Size- and charge-state-dependent reactivity of azidoacetonitrile with anionic and cationic rhodium clusters Rhn±

Iulia Balteanu, O. Petru Balaj, Brigitte S. Fox-Beyer, Paula Rodrigues, Maria Teresa Barros, Augusto M.C. Moutinho, Maria de Lourdes S. L. Costa, Martin K. Beyer, Vladimir E. Bondybey

Research output: Contribution to journalArticle

17 Citations (Scopus)

Abstract

Gas-phase reactions of anionic and cationic rhodium clusters with azidoacetonitrile are studied by Fourier transform ion cyclotron resonance (FT-ICR) mass spectrometry under near-thermal conditions. All anionic and large cationic clusters react by adding [C2,N2] in consecutive steps, either by forming interstitial carbides and nitrides or by adding two CN groups to the cluster surface. Small cationic clusters behave differently, with the unimolecular decomposition of the azide determining the reactivity. Saturation is identified via the size-dependent efficiency of consecutive reaction steps. The present results are the first study of organic azides on transition metal clusters. The observed selectivity of the reaction is in contrast to the high exothermicity of any reaction with azide species. The cationic cluster reactivity shows a gradual transition from gas-phase to surface-like behavior with increasing cluster size.

Original languageEnglish
Pages (from-to)1978-1985
Number of pages8
JournalOrganometallics
Volume23
Issue number9
DOIs
Publication statusPublished - 26 Apr 2004

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