Journal
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
Volume -, Issue 10, Pages 1516-1521Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/ejic.200901126
Keywords
Main-group elements; Ammonia; N-H bond activation; Reactivity pattern; Gas-phase ion chemistry
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Funding
- National Research Council (Canada)
- Natural Science and Engineering Research Council (Canada)
- MDS Analytical Technologies
- Fonds der Chemischen Industrie
- Deutsche Forschungsgemeinschaft (DFG)
- Alexander von Humboldt-Stiftung
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The activation of ammonia by the main-group cations Gat Ge+, As+ and Se+ has been explored both experimentally and theoretically. ICP/SIFT tandem mass spectrometer measurements of room-temperature kinetics have revealed a substantial variation in rates and product distributions across the Periodic Table of Elements. The main features of the observed primary chemistry include H-atom elimination, ammonia addition and a cation-assisted proton transfer to yield NH4+ that is second order in ammonia. These observations are shown to be completely consistent with computed potential energy surfaces for the reactions of each of the four atomic cations. Dehydrogenation by the elimination of molecular hydrogen, not observed experimentally, is shown by the calculations to be inhibited by the presence of a kinetic barrier.
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