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Elucidation of reaction mechanisms at gas-liquid interfaces in the atmosphere

Research Project

Project/Area Number 19H01154
Research Category

Grant-in-Aid for Scientific Research (A)

Allocation TypeSingle-year Grants
Section一般
Review Section Medium-sized Section 63:Environmental analyses and evaluation and related fields
Research InstitutionUniversity of Tsukuba (2022-2023)
National Institute for Environmental Studies (2019-2021)

Principal Investigator

Enami Shinichi  筑波大学, 数理物質系, 教授 (00589385)

Project Period (FY) 2019-04-01 – 2023-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥46,410,000 (Direct Cost: ¥35,700,000、Indirect Cost: ¥10,710,000)
Fiscal Year 2022: ¥4,030,000 (Direct Cost: ¥3,100,000、Indirect Cost: ¥930,000)
Fiscal Year 2021: ¥4,420,000 (Direct Cost: ¥3,400,000、Indirect Cost: ¥1,020,000)
Fiscal Year 2020: ¥6,370,000 (Direct Cost: ¥4,900,000、Indirect Cost: ¥1,470,000)
Fiscal Year 2019: ¥31,590,000 (Direct Cost: ¥24,300,000、Indirect Cost: ¥7,290,000)
Keywordsエアロゾル / 界面 / ラジラジカル / 不均一反応 / マルチフェーズ反応 / 環境 / 気候変動 / 大気汚染 / 液相 / ラジカル / 界面反応 / 大気化学 / 質量分析 / フェントン反応 / エイジング / オゾニド / バルク / 物理化学 / レボグルコサン / テルペン / 反応 / 毒性 / 表面 / フェントン / オゾン / PM2.5 / 温暖化 / 健康影響
Outline of Research at the Start

本提案研究では、気液界面反応測定手法に加えて、瞬時に起こる液相反応をその場測定できる新規手法を開発し、気液界面反応vs液相反応を直接比較できる実験システムを構築する。それにより、気液界面で起こる反応の特殊性の起源の解明を目指す。本提案研究が完成すると、大気における界面反応とバルク反応をどのように定量的に区別して扱えばよいかが明らかになり、大気モデルへの取り込みなど、多くの成果が見込まれる。

Outline of Final Research Achievements

Atmospherically important reactions at the air-water interface were investigated by interface-sensitive spray ionization mass spectrometry. Furthermore, the dual-microjets mass spectrometry was developed for direct comparison between the interface vs bulk reaction mechanisms. The important knowledge on the origin of the interface-specific mechanisms was obtained. These results will be highly valuable for future atmospheric modeling.

Academic Significance and Societal Importance of the Research Achievements

気候変動と大気汚染の問題は人類が解決すべき重大な環境問題である。これらの問題と密接に関連する大気中に浮遊する雲粒とエアロゾルの気液界面と液相で起こる化学反応機構の分子レベルでの理解は極めて重要である。本研究によって、気液界面で起こる反応の特殊性の起源の一部が初めて明らかになった。また、大気における界面反応とバルク反応をどのように定量的に区別して扱えばよいかが明らかになった。今後、大気モデルへの取り込みなど、多くの成果が見込まれるため、重要である。

Report

(6 results)
  • 2023 Final Research Report ( PDF )
  • 2022 Annual Research Report
  • 2021 Annual Research Report
  • 2020 Annual Research Report
  • 2019 Comments on the Screening Results   Annual Research Report
  • Research Products

    (37 results)

All 2024 2023 2022 2021 2020 2019 Other

All Int'l Joint Research (3 results) Journal Article (20 results) (of which Int'l Joint Research: 5 results,  Peer Reviewed: 20 results,  Open Access: 11 results) Presentation (14 results) (of which Int'l Joint Research: 3 results,  Invited: 7 results)

  • [Int'l Joint Research] Caltech(米国)

    • Related Report
      2021 Annual Research Report
  • [Int'l Joint Research] UC Riverside(米国)

    • Related Report
      2020 Annual Research Report
  • [Int'l Joint Research] Caltech(米国)

    • Related Report
      2019 Annual Research Report
  • [Journal Article] Impurity contribution to ultraviolet absorption of saturated fatty acids2023

    • Author(s)
      Saito Shota、Numadate Naoki、Teraoka Hidemasa、Enami Shinichi、Kobayashi Hirokazu、Hama Tetsuya
    • Journal Title

      Science Advances

      Volume: 9 Issue: 38

    • DOI

      10.1126/sciadv.adj6438

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Mechanism of Fenton Oxidation of Levoglucosan in Water2023

    • Author(s)
      Enami Shinichi、Morino Yu、Sato Kei
    • Journal Title

      The Journal of Physical Chemistry A

      Volume: 127 Issue: 13 Pages: 2975-2985

    • DOI

      10.1021/acs.jpca.3c00512

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 大気マルチフェーズ化学:気液界面と液中で起こるオゾン反応2023

    • Author(s)
      江波進一
    • Journal Title

      大気環境学会誌

      Volume: 58

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Direct Observation and Quantitative Measurement of OH Radical Desorption During the Ultraviolet Photolysis of Liquid Nonanoic Acid2022

    • Author(s)
      Naoki Numadate, Shota Saito, Yuki Nojima, Taka-aki Ishibashi, Shinichi Enami, and Tetsuya Hama
    • Journal Title

      The Journal of Physical Chemistry Letters

      Volume: 13 Issue: 35 Pages: 8290-8297

    • DOI

      10.1021/acs.jpclett.2c02199

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Stability of Terpenoid-Derived Secondary Ozonides in Aqueous Organic Media2022

    • Author(s)
      Junting Qiu, Michiya Fujita, Kenichi Tonokura, and Shinichi Enami
    • Journal Title

      The Journal of Physical Chemistry A

      Volume: 126 Issue: 32 Pages: 5386-5397

    • DOI

      10.1021/acs.jpca.2c04077

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Proton-Catalyzed Decomposition of Multifunctionalized Organic Hydroperoxides Derived from the Reactions of Criegee Intermediates with Ethylene Glycol in Aqueous Organic Media2022

    • Author(s)
      Enami Shinichi
    • Journal Title

      ACS Earth and Space Chemistry

      Volume: 6 Issue: 7 Pages: 1937-1947

    • DOI

      10.1021/acsearthspacechem.2c00142

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Decomposition of multifunctionalized α-alkoxyalkyl-hydroperoxides derived from the reactions of Criegee intermediates with diols in liquid phases2022

    • Author(s)
      Endo Yasuyuki、Sakamoto Yosuke、Kajii Yoshizumi、Enami Shinichi
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 24 Issue: 19 Pages: 11562-11572

    • DOI

      10.1039/d2cp00915c

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 未来の大気化学のための室内実験2022

    • Author(s)
      江波進一、石塚紳之助、羽馬哲也、猪俣敏
    • Journal Title

      大気化学研究

      Volume: 47

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Decomposition mechanism of α-alkoxyalkyl-hydroperoxides in the liquid phase: temperature dependent kinetics and theoretical calculations2022

    • Author(s)
      Hu Mingxi、Chen Kunpeng、Qiu Junting、Lin Ying-Hsuan、Tonokura Kenichi、Enami Shinichi
    • Journal Title

      Environmental Science: Atmospheres

      Volume: 2 Issue: 2 Pages: 241-251

    • DOI

      10.1039/d1ea00076d

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] テルペン由来クリーギー中間体の気液界面反応2022

    • Author(s)
      江波進一
    • Journal Title

      エアロゾル研究

      Volume: 37 Pages: 12-20

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Fates of Organic Hydroperoxides in Atmospheric Condensed Phases2021

    • Author(s)
      Enami Shinichi
    • Journal Title

      The Journal of Physical Chemistry A

      Volume: 125 Issue: 21 Pages: 4513-4523

    • DOI

      10.1021/acs.jpca.1c01513

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Hydronium Ion Acidity Above and Below the Interface of Aqueous Microdroplets2021

    • Author(s)
      Colussi Agustin J.、Enami Shinichi、Ishizuka Shinnosuke
    • Journal Title

      ACS Earth and Space Chemistry

      Volume: 5 Issue: 9 Pages: 2341-2346

    • DOI

      10.1021/acsearthspacechem.1c00067

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Effects of Metal Ions on Aqueous-Phase Decomposition of α-Hydroxyalkyl-Hydroperoxides Derived from Terpene Alcohols2021

    • Author(s)
      Hu Mingxi、Tonokura Kenichi、Morino Yu、Sato Kei、Enami Shinichi
    • Journal Title

      Environmental Science & Technology

      Volume: 55 Pages: 12893-12901

    • DOI

      10.1021/acs.est.1c04635

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] 空気-水の界面で起こる化学反応2021

    • Author(s)
      江波進一
    • Journal Title

      ぶんせき

      Volume: 8 Pages: 380-386

    • NAID

      40022674772

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Stability of Monoterpene-Derived α-Hydroxyalkyl-Hydroperoxides in Aqueous Organic Media: Relevance to the Fate of Hydroperoxides in Aerosol Particle Phases2020

    • Author(s)
      Qiu Junting、Liang Zhancong、Tonokura Kenichi、Colussi Agustin J.、Enami Shinichi
    • Journal Title

      Environmental Science & Technology

      Volume: 54 Issue: 7 Pages: 3890-3899

    • DOI

      10.1021/acs.est.9b07497

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Effects of pH on Interfacial Ozonolysis of α-Terpineol2019

    • Author(s)
      Qiu Junting、Ishizuka Shinnosuke、Tonokura Kenichi、Sato Kei、Inomata Satoshi、Enami Shinichi
    • Journal Title

      The Journal of Physical Chemistry A

      Volume: 123 Issue: 32 Pages: 7148-7155

    • DOI

      10.1021/acs.jpca.9b05434

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Acid-Catalyzed Oligomerization at the Air-Water Interface Modified by Competitive Adsorption of Surfactants2019

    • Author(s)
      Ishizuka Shinnosuke、Hama Tetsuya、Enami Shinichi
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 123 Issue: 35 Pages: 21662-21669

    • DOI

      10.1021/acs.jpcc.9b07380

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Comment on “The chemical reactions in electrosprays of water do not always correspond to those at the pristine air-water interface” by A. Gallo Jr, A. S. F. Farinha, M. Dinis, A.-H. Emwas, A. Santana, R. J. Nielsen, W. A. Goddard III and H. Mishra, Chem. Sci., 2019, 10, 25662019

    • Author(s)
      Colussi Agustin J.、Enami Shinichi
    • Journal Title

      Chemical Science

      Volume: 10 Issue: 35 Pages: 8253-8255

    • DOI

      10.1039/c9sc00991d

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Water Dramatically Accelerates the Decomposition of α-Hydroxyalkyl-Hydroperoxides in Aerosol Particles2019

    • Author(s)
      Qiu Junting、Ishizuka Shinnosuke、Tonokura Kenichi、Colussi Agustin J.、Enami Shinichi
    • Journal Title

      The Journal of Physical Chemistry Letters

      Volume: 10 Issue: 19 Pages: 5748-5755

    • DOI

      10.1021/acs.jpclett.9b01953

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Interfacial Water Mediates Oligomerization Pathways of Monoterpene Carbocations2019

    • Author(s)
      Ishizuka Shinnosuke、Matsugi Akira、Hama Tetsuya、Enami Shinichi
    • Journal Title

      The Journal of Physical Chemistry Letters

      Volume: 11 Issue: 1 Pages: 67-74

    • DOI

      10.1021/acs.jpclett.9b03110

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Open Access
  • [Presentation] 大気Å不均一科学の創成2024

    • Author(s)
      江波進一
    • Organizer
      JSTさきがけ発展研究会
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] 大気マルチフェーズ化学:気液界面と液中で起こるオゾン反応2022

    • Author(s)
      江波進一
    • Organizer
      第63回大気環境学会年会
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] 微小不均一性は液相反応にどのような影響を与えるか?2022

    • Author(s)
      江波進一
    • Organizer
      第16回分子科学討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] テルペン由来オゾニドはエアロゾル中で分解するか?2022

    • Author(s)
      江波進一, 邱鈞霆, 藤田道也, 戸野倉賢一
    • Organizer
      第27回大気化学討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 雲粒中で起こる化学反応の研究2022

    • Author(s)
      江波進一
    • Organizer
      SATテクノロジー・ショーケース2023
    • Related Report
      2021 Annual Research Report
  • [Presentation] Fates of terpenoid-derived hydroperoxides in atmospheric condensed phases2021

    • Author(s)
      Enami Shinichi
    • Organizer
      6th International Workshop on Heterogeneous Kinetics Related to Atmospheric Aerosols
    • Related Report
      2020 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 未来の大気化学のための室内実験2021

    • Author(s)
      江波進一, 石塚紳之助,羽馬哲也,猪俣敏
    • Organizer
      第26回大気化学討論会
    • Related Report
      2020 Annual Research Report
    • Invited
  • [Presentation] 空気―水の境界相で起こるラジカル反応のメカニズム2020

    • Author(s)
      江波進一
    • Organizer
      レーザー学会学術講演会第40回年次大会
    • Related Report
      2019 Annual Research Report
    • Invited
  • [Presentation] Fates of terpene alpha-hydroxyalkyl-hydroperoxides in aqueous aerosol2019

    • Author(s)
      Shinichi Enami
    • Organizer
      5th International Workshop on Heterogeneous Kinetics Related to Atmospheric Aerosols
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Interface-specific reaction pathways of monoterpene carbocations2019

    • Author(s)
      S. Ishizuka, A. Matsugi, T. Hama, S. Enami
    • Organizer
      35th Symposium on Chemical Kinetics and Dynamics
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] エアロゾル中のテルペン由来過酸化物の分解メカニズム2019

    • Author(s)
      江波進一, 邱鈞霆, 戸野倉賢一
    • Organizer
      第24回大気化学討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Microhydration Mediates Cationic Polymerization at the Air-Water Interface2019

    • Author(s)
      S. Ishizuka, A. Matsugi, T. Hama, S. Enami
    • Organizer
      第68回高分子討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] 大気圏マルチフェーズ化学2019

    • Author(s)
      江波進一
    • Organizer
      京都大学生存圏研究所大気圏セミナー
    • Related Report
      2019 Annual Research Report
    • Invited
  • [Presentation] Surfactant effects on acid-catalyzed reactions at aqueous aerosol surfaces2019

    • Author(s)
      S. Ishizuka, T. Hama, S. Enami
    • Organizer
      日本地球惑星科学連合2019年大会
    • Related Report
      2019 Annual Research Report

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Published: 2019-04-18   Modified: 2025-01-30  

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