Effect of acid pre-treatment on AuPd/SiO2 catalysts for the direct synthesis of hydrogen peroxide

被引:47
作者
Edwards, Jennifer K. [1 ]
Parker, Stewart F. [2 ]
Pritchard, James [1 ]
Piccinini, Marco [1 ]
Freakley, Simon J. [1 ]
He, Qian [3 ]
Carley, Albert F. [1 ]
Kiely, Christopher J. [3 ]
Hutchings, Graham J. [1 ]
机构
[1] Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Cardiff CF10 3AT, S Glam, Wales
[2] STFC Rutherford Appleton Lab, ISIS Facil, Didcot OX11 0QX, Oxon, England
[3] Lehigh Univ, Dept Mat Sci & Engn, Bethlehem, PA 18015 USA
关键词
GOLD-PALLADIUM CATALYSTS; PD CATALYSTS; SELECTIVE OXIDATION; H-2; O-2; H2O2; NANOPARTICLES; CHLORIDE;
D O I
10.1039/c2cy20767b
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
The direct synthesis of hydrogen peroxide is investigated using silica supported Au, Pd and AuPd catalysts. Acid pre-treatment of the silica leads to an increase in the activity of the Pd-containing catalysts and also gives rise to a synergistic enhancement in activity when Au and Pd are combined that is absent in the untreated catalysts. The acid pre-treated mono and bi metallic catalysts show much reduced H2O2 hydrogenation activity compared to their untreated counterparts. The acid pre-treatment increases the concentration of the hydroxyl groups on the support, as demonstrated using inelastic neutron scattering, which helps to disperse the metals on the support. Pd can be dispersed effectively on silica, but Au is very poorly dispersed although this is enhanced marginally by the acid pre-treatment. The origin of the synergistic effect is discussed and is considered to be related to the incorporation of a small amount of Au within the Pd nanoparticles.
引用
收藏
页码:812 / 818
页数:7
相关论文
共 26 条
[1]   Hydrogen peroxide formation in the interaction of oxygen with boron-containing Pd catalysts prereduced by hydrazine in aqueous acidic medium containing bromide anions [J].
Choudhary, VR ;
Samanta, C .
CATALYSIS LETTERS, 2005, 99 (1-2) :79-81
[2]   Activation of supported Pd metal catalysts for selective oxidation of hydrogen to hydrogen peroxide [J].
Choudhary, VR ;
Gaikwad, AG ;
Sansare, SD .
CATALYSIS LETTERS, 2002, 83 (3-4) :235-239
[3]   Role of chloride or bromide anions and protons for promoting the selective oxidation of H2 by O2 to H2O2 over supported Pd catalysts in an aqueous medium [J].
Choudhary, VR ;
Samanta, C .
JOURNAL OF CATALYSIS, 2006, 238 (01) :28-38
[4]   Au-Pd supported nanocrystals as catalysts for the direct synthesis of hydrogen peroxide from H2 and O2 [J].
Edwards, Jennifer K. ;
Thomas, Adrian ;
Carley, Albert F. ;
Herzing, Andrew A. ;
Kiely, Christopher J. ;
Hutchings, Graham J. .
GREEN CHEMISTRY, 2008, 10 (04) :388-394
[5]   Direct synthesis of hydrogen peroxide from H2 and O2 using supported Au-Pd catalysts [J].
Edwards, Jennifer K. ;
Carley, Albert F. ;
Herzing, Andrew A. ;
Kiely, Christopher J. ;
Hutchings, Graham J. .
FARADAY DISCUSSIONS, 2008, 138 :225-239
[6]   Direct Synthesis of H2O2 from H2 and O2 over Gold, Palladium, and Gold-Palladium Catalysts Supported on Acid-Pretreated TiO2 [J].
Edwards, Jennifer K. ;
Ntainjua N, Edwin ;
Carley, Albert F. ;
Herzing, Andrew A. ;
Kiely, Christopher J. ;
Hutchings, Graham J. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2009, 48 (45) :8512-8515
[7]   Palladium and Gold-Palladium Catalysts for the Direct Synthesis of Hydrogen Peroxide [J].
Edwards, Jennifer K. ;
Hutchings, Graham J. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2008, 47 (48) :9192-9198
[8]   Switching Off Hydrogen Peroxide Hydrogenation in the Direct Synthesis Process [J].
Edwards, Jennifer K. ;
Solsona, Benjamin ;
N, Edwin Ntainjua ;
Carley, Albert F. ;
Herzing, Andrew A. ;
Kiely, Christopher J. ;
Hutchings, Graham J. .
SCIENCE, 2009, 323 (5917) :1037-1041
[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