Catalytic and Magnetic Behaviors of Excessively Charged Silver, Copper, Platinum, and Rhodium Atomic Clusters

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• 作者：Shideh Ahmadi ; Xi Zhang ; Yinyan Gong ; Weiguang Zhu ; Chang Q. Sun
• 刊名：Journal of Physical Chemistry C
• 出版年：2016
• 出版时间：August 11, 2016
• 年：2016
• 卷：120
• 期：31
• 页码：17527-17536
• 全文大小：778K
• 年卷期：0
• ISSN：1932-7455

文摘

Spin-resolved density functional theory examination revealed that 0, ±1e, and ±2e additional surface charge has impact to the bond-electron-energy relaxation, and the associated catalystic and magnetic properties of M_N atomic clusters (M = Ag, Cu, Pt, and Rh; N = 13–147 atoms). Trends consistency between calculations and experimental observations confirmed our predictions [ Chem. Rev. 2015, 115, 6746] that the shorter-and-stronger bonds between undercoordinated atoms induce the local densification and quantum entrapment of the core electrons, which in turn polarize the valence electrons dominating the catalytic and magnetic performance of the clusters. The excessive charge states has an important impact to the magnetization of M_N. Specifically, even excessive charge states addition induces magnetization of all the M_N clusters while odd excessive charge addition affects only Pt and Rh clusters. Observations provide insight on the relationship between excessive charge and the intrinsic effect of the atomic undercoordination on the catalytic and magnetic properties of M_N nanoclusters.