Gas-phase synthesis and characterization of CH4-loaded hydroquinone clathrates

Jong Won Lee, Yongjae Lee, Satoshi Takeya, Taro Kawamura, Yoshitaka Yamamoto, Yun Je Lee, Ji Ho Yoon

Research output: Contribution to journalArticle

27 Citations (Scopus)

Abstract

A CH4-loaded hydroquinone (HQ) clathrate was synthesized via a gas-phase reaction using the a-form of crystalline HQ and CH4 gas at 12 MPa and room temperature. Solid-state 13C cross-polarization/magic angle spinning (CP/MAS) NMR and Raman spectroscopic measurements confirm the incorporation of CH4 molecules into the cages of the HQ clathrate framework. The chemical analysis indicates that about 69% of the cages are filled by CH4 molecules, that is, 0.69 CH4 per three HQ molecules. Rietveld refinement using synchrotron X-ray powder diffraction (XRD) data shows that the CH4-loaded HQ clathrate adopts the /3-form of HQ clathrate in a hexagonal space group R3 with lattice paramet ers of a = 16.6191 Å and c = 5.5038 Å. Timeresolved synchrotron XRD and quadrupole mass spectroscopic measurements show that the CH4-loaded HQ clathrate is stable up to 368 K and gradually transforms to the a-form by releasing the confined CH4 gases between 368-378 K. Using solid-state 13C CP/MAS NMR, the reaction kinetics between the a-form HQ and CH4 gas is qualitatively described in terms of the particle size of the crystalline HQ,

Original languageEnglish
Pages (from-to)3254-3258
Number of pages5
JournalJournal of Physical Chemistry B
Volume114
Issue number9
DOIs
Publication statusPublished - 2010 Mar 11

Fingerprint

clathrates
Gases
vapor phases
Magic angle spinning
synthesis
Synchrotrons
X ray powder diffraction
Molecules
cross polarization
metal spinning
Nuclear magnetic resonance
Polarization
Crystalline materials
synchrotrons
Rietveld refinement
gases
solid state
molecules
nuclear magnetic resonance
Reaction kinetics

All Science Journal Classification (ASJC) codes

  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films
  • Materials Chemistry

Cite this

Lee, J. W., Lee, Y., Takeya, S., Kawamura, T., Yamamoto, Y., Lee, Y. J., & Yoon, J. H. (2010). Gas-phase synthesis and characterization of CH4-loaded hydroquinone clathrates. Journal of Physical Chemistry B, 114(9), 3254-3258. https://doi.org/10.1021/jp911822e
Lee, Jong Won ; Lee, Yongjae ; Takeya, Satoshi ; Kawamura, Taro ; Yamamoto, Yoshitaka ; Lee, Yun Je ; Yoon, Ji Ho. / Gas-phase synthesis and characterization of CH4-loaded hydroquinone clathrates. In: Journal of Physical Chemistry B. 2010 ; Vol. 114, No. 9. pp. 3254-3258.
@article{07f40a248580406783d3671d566f4dcb,
title = "Gas-phase synthesis and characterization of CH4-loaded hydroquinone clathrates",
abstract = "A CH4-loaded hydroquinone (HQ) clathrate was synthesized via a gas-phase reaction using the a-form of crystalline HQ and CH4 gas at 12 MPa and room temperature. Solid-state 13C cross-polarization/magic angle spinning (CP/MAS) NMR and Raman spectroscopic measurements confirm the incorporation of CH4 molecules into the cages of the HQ clathrate framework. The chemical analysis indicates that about 69{\%} of the cages are filled by CH4 molecules, that is, 0.69 CH4 per three HQ molecules. Rietveld refinement using synchrotron X-ray powder diffraction (XRD) data shows that the CH4-loaded HQ clathrate adopts the /3-form of HQ clathrate in a hexagonal space group R3 with lattice paramet ers of a = 16.6191 {\AA} and c = 5.5038 {\AA}. Timeresolved synchrotron XRD and quadrupole mass spectroscopic measurements show that the CH4-loaded HQ clathrate is stable up to 368 K and gradually transforms to the a-form by releasing the confined CH4 gases between 368-378 K. Using solid-state 13C CP/MAS NMR, the reaction kinetics between the a-form HQ and CH4 gas is qualitatively described in terms of the particle size of the crystalline HQ,",
author = "Lee, {Jong Won} and Yongjae Lee and Satoshi Takeya and Taro Kawamura and Yoshitaka Yamamoto and Lee, {Yun Je} and Yoon, {Ji Ho}",
year = "2010",
month = "3",
day = "11",
doi = "10.1021/jp911822e",
language = "English",
volume = "114",
pages = "3254--3258",
journal = "Journal of Physical Chemistry B Materials",
issn = "1520-6106",
publisher = "American Chemical Society",
number = "9",

}

Lee, JW, Lee, Y, Takeya, S, Kawamura, T, Yamamoto, Y, Lee, YJ & Yoon, JH 2010, 'Gas-phase synthesis and characterization of CH4-loaded hydroquinone clathrates', Journal of Physical Chemistry B, vol. 114, no. 9, pp. 3254-3258. https://doi.org/10.1021/jp911822e

Gas-phase synthesis and characterization of CH4-loaded hydroquinone clathrates. / Lee, Jong Won; Lee, Yongjae; Takeya, Satoshi; Kawamura, Taro; Yamamoto, Yoshitaka; Lee, Yun Je; Yoon, Ji Ho.

In: Journal of Physical Chemistry B, Vol. 114, No. 9, 11.03.2010, p. 3254-3258.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Gas-phase synthesis and characterization of CH4-loaded hydroquinone clathrates

AU - Lee, Jong Won

AU - Lee, Yongjae

AU - Takeya, Satoshi

AU - Kawamura, Taro

AU - Yamamoto, Yoshitaka

AU - Lee, Yun Je

AU - Yoon, Ji Ho

PY - 2010/3/11

Y1 - 2010/3/11

N2 - A CH4-loaded hydroquinone (HQ) clathrate was synthesized via a gas-phase reaction using the a-form of crystalline HQ and CH4 gas at 12 MPa and room temperature. Solid-state 13C cross-polarization/magic angle spinning (CP/MAS) NMR and Raman spectroscopic measurements confirm the incorporation of CH4 molecules into the cages of the HQ clathrate framework. The chemical analysis indicates that about 69% of the cages are filled by CH4 molecules, that is, 0.69 CH4 per three HQ molecules. Rietveld refinement using synchrotron X-ray powder diffraction (XRD) data shows that the CH4-loaded HQ clathrate adopts the /3-form of HQ clathrate in a hexagonal space group R3 with lattice paramet ers of a = 16.6191 Å and c = 5.5038 Å. Timeresolved synchrotron XRD and quadrupole mass spectroscopic measurements show that the CH4-loaded HQ clathrate is stable up to 368 K and gradually transforms to the a-form by releasing the confined CH4 gases between 368-378 K. Using solid-state 13C CP/MAS NMR, the reaction kinetics between the a-form HQ and CH4 gas is qualitatively described in terms of the particle size of the crystalline HQ,

AB - A CH4-loaded hydroquinone (HQ) clathrate was synthesized via a gas-phase reaction using the a-form of crystalline HQ and CH4 gas at 12 MPa and room temperature. Solid-state 13C cross-polarization/magic angle spinning (CP/MAS) NMR and Raman spectroscopic measurements confirm the incorporation of CH4 molecules into the cages of the HQ clathrate framework. The chemical analysis indicates that about 69% of the cages are filled by CH4 molecules, that is, 0.69 CH4 per three HQ molecules. Rietveld refinement using synchrotron X-ray powder diffraction (XRD) data shows that the CH4-loaded HQ clathrate adopts the /3-form of HQ clathrate in a hexagonal space group R3 with lattice paramet ers of a = 16.6191 Å and c = 5.5038 Å. Timeresolved synchrotron XRD and quadrupole mass spectroscopic measurements show that the CH4-loaded HQ clathrate is stable up to 368 K and gradually transforms to the a-form by releasing the confined CH4 gases between 368-378 K. Using solid-state 13C CP/MAS NMR, the reaction kinetics between the a-form HQ and CH4 gas is qualitatively described in terms of the particle size of the crystalline HQ,

UR - http://www.scopus.com/inward/record.url?scp=77749344543&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=77749344543&partnerID=8YFLogxK

U2 - 10.1021/jp911822e

DO - 10.1021/jp911822e

M3 - Article

VL - 114

SP - 3254

EP - 3258

JO - Journal of Physical Chemistry B Materials

JF - Journal of Physical Chemistry B Materials

SN - 1520-6106

IS - 9

ER -