Synthesis, characterization, and testing of supported Au catalysts prepared from atomically-tailored Au38(SC12H25)24 clusters

被引:71
作者
Gaur, Sarthak [1 ]
Miller, Jeffrey T. [2 ]
Stellwagen, Daniel [3 ]
Sanampudi, Ashwin [1 ]
Kumar, Challa S. S. R. [4 ]
Spivey, James J. [1 ]
机构
[1] Louisiana State Univ, Cain Dept Chem Engn, Baton Rouge, LA 70820 USA
[2] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA
[3] Univ Utrecht, Debye Inst Nanomat Sci, NL-3584 CG Utrecht, Netherlands
[4] J Bennett Johnston Sr Ctr Adv Microstruct & Devic, Baton Rouge, LA 70806 USA
关键词
MONOLAYER-PROTECTED CLUSTERS; SELF-ASSEMBLED MONOLAYERS; TEMPERATURE CO OXIDATION; GOLD NANOPARTICLES; AU/TIO2; CATALYSTS; INFRARED-SPECTROSCOPY; ELECTRON-MICROSCOPY; CARBON-MONOXIDE; PARTICLE-SIZE; TIO2;
D O I
10.1039/c1cp22438g
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
Nearly monodispersed Au-38(SC12H25)(24) clusters (1.7 +/- 0.2 nm) were synthesized using a modified Brust process while utilizing a "thiol etching'' approach for the ligand exchange. HRTEM, MALDI, FTIR, and XAS analysis confirmed the formation of the 38-atom clusters in solution. This solution was used to impregnate a microporous TiO2 support to give 0.7% Au-38/TiO2 catalyst. Subsequent drying in air and treatment with H-2/He at 400 degrees C removed most of the sulfur ligands, and also increased the Au cluster size to 3.9 +/- 0.96 nm. XPS and EXAFS analysis of this supported catalyst showed trace levels of residual sulfides, apparently located at the Au-TiO2 interface. CO oxidation tests on these supported clusters show an activation energy and range of TOFs comparable to those reported by others. These results suggest that supported Au clusters of controllable size can be prepared with this thiol-ligated solution-based method, providing a new approach to the synthesis of these catalysts.
引用
收藏
页码:1627 / 1634
页数:8
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