Microstructural development and catalytic performance of Au-Pd nanoparticles on Al2O3 supports:: The effect of heat treatment temperature and atmosphere

被引:78
作者
Herzing, A. A. [1 ,2 ]
Carley, A. F. [3 ]
Edwards, J. K. [3 ]
Hutchings, G. J. [3 ]
Kiely, C. J. [1 ]
机构
[1] Lehigh Univ, Ctr Adv Mat & Nanotechnol, Bethlehem, PA 18015 USA
[2] NIST, Gaithersburg, MD 20899 USA
[3] Cardiff Univ, Sch Chem, Cardiff CF10 3AT, Wales
关键词
D O I
10.1021/cm702762d
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
Au-Pd nanoparticles supported on a variety of oxides are known to be highly active catalysts for a number of interesting reactions, including the direct synthesis of H2O2 from H-2 and O-2. A systematic series of Au-Pd/Al2O3 catalysts, subjected to a variety of heat treatments, have been examined by STEM-XEDS and XPS in an effort to track the microstructural development of the bimetallic particles. It was observed that the nature and size distribution of the AuPd particles was highly dependent upon both the heat treatment temperature and the atmosphere. As synthesized particles were homogeneous alloys, but subsequent calcination in air produced metal particles which showed a progressive enrichment of Pd at their surface. The change from homogeneous alloy to Pd-rich shell/Au-rich core morphology and increase in average particle size induced by the calcination treatment was accompanied by a significant decrease in the activity of the catalyst. However, the calcination step is deemed to be necessary to produce a stable reusable catalyst that resists leaching of the metal from the oxide surface into solution. Furthermore, it is shown that the subsequent reduction of a previously calcined catalyst is highly deleterious to its performance and stimulates many of the AuPd particles to "invert" and form a Pd-rich core/Au-rich shell morphology.
引用
收藏
页码:1492 / 1501
页数:10
相关论文
共 30 条
[1]   Quantitative characterization of nanoprecipitates in irradiated low-alloy steels: advances in the application of FEG-STEM quantitative microanalysis to real materials [J].
Burke, M. G. ;
Watanabe, M. ;
Williams, D. B. ;
Hyde, J. M. .
JOURNAL OF MATERIALS SCIENCE, 2006, 41 (14) :4512-4522
[2]   The promotional effect of gold in catalysis by palladium-gold [J].
Chen, MS ;
Kumar, D ;
Yi, CW ;
Goodman, DW .
SCIENCE, 2005, 310 (5746) :291-293
[3]   Direct oxidation of H2 to H2O2 and decomposition of H2O2 over oxidized and reduced Pd-containing zeolite catalysts in acidic medium [J].
Choudhary, VR ;
Sansare, SD ;
Gaikwad, AG .
CATALYSIS LETTERS, 2002, 84 (1-2) :81-87
[4]  
CHOUDHARY VR, 2004, CHEM COMMUN, V18, P2004
[5]  
de Boer FR., 1988, COHESION METALS TRAN
[6]   The direct formation of H2O2 from H2 and O2 over colloidal palladium [J].
Dissanayake, DP ;
Lunsford, JH .
JOURNAL OF CATALYSIS, 2003, 214 (01) :113-120
[7]   Evidence for the role of colloidal palladium in the catalytic formation of H2O2 from H2 and O2 [J].
Dissanayake, DP ;
Lunsford, JH .
JOURNAL OF CATALYSIS, 2002, 206 (02) :173-176
[8]  
Edwards J, 2007, J MATER RES, V22, P831, DOI 10.1557/JMR.2007.0117
[9]   Direct synthesis of hydrogen peroxide from H2 and O2 using TiO2-supported Au-Pd catalysts [J].
Edwards, JK ;
Solsona, BE ;
Landon, P ;
Carley, AF ;
Herzing, A ;
Kiely, CJ ;
Hutchings, GJ .
JOURNAL OF CATALYSIS, 2005, 236 (01) :69-79
[10]   Direct synthesis of hydrogen peroxide from H2 andO2 using Au-Pd/Fe2O3 catalysts [J].
Edwards, JK ;
Solsona, B ;
Landon, P ;
Carley, AF ;
Herzing, A ;
Watanabe, M ;
Kiely, CJ ;
Hutchings, GJ .
JOURNAL OF MATERIALS CHEMISTRY, 2005, 15 (43) :4595-4600