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Three-dimensional behavior analysis of stable and metastable structures of clathrate hydrates

Research Project

Project/Area Number 20K05440
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Review Section Basic Section 32010:Fundamental physical chemistry-related
Research InstitutionNational Institute of Advanced Industrial Science and Technology

Principal Investigator

Takeya Satoshi  国立研究開発法人産業技術総合研究所, 計量標準総合センター, 研究グループ 付 (40357421)

Project Period (FY) 2020-04-01 – 2023-03-31
Project Status Completed (Fiscal Year 2022)
Budget Amount *help
¥4,290,000 (Direct Cost: ¥3,300,000、Indirect Cost: ¥990,000)
Fiscal Year 2022: ¥1,040,000 (Direct Cost: ¥800,000、Indirect Cost: ¥240,000)
Fiscal Year 2021: ¥1,560,000 (Direct Cost: ¥1,200,000、Indirect Cost: ¥360,000)
Fiscal Year 2020: ¥1,690,000 (Direct Cost: ¥1,300,000、Indirect Cost: ¥390,000)
KeywordsTBAB / セミクラスレート / ガスハイドレート / 構造解析 / X線CT / X線CT / クラスレート / 可視化 / 結晶構造解析
Outline of Research at the Start

本研究では、クラスレートハイドレート(ハイドレート)を研究対象とし、準安定相の発現メカニズムの解明を目的としている。ハイドレートが氷や水溶液と共存する三次元状態の可視化を行い、水和数の違いによる結晶構造の違いを僅かな密度の差から検出する。マクロスケールでの位相コントラストX線CT測定を実施し、粉末X線結晶構造解析により得られる安定相の密度を基準に、ハイドレートの安定相・準安定相、さらには水(液体もしくは固体)の三次元密度分布解析を実施する。得られた密度情報から、準安定相の構造について考察するとともに、安定相・準安定相の発現メカニズムを明らかにする。

Outline of Final Research Achievements

The density difference between hydrate and ice or water is miniscule, and it is difficult to distinguish hydrate from water or ice using conventional X-ray CT measurements. In this study, we succeeded in nondestructive observation of TBAB hydrate coexisting with ice by the phase contrast method using 35 keV synchrotron radiation monochromatic X-rays and the absorption contrast method. Comparison based on gray contrast of X-ray CT with reference to ice crystals enabled verification of the distribution inside the sample of TBAB hydrate with a hydration number of 38, for which the crystal structure is known. In addition, optimization of the measurement and analysis methods was carried out for density comparison and density analysis analysis of the internal structure by X-ray CT.

Academic Significance and Societal Importance of the Research Achievements

本研究で実現したハイドレートの評価手法は、ハイドレートや氷以外の等の物質にも応用可能なものである。例えば、環境・エネルギー分野に貢献する低環境負荷な材料が求められ、水素・炭素・窒素・酸素などの軽元素で構成される軽元素材料の需要が高まっている。新規材料の製品への利用のためには、材料の構造・形態と物性の相関の理解が求められている。このため、三次元構造の定量解析が重要で、三次元イメージング手法に対する計測ニーズが高まっている。密度差の小さな樹脂などの高分子材料等、様々な三次元計測への応用も可能で、社会的な意義が高く波及効果は大きいといえる。

Report

(4 results)
  • 2022 Annual Research Report   Final Research Report ( PDF )
  • 2021 Research-status Report
  • 2020 Research-status Report
  • Research Products

    (18 results)

All 2023 2022 2021 2020

All Journal Article (10 results) (of which Int'l Joint Research: 1 results,  Peer Reviewed: 10 results) Presentation (8 results) (of which Int'l Joint Research: 1 results,  Invited: 1 results)

  • [Journal Article] Thermally Induced Phase Transition of Cubic Structure II Hydrate: Crystal Structures of Tetrahydropyran-CO2 Binary Hydrate2023

    • Author(s)
      Takeya Satoshi、Fujihisa Hiroshi、Alavi Saman、Ohmura Ryo
    • Journal Title

      The Journal of Physical Chemistry Letters

      Volume: 14 Issue: 7 Pages: 1885-1891

    • DOI

      10.1021/acs.jpclett.2c03392

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Dissociation Kinetics and Metastability of Carbon Monoxide Hydrates Correlating with Phase Change in Water Ice2022

    • Author(s)
      Takeya Satoshi、Yahagi Daisuke、Hachikubo Akihiro
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 126 Issue: 30 Pages: 12391-12398

    • DOI

      10.1021/acs.jpcc.2c03673

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] X-ray Imaging of Clathrate Hydrates as Gas Storage Materials: Absorption Contrast of Low-Density and Low-Absorption Materials Using Energy-Dependent X-ray Computed Tomography2022

    • Author(s)
      Takeya Satoshi、Muromachi Sanehiro、Yoneyama Akio
    • Journal Title

      Energy & Fuels

      Volume: 36 Issue: 18 Pages: 10659-10666

    • DOI

      10.1021/acs.energyfuels.2c01319

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Transformation process of ice crystallized from a glassy dilute trehalose aqueous solution2022

    • Author(s)
      Suzuki Yoshiharu、Takeya Satoshi
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 24 Issue: 43 Pages: 26659-26667

    • DOI

      10.1039/d2cp02712g

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Crystal Structure and Guest Distribution of N2O Hydrate Determined by Powder X-ray Diffraction Measurements2022

    • Author(s)
      Takeya Satoshi、Hachikubo Akihiro
    • Journal Title

      Crystal Growth & Design

      Volume: 22 Issue: 2 Pages: 1345-1351

    • DOI

      10.1021/acs.cgd.1c01286

    • Related Report
      2021 Research-status Report
    • Peer Reviewed
  • [Journal Article] Superheating of Structure I Gas Hydrates within the Structure II Cyclopentane Hydrate Shell2022

    • Author(s)
      Takeya Satoshi、Muromachi Sanehiro、Yoneyama Akio、Hirano Keiichi、Hyodo Kazuyuki、Ripmeester John A.
    • Journal Title

      The Journal of Physical Chemistry Letters

      Volume: 13 Issue: 9 Pages: 2130-2136

    • DOI

      10.1021/acs.jpclett.2c00264

    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Dissociation kinetics of propane-methane and butane-methane hydrates below the melting point of ice2021

    • Author(s)
      Takeya Satoshi、Hachikubo Akihiro
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 23 Issue: 28 Pages: 15003-15009

    • DOI

      10.1039/d1cp01381e

    • Related Report
      2021 Research-status Report
    • Peer Reviewed
  • [Journal Article] Distortion of the Host Water Cages of Structure I Gas Hydrates: Structural Analysis of C2H4 Hydrate by Powder X-ray Diffraction2021

    • Author(s)
      Takeya Satoshi、Hachikubo Akihiro
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 125 Issue: 51 Pages: 28150-28156

    • DOI

      10.1021/acs.jpcc.1c09464

    • Related Report
      2021 Research-status Report
    • Peer Reviewed
  • [Journal Article] X-Ray attenuation and image contrast in the X-ray computed tomography of clathrate hydrates depending on guest species2020

    • Author(s)
      Satoshi Takeya, Sanehiro Muromachi, Akihiro Hachikubo, Ryo Ohmura, Kazuyuki Hyodo and Akio Yoneyama
    • Journal Title

      Phys.Chem.Chem.Phys.

      Volume: 22 Issue: 47 Pages: 27658-27665

    • DOI

      10.1039/d0cp05466f

    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Journal Article] Slow Crystal Growth of Cubic Ice with Stacking Faults in a Glassy Dilute Glycerol Aqueous Solution2020

    • Author(s)
      Suzuki Yoshiharu、Takeya Satoshi
    • Journal Title

      The Journal of Physical Chemistry Letters

      Volume: 11 Issue: 21 Pages: 9432-9438

    • DOI

      10.1021/acs.jpclett.0c02716

    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Presentation] 天然メタンハイドレートの高分解能X線CT観察2022

    • Author(s)
      竹谷敏、八久保晶弘、山下聡、南尚嗣、坂上寛敏、米山明男
    • Organizer
      日本地球惑星科学連合2022年大会
    • Related Report
      2022 Annual Research Report
  • [Presentation] メタンハイドレートの液中保存2022

    • Author(s)
      竹谷敏、室町実大、平野馨一、兵藤一行、米山明男
    • Organizer
      第31回日本エネルギー学会大会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 氷点下温度におけるガスハイドレートの分解と氷の相転移2022

    • Author(s)
      竹谷敏、矢作大輔、八久保晶弘
    • Organizer
      雪氷研究大会(2022・札幌)
    • Related Report
      2022 Annual Research Report
  • [Presentation] 天然メタンハイドレートの三次元非破壊観察2021

    • Author(s)
      竹谷敏、八久保晶弘、山下聡、南尚嗣、坂上寛敏、米山明男
    • Organizer
      日本地球惑星科学連合2021年大会
    • Related Report
      2021 Research-status Report
  • [Presentation] クラスレートハイドレートの吸収X線CT観察2021

    • Author(s)
      竹谷敏、室町実大、八久保晶弘、兵藤一行、米山明男
    • Organizer
      第30回日本エネルギー学会大会
    • Related Report
      2021 Research-status Report
  • [Presentation] Dissociation kinetics of gas hydrates below ice point2021

    • Author(s)
      Satoshi TAKEYA
    • Organizer
      IChES 2021
    • Related Report
      2020 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] メタン+プロパン混合ガスハイドレートの 分解挙動観察2021

    • Author(s)
      竹谷 敏、鎌田 諒也、八久保 晶弘
    • Organizer
      日本地球惑星科学連合2022年大会
    • Related Report
      2020 Research-status Report
  • [Presentation] 海底より採取したメタンハイドレートの吸収X線CT観察2021

    • Author(s)
      竹谷敏、八久保晶弘、山下聡、南尚嗣、坂上寛敏、米山明男
    • Organizer
      第29回日本エネルギー学会大会
    • Related Report
      2020 Research-status Report

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Published: 2020-04-28   Modified: 2024-01-30  

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