Aqueous Phase Reforming of ethylene glycol - Role of intermediates in catalyst performance

被引:76
作者
de Vlieger, D. J. M. [1 ]
Mojet, B. L. [1 ]
Lefferts, L. [1 ]
Seshan, K. [1 ]
机构
[1] Univ Twente, Fac Sci & Technol, MESA Inst, Catalyt Proc & Mat CPM, NL-7500 AE Enschede, Netherlands
关键词
Boehmite; Raman; FTIR spectroscopy; Deactivation; Acetic acid; Sustainable; METAL-CATALYSTS; ACETIC-ACID; OXYGENATED HYDROCARBONS; SUPERCRITICAL WATER; HYDROGEN-PRODUCTION; RENEWABLE HYDROGEN; CARBON FORMATION; ETHANOL; GLYCEROL; ALUMINA;
D O I
10.1016/j.jcat.2012.05.019
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
Liquid product formation during the aqueous catalytic reforming of ethylene glycol (EG) was studied up to 450 degrees C and 250 bar pressure. Methanol, ethanol, and acetic acid were the main liquid by-products during EG reforming in the presence of alumina-supported Pt and Pt-Ni catalysts. The effect of these by-products on selectivity and catalyst stability was further investigated by studying reforming of these components. Reforming of these products was shown to be responsible for the formation of alkanes. The high dehydrogenation activity of Pt-Ni catalysts leads to high H-2 yields during EG reforming by (i) suppressing the formation of methane during methanol reforming (a major by-product of EG reforming) and (ii) suppressing the formation of acetic acid. In addition, the decrease in acetic acid formation showed a positive effect on catalyst lifetime. Acetic acid was found to be responsible for hydroxylation of the Al2O3 support, leading to migration and coverage of the metal particles by Al(OH)(x) and resulting in deactivation of the Pt-based catalysts. (C) 2012 Elsevier Inc. All rights reserved.
引用
收藏
页码:239 / 245
页数:7
相关论文
共 38 条
[21]   Ethanol reforming for hydrogen production in a hybrid electric vehicle: process optimisation [J].
Klouz, V ;
Fierro, V ;
Denton, P ;
Katz, H ;
Lisse, JP ;
Bouvot-Mauduit, S ;
Mirodatos, C .
JOURNAL OF POWER SOURCES, 2002, 105 (01) :26-34
[22]   Production of renewable hydrogen from aqueous-phase reforming of glycerol over Pt catalysts supported on different oxides [J].
Menezes, Andre O. ;
Rodrigues, Michelly T. ;
Zimmaro, Adriana ;
Borges, Luiz E. P. ;
Fraga, Marco A. .
RENEWABLE ENERGY, 2011, 36 (02) :595-599
[23]   Water density dependence of formaldehyde reaction in supercritical water [J].
Osada, M ;
Watanabe, M ;
Sue, K ;
Adschiri, T ;
Arai, K .
JOURNAL OF SUPERCRITICAL FLUIDS, 2004, 28 (2-3) :219-224
[24]   Structural Changes of γ-Al2O3-Supported Catalysts in Hot Liquid Water [J].
Ravenelle, Ryan M. ;
Copeland, John R. ;
Kim, Wun-Gwi ;
Crittenden, John C. ;
Sievers, Carsten .
ACS CATALYSIS, 2011, 1 (05) :552-561
[25]   Surface modification of solution combustion synthesized Ni/Al2O3 catalyst for aqueous-phase reforming of ethanol [J].
Roy, B. ;
Loganathan, K. ;
Pham, H. N. ;
Datye, A. K. ;
Leclerc, C. A. .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2010, 35 (21) :11700-11708
[26]   Comparison of Raman spectra in characterizing gibbsite, bayerite, diaspore and boehmite [J].
Ruan, HD ;
Frost, RL ;
Kloprogge, JT .
JOURNAL OF RAMAN SPECTROSCOPY, 2001, 32 (09) :745-750
[27]   Catalysts for methanol steam reforming-A review [J].
Sa, Sandra ;
Silva, Hugo ;
Brandao, Lucia ;
Sousa, Jose M. ;
Mendes, Adelio .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2010, 99 (1-2) :43-57
[28]   A perspective on catalysis in sub- and supercritical water [J].
Savage, Phillip E. .
JOURNAL OF SUPERCRITICAL FLUIDS, 2009, 47 (03) :407-414
[29]   Aqueous-phase reforming of oxygenated hydrocarbons over Sn-modified Ni catalysts [J].
Shabaker, JW ;
Huber, GW ;
Dumesic, JA .
JOURNAL OF CATALYSIS, 2004, 222 (01) :180-191
[30]   Ethanol and ethylene glycol on Ni/Pt(111) bimetallic surfaces: A DFT and HREELS study [J].
Skoplyak, Orest ;
Barteau, Mark A. ;
Chen, Jingguang G. .
SURFACE SCIENCE, 2008, 602 (23) :3578-3587