Hydrogen production by ethanol steam reforming on nickel catalysts: Effect of support modification by CeO2 and La2O3

被引:80
作者
Dan, Monica [1 ]
Mihet, Maria [1 ]
Tasnadi-Asztalos, Zsolt [2 ]
Imre-Lucaci, Arpad [2 ]
Katona, Gabriel [2 ]
Lazar, Mihaela D. [1 ]
机构
[1] Natl Inst Res & Dev Isotop & Mol Technol, Cluj Napoca 400293, Romania
[2] Univ Babes Bolyai, Fac Chem & Chem Engn, Cluj Napoca 400028, Romania
关键词
Hydrogen; Ethanol steam reforming; CeO2 promoted catalysts; La2O3 promoted catalyst; Thermodynamic evaluation of ethanol steam reforming; TEMPERATURE-PROGRAMMED-REDUCTION; BIO-ETHANOL; THERMODYNAMIC ANALYSIS; REACTION-MECHANISM; ALUMINA CATALYSTS; SURFACE-AREA; NI; METHANE; BEHAVIOR; SILICA;
D O I
10.1016/j.fuel.2015.01.050
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
Ethanol steam reforming at low temperatures and high water: ethanol ratios was studied on Ni (8 wt.%) catalysts deposited on CeO2 (6 wt.%) or La2O3 (6 wt.%) promoted alumina and zirconia supports. The catalysts were prepared by successive impregnation: first the rare earth oxide and then the Ni, and characterized by XRD, H-2 chemisorption, TPR and H-2-TPD. Promotion of both alumina and zirconia with CeO2 and La2O3 leads to changes in the Ni - support interaction resulting in much better dispersion and stabilization of the Ni nanoparticles on the catalyst surface. For La2O3 promoted catalysts 100% ethanol conversion was obtained in the experimental conditions used in this work, at temperatures as low as 300 degrees C. The ethanol conversion was improved by the addition of CeO2 to zirconia supported catalyst, but was not significantly influenced by the addition of CeO2 to alumina supported one. A thermodynamic study of ethanol steam reforming was performed (CHEMCAD process simulator and Gibbs reactor with calculations based on free energy minimization), in order to find the thermodynamic equilibrium composition of reaction products in the particular experimental reaction conditions used in this work. The reaction products mixture at 350 degrees C contains higher proportion of hydrogen and lower proportion of methane than the equilibrium concentration predicted by thermodynamic analysis. The best hydrogen yield was obtained for Ni/La2O3-ZrO2 catalyst. All catalysts except Ni/ZrO2 are stable in 24 h time on stream experiments. (C) 2015 Elsevier Ltd. All rights reserved.
引用
收藏
页码:260 / 268
页数:9
相关论文
共 41 条
[1]   The Hydrogen Issue [J].
Armaroli, Nicola ;
Balzani, Vincenzo .
CHEMSUSCHEM, 2011, 4 (01) :21-36
[2]   Low Temperature Steam Reforming of Ethanol Over Supported Noble Metal Catalysts [J].
Basagiannis, Aristides C. ;
Panagiotopoulou, Paraskevi ;
Verykios, Xenophon E. .
TOPICS IN CATALYSIS, 2008, 51 (1-4) :2-12
[3]   Steam reforming of ethanol at medium pressure over Ru/Al2O3: effect of temperature and catalyst deactivation [J].
Bilal, Muhammad ;
Jackson, S. David .
CATALYSIS SCIENCE & TECHNOLOGY, 2012, 2 (10) :2043-2051
[4]   Steam reforming of ethanol for production of hydrogen over Ni/CeO2-ZrO2 catalyst:: Effect of support and metal loading [J].
Biswas, Prakash ;
Kunzru, Deepak .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2007, 32 (08) :969-980
[5]   Nickel nanoparticles supported on silica of low surface area. Hydrogen chemisorption and TPD and catalytic properties [J].
Boudjahem, AG ;
Monteverdi, S ;
Mercy, M ;
Ghanbaja, D ;
Bettahar, MM .
CATALYSIS LETTERS, 2002, 84 (1-2) :115-122
[6]   Steam-reforming of ethanol for hydrogen production [J].
Bshish, Ahmed ;
Yakoob, Zahira ;
Narayanan, Binitha ;
Ramakrishnan, Resmi ;
Ebshish, Ali .
CHEMICAL PAPERS, 2011, 65 (03) :251-266
[7]   Ethanol steam reforming over NiLaZr and NiCuLaZr mixed metal oxide catalysts [J].
Bussi, Juan ;
Musso, Mauricio ;
Veiga, Santiago ;
Bespalko, Nicolas ;
Faccio, Ricardo ;
Roger, Anne-Cecile .
CATALYSIS TODAY, 2013, 213 :42-49
[8]   Gold, palladium and gold-palladium supported on silica catalysts prepared by sol-gel method: synthesis, characterization and catalytic behavior in the ethanol steam reforming [J].
da Silva, Anderson G. M. ;
Robles-Dutenhefner, Patricia A. ;
Dias, Anderson ;
Fajardo, Humberto V. ;
Lovon, Adriana S. P. ;
Lovon-Quintana, Juan J. ;
Valenca, Gustavo P. .
JOURNAL OF SOL-GEL SCIENCE AND TECHNOLOGY, 2013, 67 (02) :273-281
[9]   Bimetallic heterogeneous catalysts for hydrogen production [J].
Dal Santo, Vladimiro ;
Gallo, Alessandro ;
Naldoni, Alberto ;
Guidotti, Matteo ;
Psaro, Rinaldo .
CATALYSIS TODAY, 2012, 197 (01) :190-205
[10]   Modified Ni-Cu Catalysts for Ethanol Steam Reforming [J].
Dan, M. ;
Mihet, M. ;
Almasan, V. ;
Borodi, G. ;
Katona, G. ;
Muresan, L. ;
Lazar, M. D. .
PROCESSES IN ISOTOPES AND MOLECULES (PIM 2013), 2013, 1565 :208-214