Steam Reforming of Ethanol over Skeletal Ni-based Catalysts: A Temperature Programmed Desorption and Kinetic Study

被引:37
|
作者
Zhang, Chengxi [1 ]
Li, Shuirong [1 ]
Wu, Gaowei [1 ]
Huang, Zhiqi [1 ]
Han, Zhiping [1 ]
Wang, Tuo [1 ]
Gong, Jinlong [1 ]
机构
[1] Tianjin Univ, Key Lab Green Chem Technol, Minist Educ, Sch Chem Engn & Technol,Collaborat Innovat Ctr Ch, Tianjin 300072, Peoples R China
基金
美国国家科学基金会;
关键词
ethanol steam reforming; Raney ni; kinetics; eley-rideal mechanism; ethanol decomposition; GAS SHIFT REACTION; BED TUBULAR REACTOR; HYDROGEN-PRODUCTION; BIO-ETHANOL; ETHYLENE-GLYCOL; REACTION-MECHANISM; NICKEL-CATALYSTS; CARBON-MONOXIDE; H-2; PRODUCTION; CRUDE ETHANOL;
D O I
10.1002/aic.14264
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
An investigation on reaction scheme and kinetics for ethanol steam reforming on skeletal nickel catalysts is described. Catalytic activity of skeletal nickel catalyst for low-temperature steam reforming has been studied in detail, and the reasons for its high reactivity for H-2 production are attained by probe reactions. Higher activity of water gas shift reaction and methanation contributes to the low CO selectivity. Cu and Pt addition can promote WGSR and suppress methanation, and, thus, improve H-2 production. A reaction scheme on skeletal nickel catalyst has been proposed through temperature programmed reaction spectroscopy experiments. An Eley-Rideal model is put forward for kinetic studies, which contains three surface reactions: ethanol decomposition, water gas shift reaction, and methane steam reforming reaction. The kinetics was studied at 300-400 degrees C using a randomized algorithms method and a least-squares method to solve the differential equations and fit the experimental data; the goodness of fit obtained with this model is above 0.95. The activation energies for the ethanol decomposition, methane steam reforming, and water gas shift reaction are 187.7 kJ/mol, 138.5 kJ/mol and 52.8 kJ/mol, respectively. Thus, ethanol decomposition was determined to be the rate determining reaction of ethanol steam reforming on skeletal nickel catalysts. (c) 2013 American Institute of Chemical Engineers AIChE J 60: 635-644, 2014
引用
收藏
页码:635 / 644
页数:10
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