期刊
INTERNATIONAL JOURNAL OF MASS SPECTROMETRY
卷 254, 期 3, 页码 183-188出版社
ELSEVIER SCIENCE BV
DOI: 10.1016/j.ijms.2006.06.003
关键词
catalysis platinum; C-H activation; methane; dehydrogenation kinetics
Bimolecular reactions of cationic platinum clusters Pt-n(+), n = 1-24, and anionic platinum clusters Pt-n(-), n = 3-22, with CH4 and CD4 are studied under low pressure conditions in an FT-ICR mass spectrometer, using an isotopically enriched Pt-195 sample. Strongly size-dependent dehydrogenation and formation of PtnCH2+/- is observed for both charge states. Starting with n = 12, cationic clusters also afford stabilization of a [Pt-n, CH4](+) adduct, presumably the HPtnCH3+ insertion compound. Deuteration shifts the lower limit for adduct formation to n = 8. It is suggested that the strong reactivity fluctuations over a wide size range are the gas phase fingerprint of a good heterogeneous catalyst material. (C) 2006 Elsevier B.V. All rights reserved.
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