Efficient Room‐Temperature Methane Activation by the Closed‐Shell, Metal‐Free Cluster [OSiOH] + : A Novel Mechanistic Variant | Zendy

Sun Xiaoyan | Zendy; Zhou Shaodong | Zendy; Schlangen Maria | Zendy; Schwarz Helmut | Zendy

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Efficient Room‐Temperature Methane Activation by the Closed‐Shell, Metal‐Free Cluster [OSiOH] + : A Novel Mechanistic Variant

Author(s) -

Sun Xiaoyan,

Zhou Shaodong,

Schlangen Maria,

Schwarz Helmut

Publication year - 2016

Publication title -

chemistry – a european journal

Language(s) - English

Resource type - Journals

SCImago Journal Rank - 1.687

H-Index - 242

eISSN - 1521-3765

pISSN - 0947-6539

DOI - 10.1002/chem.201601981

Subject(s) - reactivity (psychology) , chemistry , fourier transform ion cyclotron resonance , cluster (spacecraft) , methane , mass spectrometry , shell (structure) , ion , methanol , metal , open shell , analytical chemistry (journal) , organic chemistry , materials science , medicine , alternative medicine , pathology , chromatography , computer science , composite material , programming language

The closed‐shell cluster ion [OSiOH] + is generated in the gas phase and its reactivity towards the thermal activation of CH 4 has been examined using Fourier transform‐ion cyclotron resonance (FT‐ICR) mass spectrometry in conjunction with state‐of‐the‐art quantum chemical calculations. Quite unexpectedly at room temperature, [OSiOH] + efficiently mediates C−H bond activation, giving rise to [SiOH] + and [SiOCH 3 ] + with the concomitant formation of methanol and water, respectively. Mechanistic aspects for this unprecedented reactivity pattern are presented, and the properties of the [OSiOH] + /CH 4 couple are compared with those of the closed‐shell systems [OCOH] + /CH 4 and [MgOH] + /CH 4 ; the last two couples exhibit an entirely different reactivity scenario.

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