The role of surface reactions on the active and selective catalyst design for bioethanol steam reforming

被引:26
作者
Benito, M. [1 ,2 ]
Padilla, R. [1 ]
Serrano-Lotina, A. [1 ]
Rodriguez, L. [1 ]
Brey, J. J. [3 ]
Daza, L. [1 ]
机构
[1] CSIC, Inst Catalisis & Petroleoquim, E-28049 Madrid, Spain
[2] CIEMAT, E-28040 Madrid, Spain
[3] Hynergreen Technol, Seville 41018, Spain
关键词
Bioethanol; Reforming; Bio-energy; Hydrogen; Fuel processor; Fuel cell; HYDROGEN-PRODUCTION; THERMODYNAMIC ANALYSIS; OXIDE CATALYST; BIO-ETHANOL; FUEL-CELLS; ACETONE; CONVERSION; STABILITY; MECHANISM; INSIGHTS;
D O I
10.1016/j.jpowsour.2009.02.015
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
In order to study the role of surface reactions involved in bioethanol steam reforming mechanism, a very active and selective catalyst for hydrogen production was analysed. The highest activity was obtained at 700 degrees C, temperature at which the catalyst achieved an ethanol conversion of 100% and a selectivity to hydrogen close to 70%. It also exhibited a very high hydrogen production efficiency, higher than 4.5 mol H-2 per mol of EtOH fed. The catalyst was operated at a steam to carbon ratio (S/C) of 4.8, at 700 degrees C and atmospheric pressure. No by-products, such as ethylene or acetaldehyde were observed. In order to consider a further application in an ethanol processor, a long-term stability test was performed under the conditions previously reported. After 750h, the catalyst still exhibited a high stability and selectivity to hydrogen production. Based on the intermediate products detected by temperature programmed desorption and reaction (TPD and TPR) experiments, a reaction pathway was proposed. Firstly, the adsorbed ethanol is dehydrogenated to acetaldehyde producing hydrogen. Secondly, the adsorbed acetaldehyde is transformed into acetone via acetic acid formation. Finally, acetone is reformed to produce hydrogen and carbon dioxide, which were the final reaction products. The promotion of such reaction sequence is the key to develop an active, selective and stable catalyst. which is the technical barrier for hydrogen production by ethanol reforming. (C) 2009 Elsevier B.V. All rights reserved.
引用
收藏
页码:158 / 164
页数:7
相关论文
共 33 条
[1]   Carbon formation and its influence on ethanol steam reforming over Ni/Al2O3 catalysts [J].
Alberton, Andre L. ;
Souza, Mariana M. V. M. ;
Schmal, Martin .
CATALYSIS TODAY, 2007, 123 (1-4) :257-264
[2]  
[Anonymous], IMP MIN 10 OBL BIOF
[3]   Characterization of the activity and stability of supported cobalt catalysts for the steam reforming of ethanol [J].
Batista, MS ;
Santos, RKS ;
Assaf, EM ;
Assaf, JM ;
Ticianelli, EA .
JOURNAL OF POWER SOURCES, 2003, 124 (01) :99-103
[4]   Thermodynamic analysis and performance of a 1 kW bioethanol processor for a PEMFC operation [J].
Benito, M. ;
Padilla, R. ;
Sanz, J. L. ;
Daza, L. .
JOURNAL OF POWER SOURCES, 2007, 169 (01) :123-130
[5]   Bio-ethanol steam reforming: Insights on the mechanism for hydrogen production [J].
Benito, M ;
Sanz, JL ;
Isabel, R ;
Padilla, R ;
Arjona, R ;
Daza, L .
JOURNAL OF POWER SOURCES, 2005, 151 :11-17
[6]  
BENITO M, 2006, Patent No. 2006075035
[7]   TEMPERATURE-PROGRAMMED REACTION STUDIES OF THE INTERACTION OF METHYL FORMATE AND ETHANOL WITH POLYCRYSTALLINE ZINC-OXIDE [J].
BOWKER, M ;
HOUGHTON, H ;
WAUGH, KC .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1982, 78 :2573-2582
[8]   TEMPERATURE-PROGRAMMED DESORPTION STUDIES OF ALCOHOL DECOMPOSITION ON ZNO - 1-PROPANOL, 1-BUTANOL, AND 2-BUTANOL [J].
BOWKER, M ;
PETTS, RW ;
WAUGH, KC .
JOURNAL OF CATALYSIS, 1986, 99 (01) :53-61
[9]   Catalytic transformation of ethanol into acetone using copper-pyrochlore catalysts [J].
Bussi, J ;
Parodi, S ;
Irigaray, B ;
Kieffer, R .
APPLIED CATALYSIS A-GENERAL, 1998, 172 (01) :117-129
[10]  
Coker A.K., 2001, MODELLING CHEM KINET