Electron Spin Resonance Study on γ-Ray-Induced Methyl Radicals in Methane Hydrates

Takeya, Kei; Nango, Kouhei; Sugahara, Takeshi; Ohgaki, Kazunari; Tani, Atsushi; Ito, H.; Okada, Michio; Kasai, Toshio

doi:10.1143/jjap.43.353

Cited by 25 publications

(40 citation statements)

References 14 publications

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“…These values are in agreement with the literature [10,11]. Other than isobutyl and tert-butyl radicals, the signals of H and D atoms were also observed at 120 K. OD radicals were not observed even at 77 K, which is consistent with the previous reports on the γ-ray-irradiated methane [1], ethane [3], and propane [4] hydrates. To quantify the amounts of each butyl radical, the ESR spectrum was deconvoluted based on the ESR parameters determined at each temperature.…”

Section: Esr Spectrum Of Induced Radicalssupporting

confidence: 93%

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Intermolecular Hydrogen Transfer in Isobutane Hydrate

et al. 2012

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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.

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Section: Esr Spectrum Of Induced Radicalssupporting

confidence: 93%

“…We have reported the thermal stabilities of methyl, ethyl, and propyl radicals in the γ-ray-irradiated simple methane [1,2], ethane [3], and propane [4] hydrate systems. The radicals in other clathrate hydrates have been investigated [5][6][7].…”

Section: Introductionmentioning

confidence: 99%

Intermolecular Hydrogen Transfer in Isobutane Hydrate

et al. 2012

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“…3) was evaluated as the signal intensity in this paper because the difference of the spectrum shapes for all measurements was negligible. Although an unidentified signal at g = 2.0014 was reported by Takeya et al (2004), it was not observed in this sample. This signal may be caused by some impurities.…”

Section: Resultscontrasting

confidence: 53%

“…5 because Takeya et al (2004) mentioned that the radical decayed according to a second order decay model through the dimerization process to form ethane (see Appendix). Fig.…”

Section: Resultsmentioning

confidence: 99%

“…In our previous study, synthetic methane hydrate irradiated by -rays at 77 K was measured by electron spin resonance (ESR) to identify radiation-induced radicals and reveal their thermal stability at atmospheric pressure (Takeya et al, 2004). The methyl radical was the most thermally stable and decayed at around 200 K, close to the dissociation temperature of methane hydrate at atmospheric pressure (Sloan, 1998).…”

Section: Introductionmentioning

confidence: 99%

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Thermal stability of methyl radical in γ-ray irradiated methane hydrate under different pressure from 0.003 to 1 MPa

Tani

Ishikawa

Takeya

2006

Radiation Measurements

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Clathrate Hydrates as a Kind of Promising Ice Nanoreactors

Chang,

Cheng,

2024

Chemistry A European J

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Since their discovery, clathrate hydrates (CHs) have received great attention both from theoretical and experimental aspects due to their great potential for gas storage and prospective applications as icy crystal materials. However, there has been limited research on the decomposition, reduction or other reactions of gases enclosed in CHs. Thanks to their unique hydrogen bonding network and cavity structures, CHs can serve as the promising nanoreactors to achieve chemical conversions, e.g. reducing greenhouse gases. In this review‐type article, we characterize the potential performance of such CHs nanoreactors by discussing their multiple functions including important roles of hydrogen bonds in CHs, e.g. the confinement effect and proton source, and then discuss the enhanced electron‐binding ability of guest molecules and the structures and properties of trapped electrons in the stacked nanocages, which contribute to our understanding of chemical reactions occurring in CHs. Finally, we provide detailed analyses of representative reaction mechanisms underwent in CH nanoreactors and effective investigation methods. This review‐type article aims to provide a detailed summary about the functional characteristics of CHs and reactivity in CHs, which make CHs a kind of promising icy nanoreactors.

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Electron Spin Resonance Study on γ-Ray-Induced Methyl Radicals in Methane Hydrates

Cited by 25 publications

References 14 publications

Intermolecular Hydrogen Transfer in Isobutane Hydrate

Intermolecular Hydrogen Transfer in Isobutane Hydrate

Thermal stability of methyl radical in γ-ray irradiated methane hydrate under different pressure from 0.003 to 1 MPa

Clathrate Hydrates as a Kind of Promising Ice Nanoreactors

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