ;
Barteau, Mark A. .
CHEMSUSCHEM, 2008, 1 (11) :905-910