Shape- and Size-Specific Chemistry of Ag Nanostructures in Catalytic Ethylene Epoxidation

被引:203
作者
Christopher, Phillip [1 ]
Linic, Suljo [1 ]
机构
[1] Univ Michigan, Dept Chem Engn, Ann Arbor, MI 48109 USA
基金
美国国家科学基金会;
关键词
epoxidation; heterogeneous catalysis; nanomaterials; selectivity; silver; HETEROGENEOUS CATALYSIS; SILVER NANOPARTICLES; SURFACE-CHEMISTRY; DFT CALCULATIONS; POLYOL SYNTHESIS; SELECTIVITY; NANOWIRES; AG(111); MORPHOLOGY; PARTICLES;
D O I
10.1002/cctc.200900231
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
Catalytic selectivity in the epoxidation of ethylene to form ethylene oxide on alumina-supported silver catalysts is dependent on the geometric structure of catalytically active Ag particles and reaction conditions. Shape and size controlled synthesis of Ag nanoparticles is used to show that silver nanocubes exhibit higher selectivity than nanowires and nanospheres. For a given shape, larger particles offer improved selectivity. The enhanced selectivity toward ethylene oxide is attributed to the nature of the exposed Ag surface facets; Ag nanocubes and nanowires are dominated by (100) surface facet and Ag nanospheres are dominated by (111). Furthermore, the concentration of under-coordinated surface sites is related to diminished selectivity to ethylene oxide., We demonstrate, that a simple model can account for the impact of chemical and physical factors, on, the reaction selectivity. These observations have also been used, to design a selective catalyst for the ethylene epoxidation reaction.
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页码:78 / 83
页数:6
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