Structure and reactivity of Ru nanoparticles supported on modified graphite surfaces: A study of the model catalysts for ammonia synthesis

被引:116
作者
Song, Z [1 ]
Cai, TH [1 ]
Hanson, JC [1 ]
Rodriguez, JA [1 ]
Hrbek, J [1 ]
机构
[1] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA
关键词
D O I
10.1021/ja031718s
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Supported ruthenium metal catalysts have higher activity than traditional iron-based catalysts used industrially for ammonia synthesis. A study of a model Ru/C catalyst was carried out to advance the understanding of structure and reactivity correlations in this structure-sensitive reaction where dinitrogen dissociation is the rate-limiting step. Ru particles were grown by chemical vapor deposition (CVD) via a Ru-3(CO)(12) precursor on a highly oriented pyrolytic graphite (HOPG) surface modified with one-atomic-layer-deep holes mimicking activated carbon support. Scanning tunneling microscopy (STM) has been used to investigate the growth, structure, and morphology of the Ru particles. Thermal desorption of dissociatively adsorbed nitrogen has been used to evaluate the reactivity of the Ru/HOPG model catalysts. Two different Ru particle structures with different reactivities to N-2 dissociation have been identified. The initial sticking coefficient for N2 dissociative adsorption on the Ru/HOPG model catalysts is similar to10(-6), 4 orders larger compared to that of Ru single-crystal surfaces.
引用
收藏
页码:8576 / 8584
页数:9
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