Production of hydrogen via partial oxidation of methanol over Au/TiO2 catalysts

被引:70
作者
Chang, FW [1 ]
Yu, HY [1 ]
Roselin, LS [1 ]
Yang, HC [1 ]
机构
[1] Natl Cent Univ, Dept Chem & Mat Engn, Chungli 32001, Taiwan
关键词
D O I
10.1016/j.apcata.2005.05.024
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Selective production of hydrogen by partial oxidation of methanol (CH(3)oH -> (1/2)O-2 -> 2H(2) + CO2) over Au/TiO2 catalysts, prepared by a deposition-precipitation method, was studied. The catalysts were characterized by XRD, TEM, and XPS analyses. TEM observations show that the Au/TiO2 catalysts exhibit hemispherical gold particles, which are strongly attached to the metal oxide support at their flat planes. The size of the gold particles decreases from 3.5 to 1.9 nm during preparation of the catalysts with the rise in pH from 6 to 9 and increases from 2.9 to 4.3 nm with the rise in calcination temperature up to 673 K. XPS analyses demonstrate that in uncalcined catalysts gold existed in three different states: i.e., metallic gold (Au-0), non-metallic gold (Au delta+) and AU(2)O(3), and in catalysts calcined at 573 K only in metallic state. The catalytic activity is strongly dependent on the gold particle size. The catalyst precipitated at pH 8 and uncalcined catalysts show the highest activity for hydrogen generation. The partial pressure of oxygen plays an important role in determining the product distribution. There is no carbon monoxide detected when the O-2/CH3OH molar ratio in the feed is 0.3. Both hydrogen selectivity and methanol conversion increase with increasing the reaction temperature. The reaction pathway is suggested to consist of consecutive methanol combustion, partial oxidation and steam reforming. (c) 2005 Elsevier B.V. All rights reserved.
引用
收藏
页码:138 / 147
页数:10
相关论文
共 39 条
[1]   Production of hydrogen by partial oxidation of methanol over ZnO-supported palladium catalysts prepared by microemulsion technique [J].
Agrell, J ;
Germani, G ;
Järås, SG ;
Boutonnet, M .
APPLIED CATALYSIS A-GENERAL, 2003, 242 (02) :233-245
[2]   Production of hydrogen from methanol over binary Cu/ZnO catalysts - Part II. Catalytic activity and reaction pathways [J].
Agrell, J ;
Boutonnet, M ;
Fierro, JLG .
APPLIED CATALYSIS A-GENERAL, 2003, 253 (01) :213-223
[3]   Production of hydrogen by partial oxidation of methanol over Cu/ZnO catalysts prepared by microemulsion technique [J].
Agrell, J ;
Hasselbo, K ;
Jansson, K ;
Järås, SG ;
Boutonnet, M .
APPLIED CATALYSIS A-GENERAL, 2001, 211 (02) :239-250
[4]   Partial oxidation of methanol to produce hydrogen over Cu-Zn-based catalysts [J].
Alejo, L ;
Lago, R ;
Pena, MA ;
Fierro, JLG .
APPLIED CATALYSIS A-GENERAL, 1997, 162 (1-2) :281-297
[5]  
APPLEBY J, 1989, FUEL CELL HDB, P177
[6]   Oxidation of CO on gold supported catalysts prepared by laser vaporization: Direct evidence of support contribution [J].
Arrii, S ;
Morfin, F ;
Renouprez, AJ ;
Rousset, JL .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (04) :1199-1205
[7]   PHOTOASSISTED HYDROGEN-PRODUCTION FROM A WATER-ETHANOL SOLUTION - A COMPARISON OF ACTIVITIES OF AU-TIO2 AND PT-TIO2 [J].
BAMWENDA, GR ;
TSUBOTA, S ;
NAKAMURA, T ;
HARUTA, M .
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY, 1995, 89 (02) :177-189
[8]   Gold catalysts supported on titanium oxide for catalytic wet air oxidation of succinic acid [J].
Besson, M ;
Kallel, A ;
Gallezot, P ;
Zanella, R ;
Louis, C .
CATALYSIS COMMUNICATIONS, 2003, 4 (09) :471-476
[9]   FTIR study of the low-temperature water-gas shift reaction on Au/Fe2O3 and Au/TiO2 catalysts [J].
Boccuzzi, F ;
Chiorino, A ;
Manzoli, M ;
Andreeva, D ;
Tabakova, T .
JOURNAL OF CATALYSIS, 1999, 188 (01) :176-185
[10]   Au/TiO2 nanosized samples:: A catalytic, TEM, and FTIR study of the effect of calcination temperature on the CO oxidation [J].
Boccuzzi, F ;
Chiorino, A ;
Manzoli, M ;
Lu, P ;
Akita, T ;
Ichikawa, S ;
Haruta, M .
JOURNAL OF CATALYSIS, 2001, 202 (02) :256-267