Intermolecular Hydrogen Transfer in Isobutane HydrateReport as inadecuate


Intermolecular Hydrogen Transfer in Isobutane Hydrate


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1

Division of Chemical Engineering, Graduate School of Engineering Science, Osaka University, 1-3 Machikaneyama, Toyonaka, Osaka 560-8531, Japan

2

Department of Earth and Space Science, Graduate School of Science, Osaka University, 1-1 Machikaneyama, Toyonaka, Osaka 560-0043, Japan

3

Department of Electrical and Electronic Engineering and Information Engineering, Graduate School of Engineering, Nagoya University, Furo, Chikusa-ku, Nagoya, Aichi 464-8603, Japan





*

Author to whom correspondence should be addressed.



Abstract Electron spin resonance ESR spectra of butyl radicals induced with γ-ray irradiation in the simple isobutane 2-methylpropane hydrate prepared with deuterated water were investigated. Isothermal annealing results of the γ-ray-irradiated isobutane hydrate reveal that the isobutyl radical in a large cage withdraws a hydrogen atom from the isobutane molecule through shared hexagonal-faces of adjacent large cages. During this -hydrogen picking- process, the isobutyl radical is apparently transformed into a tert-butyl radical, while the sum of isobutyl and tert-butyl radicals remains constant. The apparent transformation from isobutyl to tert-butyl radicals is an irreversible first-order reaction and the activation energy was estimated to be 35 ± 3 kJ-mol, which was in agreement with the activation energy 39 ± 5 kJ-mol of hydrogen picking in the γ-ray-irradiated propane hydrate with deuterated water. View Full-Text

Keywords: hydrogen abstraction; clathrate hydrate; radical; electron spin resonance; activation energy hydrogen abstraction; clathrate hydrate; radical; electron spin resonance; activation energy





Author: Naohiro Kobayashi 1, Takashi Minami 1, Atsushi Tani 2, Mikio Nakagoshi 1, Takeshi Sugahara 1, Kei Takeya 3 and Kazunari Ohgaki 1,*

Source: http://mdpi.com/



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