Hydrogen production by steam reforming of ethanol over nickel supported on La-modified alumina catalysts prepared by sol-gel

被引:67
作者
Melchor-Hernandez, C. [1 ]
Gomez-Cortes, A. [1 ]
Diaz, G. [1 ]
机构
[1] Univ Nacl Autonoma Mexico, Inst Fis, Mexico City 04510, DF, Mexico
关键词
Hydrogen; Ethanol; Lanthana-alumina; Nickel; Sol-gel; TEMPERATURE-PROGRAMMED-REDUCTION; STRUCTURAL-PROPERTIES; NI; REFORMATION; OXIDATION; METHANE; CARBON; PD;
D O I
10.1016/j.fuel.2013.01.047
中图分类号
TE [石油、天然气工业]; TK [能源与动力工程];
学科分类号
0807 ; 0820 ;
摘要
The catalytic properties for steam reforming of ethanol (SRE) of 10 wt.% nickel supported on La-modified alumina prepared by sol-gel were studied. Lanthanum oxide content was in the range 0-12 wt.%. Supports were calcined at 650 degrees C and catalysts were calcined at 450 degrees C and reduced at 600 degrees C. Catalysts were characterized by ICP, XRD, TPR, TPO and TEM. The progressive La-addition to the support had several effects: a structural effect in the alumina, promotion of a better dispersion of the NiO phase and increased number of NiO species reducing at lower temperature. Average Ni crystal size as determined by XRD in reduced samples was 6.3 nm. The SRE at molar ratio H2O/EtOH = 3 was studied and ethanol conversion as a function of temperature showed small differences as a function of the lanthanum content, but the hydrogen yield was much more important for La-containing catalysts. Deactivation experiments at 500 degrees C showed that catalysts with higher La content were more stable and that the strong decrease in the ethanol conversion occurred in the first hours on stream at these experimental conditions. A good correlation between deactivation trend, ethylene evolution and occurrence of lower temperature gasified carbon-type residues was established with the support composition. Sintering of Ni particles occurred in all samples after reaction, but despite the presence of larger Ni particles in the Ni/Al2O3-La12 catalyst this was the most stable one. As lanthanum species are progressively present in the support its contribution to stabilization of the catalyst is certainly related to the enhancement of gasification of carbon residues on the surface of the catalyst but also to a close interaction with nickel particles. (c) 2013 Elsevier Ltd. All rights reserved.
引用
收藏
页码:828 / 835
页数:8
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