Intermolecular Hydrogen Transfer in Isobutane Hydrate

Naohiro Kobayashi, Takashi Minami, Atsushi Tani, Mikio Nakagoshi, Takeshi Sugahara, Kei Takeya and Kazunari Ohgaki
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Naohiro Kobayashi: Division of Chemical Engineering, Graduate School of Engineering Science, Osaka University, 1-3 Machikaneyama, Toyonaka, Osaka 560-8531, Japan
Takashi Minami: Division of Chemical Engineering, Graduate School of Engineering Science, Osaka University, 1-3 Machikaneyama, Toyonaka, Osaka 560-8531, Japan
Atsushi Tani: Department of Earth and Space Science, Graduate School of Science, Osaka University, 1-1 Machikaneyama, Toyonaka, Osaka 560-0043, Japan
Mikio Nakagoshi: Division of Chemical Engineering, Graduate School of Engineering Science, Osaka University, 1-3 Machikaneyama, Toyonaka, Osaka 560-8531, Japan
Takeshi Sugahara: Division of Chemical Engineering, Graduate School of Engineering Science, Osaka University, 1-3 Machikaneyama, Toyonaka, Osaka 560-8531, Japan
Kei Takeya: Department of Electrical and Electronic Engineering and Information Engineering, Graduate School of Engineering, Nagoya University, Furo, Chikusa-ku, Nagoya, Aichi 464-8603, Japan
Kazunari Ohgaki: Division of Chemical Engineering, Graduate School of Engineering Science, Osaka University, 1-3 Machikaneyama, Toyonaka, Osaka 560-8531, Japan

Energies, 2012, vol. 5, issue 6, 1-8

Abstract: Electron spin resonance (ESR) spectra of butyl radicals induced with ?-ray irradiation in the simple isobutane (2-methylpropane) hydrate (prepared with deuterated water) were investigated. Isothermal annealing results of the ?-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 ?-ray-irradiated propane hydrate with deuterated water.

Keywords: hydrogen abstraction; clathrate hydrate; radical; electron spin resonance; activation energy (search for similar items in EconPapers)
JEL-codes: Q Q0 Q4 Q40 Q41 Q42 Q43 Q47 Q48 Q49 (search for similar items in EconPapers)
Date: 2012
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