Department of Chemistry, York University, Toronto, ON M3J 1P3, Canada.
Phys Chem Chem Phys. 2012 Sep 21;14(35):12122-9. doi: 10.1039/c2cp41286a. Epub 2012 Jul 30.
CO oxidation on Pt nanoclusters of approximately 1 nm in size was studied using density functional theory (DFT). Reaction barriers on various sites of a cuboctahedral 55-atom cluster and of several two-layer plane clusters representing (111) and (100) facets of the 147-atom cluster have been calculated at various coverage. The effect of atomic structure of various clusters was discussed. It was concluded that the 147-atom cuboctahedral cluster reveals properties of the Pt single crystal surfaces, while a 55-atom cluster cannot be fully described in terms of Pt single crystal surfaces. It was found that CO oxidation may occur faster at higher coverage and that for cluster sizes up to a few nanometers in size, larger platinum clusters can be more efficient in CO oxidation than the smaller clusters. The size effect was found to depend upon coverage.
使用密度泛函理论（DFT）研究了尺寸约为 1nm 的 Pt 纳米团簇上的 CO 氧化。在不同的覆盖率下，计算了具有不同原子结构的 55-原子的立方八面体团簇和几个代表 147-原子团簇的（111）和（100）面的双层平面团簇在各个位点上的反应势垒。讨论了各种团簇原子结构的影响。结果表明，147-原子的立方八面体团簇显示出 Pt 单晶表面的性质，而 55-原子的团簇不能完全用 Pt 单晶表面来描述。结果发现，CO 氧化在较高的覆盖率下可能会更快发生，并且对于尺寸在几纳米大小的团簇，较大的铂团簇在 CO 氧化方面可能比较小的团簇更有效。发现尺寸效应取决于覆盖率。
