Carbon formation and its influence on ethanol steam reforming over Ni/Al2O3 catalysts

被引:222
作者
Alberton, Andre L.
Souza, Mariana M. V. M.
Schmal, Martin [1 ]
机构
[1] Univ Fed Rio de Janeiro, COPPE, Peq, Nucat, BR-21941 Rio De Janeiro, Brazil
[2] Univ Fed Rio de Janeiro, Escola Quim, BR-21941 Rio De Janeiro, Brazil
关键词
ethanol steam reforming; Ni/Al2O3; catalysts; deactivation; coke deposition;
D O I
10.1016/j.cattod.2007.01.062
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Ethanol steam reforming was studied over Ni/Al2O3 catalysts. The effect of support (alpha- and gamma-Al2O3), metal loading and a comparison between conventional H-2 reduction with an activation method employing a CH4/O-2 mixture was investigated. The properties of catalysts were studied by N-2 physisorption, X-ray diffraction (XRD) and temperature programmed reduction (TPR). After activity tests, the catalysts were analyzed by scanning electron microscopy (SEM) and thermogravimetric analysis (TG/DTA). Ni supported on gamma-Al2O3 was more active for H-2 production than the catalyst supported on alpha-Al2O3. Metal loading did not affect the catalytic performance. The alternative activation method with CH4/O-2 mixture affected differently the activity and stability of the Ni/gamma-Al2O3 and the Ni/alpha-Al2O3 catalyst. This activation method increased significantly the stability of Ni/alpha-Al2O3 compared to H-2 reduction. SEM and TG/DTA analysis indicate the formation of filamentous carbon during the CH4/O-2 activation step, which is associated with the increasing catalyst activity and stability. The effect of temperature on the type of carbon formed was investigated; indicating that filamentous coke increased activity while encapsulating coke promoted deactivation. A discussion about carbon formation and the influence on the activity is presented. (c) 2007 Elsevier B.V. All rights reserved.
引用
收藏
页码:257 / 264
页数:8
相关论文
共 28 条
[1]   Bio-ethanol catalytic steam reforming over supported metal catalysts [J].
Auprêtre, F ;
Descorme, C ;
Duprez, D .
CATALYSIS COMMUNICATIONS, 2002, 3 (06) :263-267
[2]   Steam reforming and graphite formation on Ni catalysts [J].
Bengaard, HS ;
Norskov, JK ;
Sehested, J ;
Clausen, BS ;
Nielsen, LP ;
Molenbroek, AM ;
Rostrup-Nielsen, JR .
JOURNAL OF CATALYSIS, 2002, 209 (02) :365-384
[3]  
Bokx P. K. D., 1985, J CATAL, V96, P454
[4]   Production of hydrogen for fuel cells by reformation of biomass-derived ethanol [J].
Fatsikostas, AN ;
Kondarides, DI ;
Verykios, XE .
CATALYSIS TODAY, 2002, 75 (1-4) :145-155
[5]   Steam reforming of ethanol on Ni/MgO catalysts:: H2 production for MCFC [J].
Freni, S ;
Cavallaro, S ;
Mondello, N ;
Spadaro, L ;
Frusteri, F .
JOURNAL OF POWER SOURCES, 2002, 108 (1-2) :53-57
[6]   Production of hydrogen for MC fuel cell by steam reforming of ethanol over MgO supported Ni and Co catalysts [J].
Freni, S ;
Cavallaro, S ;
Mondello, N ;
Spadaro, L ;
Frusteri, F .
CATALYSIS COMMUNICATIONS, 2003, 4 (06) :259-268
[7]   Steam reforming of bio-ethanol on alkali-doped Ni/MgO catalysts: hydrogen production for MC fuel cell [J].
Frusteri, F ;
Freni, S ;
Chiodo, V ;
Spadaro, L ;
Di Blasi, O ;
Bonura, G ;
Cavallaro, S .
APPLIED CATALYSIS A-GENERAL, 2004, 270 (1-2) :1-7
[8]   HYDROGEN-PRODUCTION BY THE STEAM REFORMING OF ETHANOL - THERMODYNAMIC ANALYSIS [J].
GARCIA, EY ;
LABORDE, MA .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 1991, 16 (05) :307-312
[9]   Coke formation over a nickel catalyst under methane dry reforming conditions:: Thermodynamic and kinetic models [J].
Ginsburg, JM ;
Piña, J ;
El Solh, T ;
de Lasa, HI .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2005, 44 (14) :4846-4854
[10]   THE ROLE OF ANION IN THE PREPARATION OF NICKEL-CATALYST DETECTED BY TPR AND FTIR SPECTRA [J].
HO, SC ;
CHOU, TC .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1995, 34 (07) :2279-2284