TY - JOUR
T1 - Steam reforming of ethanol over skeletal Ni-based catalysts
T2 - A temperature programmed desorption and kinetic study
AU - Zhang, Chengxi
AU - Li, Shuirong
AU - Wu, Gaowei
AU - Huang, Zhiqi
AU - Han, Zhiping
AU - Wang, Tuo
AU - Gong, Jinlong
PY - 2014/2
Y1 - 2014/2
N2 - 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 H2 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 H2 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°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.
AB - 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 H2 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 H2 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°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.
KW - Eley-rideal mechanism
KW - Ethanol decomposition
KW - Ethanol steam reforming
KW - Kinetics
KW - Raney ni
UR - http://www.scopus.com/inward/record.url?scp=84892438064&partnerID=8YFLogxK
U2 - 10.1002/aic.14264
DO - 10.1002/aic.14264
M3 - Article
AN - SCOPUS:84892438064
SN - 0001-1541
VL - 60
SP - 635
EP - 644
JO - AIChE Journal
JF - AIChE Journal
IS - 2
ER -