Hierarchically Ordered Nanoporous Pd/SBA-15 Catalyst for the Aerobic Selective Oxidation of Sterically Challenging Allylic Alcohols

被引:54
|
作者
Parlett, Christopher M. A. [1 ]
Keshwalla, Pooja [1 ]
Wainwright, Stephen G. [2 ]
Bruce, Duncan W. [2 ]
Hondow, Nicole S. [3 ]
Wilson, Karen [1 ]
Lee, Adam F. [1 ]
机构
[1] Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Cardiff CF10 3AT, S Glam, Wales
[2] Univ York, Dept Chem, York YO10 4PF, N Yorkshire, England
[3] Univ Leeds, Inst Mat Res, Leeds LS2 9JT, W Yorkshire, England
来源
ACS CATALYSIS | 2013年 / 3卷 / 09期
基金
英国工程与自然科学研究理事会;
关键词
palladium; selective oxidation; alcohol; hierarchical; macroporous; mesoporous; SBA-15; LIQUID-PHASE OXIDATION; SUPERCRITICAL CARBON-DIOXIDE; MOLECULAR-OXYGEN; CROTYL ALCOHOL; PALLADIUM NANOPARTICLES; SUPPORTED PALLADIUM; PD NANOPARTICLES; SILICA; SURFACE; DESIGN;
D O I
10.1021/cs400371a
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 utility of a hierarchically ordered nanoporous SBA-15 architecture, comprising 270 nm macropores and 5 nm mesopores (MM-SBA-15), for the catalytic aerobic selective oxidation of sterically challenging allylic alcohols is shown. Detailed bulk and surface characterization reveals that incorporation of complementary macropores into mesoporous SBA-15 enhances the dispersion of sub 2 nm Pd nanoparticles and thus their degree of surface oxidation. Kinetic profiling reveals a relationship between nanoparticle dispersion and oxidation rate, identifying surface PdO as the catalytically active phase. Hierarchical nanoporous Pd/MM-SBA-15 outperforms mesoporous analogues in allylic alcohol selective oxidation by (i) stabilizing PdO nanoparticles and (ii) dramatically improving in-pore diffusion and access to active sites by sesquiterpenoid substrates such as farnesol and phytol.
引用
收藏
页码:2122 / 2129
页数:8
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