The role of the support in achieving high selectivity in the direct formation of hydrogen peroxide

被引:91
作者
Edwin, Ntainjua N. [1 ]
Edwards, Jennifer K. [1 ]
Carley, Albert F. [1 ]
Lopez-Sanchez, Jose Antonio [1 ]
Moulijn, Jacob A. [1 ]
Herzing, Andrew A. [2 ,3 ]
Kiely, Christopher J. [2 ]
Hutchings, Graham J. [1 ]
机构
[1] Cardiff Univ, Sch Chem, Cardiff CF10 3AT, S Glam, Wales
[2] Lehigh Univ, Ctr Adv Mat & Nanotechnol, Bethlehem, PA 18015 USA
[3] Natl Inst Stand & Technol, Surface & Microanal Sci Div, Gaithersburg, MD 20899 USA
基金
英国工程与自然科学研究理事会;
关键词
D O I
10.1039/b809881f
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Pd-only, Au-only and bimetallic AuPd catalysts supported on a range of supports (Al2O3, TiO2, MgO, and C) have been prepared by impregnation and tested for the hydrogenation and decomposition of hydrogen peroxide under conditions similar to those used in direct synthesis of hydrogen peroxide. Hydrogenation and decomposition are the main pathways for loss of selectivity and yield in the direct synthesis reaction, and the support is found to be a crucial parameter with respect to hydrogenation and decomposition activity. We show that by making the right choice of support for both the monometallic and bimetallic Au and Pd catalysts, it is possible to achieve very low hydrogen peroxide hydrogenation and decomposition activity, thus enhancing hydrogen peroxide productivity during synthesis. Carbon is found to be the optimal support for both monometallic Au and Pd catalysts as well as Au -Pd alloys, since carbon-supported catalysts gave the lowest hydrogenation and decomposition activities. Au-only catalysts were generally less active than Pd-only catalysts when utilizing the same support and metal loading. The addition of Au to Pd catalysts supported on TiO2 and carbon resulted in a decrease in both H2O2 hydrogenation and decomposition while the reverse effect was observed for the Al2O3 and MgO-supported catalysts. These effects are discussed in terms of the basicity of the support, and in particular the isoelectronic point of the support, which is a major factor in controlling the stability of hydrogen peroxide under reaction conditions.
引用
收藏
页码:1162 / 1169
页数:8
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