Direct synthesis of hydrogen peroxide from H2 and O2 using Pd and Au catalysts

被引:342
作者
Landon, P
Collier, PJ
Carley, AF
Chadwick, D
Papworth, AJ
Burrows, A
Kiely, CJ
Hutchings, GJ
机构
[1] Cardiff Univ, Dept Chem, Cardiff CF10 3TB, S Glam, Wales
[2] Univ London Imperial Coll Sci Technol & Med, Dept Chem Engn, London SW7 2BY, England
[3] Univ Liverpool, Dept Engn & Chem, Liverpool L69 3BX, Merseyside, England
[4] Lehigh Univ, Dept Mat Sci & Engn, Bethlehem, PA 18015 USA
关键词
D O I
10.1039/b211338b
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 from H-2 and O-2 using a range of supported metal catalysts is described and discussed. A detailed study of the factors influencing the formation and decomposition of hydrogen peroxide is presented for a Pd/sulfonated carbon catalyst in a methanol/water solvent. The use of low temperatures (1-2 degreesC) and short reaction (residence) time are identified as the key factors that favour high selectivity to hydrogen peroxide. Decomposition of hydrogen peroxide, mainly via further hydrogenation, prevents the formation of high concentrations of hydrogen peroxide. Combustion of hydrogen to water is a competing reaction that becomes significant at higher temperatures, but this can be partially inhibited by the addition of HBr. A second set of supported Pd and Au catalysts are evaluated for the direct synthesis of hydrogen peroxide using supercritical CO2 as a solvent. The use of supercritical CO2 is shown to be beneficial when compared with hydrogen peroxide formation at a temperature just below the critical temperature for CO2. However, at the critical temperature of CO2 (31.1 degreesC), the decomposition of hydrogen peroxide is rapid and only low rates of hydrogen peroxide formation are observed. At low temperature (2 degreesC) supported Au catalysts are shown to be very selective for the synthesis of hydrogen peroxide. The rate of hydrogen peroxide synthesis is enhanced markedly when Pd is present with Au and a detailed scanning transmission electron microscopy study shows that the 2-9 nm metal nanoparticles present in this supported catalyst are a Au:Pd alloy.
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页码:1917 / 1923
页数:7
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