論文

査読有り
2016年2月

Reactivity Control of Rhodium Cluster Ions by Alloying with Tantalum Atoms

JOURNAL OF PHYSICAL CHEMISTRY A
  • Fumitaka Mafune
  • ,
  • Yuki Tawaraya
  • ,
  • Satoshi Kudoh

120
6
開始ページ
861
終了ページ
867
記述言語
英語
掲載種別
研究論文(学術雑誌)
DOI
10.1021/acs.jpca.5b11898
出版者・発行元
AMER CHEMICAL SOC

Gas phase, bielement rhodium and tantalum clusters, RhnTam+ (n + m = 6), were prepared by the double laser ablation of Rh and Ta rods in He carrier gas. The clusters were introduced into a reaction gas cell filled with nitric oxide (NO) diluted with He and were subjected to collisions with NO and He at room temperature. The product species were observed by mass spectrometry, demonstrating that the NO molecules were sequentially adsorbed on the RhnTam+ clusters to form RhnTam+NxOx (x = 1, 2, 3, ...) species. In addition, oxide clusters, RhnTam+O2, were also observed, suggesting that the NO molecules were dissociatively adsorbed on the cluster, the N atoms migrated on the surface to form N-2, and the N-2 molecules were released from RhnTam+N2O2. The reactivity, leading to oxide formation, was composition dependent: oxide clusters were dominantly formed for the bielement clusters containing both Rh and Ta atoms, whereas such clusters were hardly formed for the single-element Rh(n)(+)and Ta-m(+) clusters. DFT calculations indicated that the Ta atoms induce dissociation of NO on the clusters by lowering the dissociation energy, whereas the Rh atoms enable release of N-2 by lowering the binding energy of the N atoms on the clusters.

Web of Science ® 被引用回数 : 12

リンク情報
DOI
https://doi.org/10.1021/acs.jpca.5b11898
Web of Science
https://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcAuth=JSTA_CEL&SrcApp=J_Gate_JST&DestLinkType=FullRecord&KeyUT=WOS:000370678600002&DestApp=WOS_CPL