Elucidation of photochemical aging process of atmospheric aerosol

• Project/Area Number: 15H05328
• Research Category: Grant-in-Aid for Young Scientists (A)
• Allocation Type: Single-year Grants
• Research Field: Environmental dynamic analysis
• Research Institution: National Institute for Environmental Studies (2016-2018); Kyoto University (2015)
• Principal Investigator: ENAMI SHINICHI 国立研究開発法人国立環境研究所, 環境計測研究センター, 主任研究員 (00589385)
• Project Period (FY): 2015-04-01 – 2019-03-31
• Project Status: Completed (Fiscal Year 2018)
• Budget Amount: ¥23,660,000 (Direct Cost: ¥18,200,000、Indirect Cost: ¥5,460,000); Fiscal Year 2018: ¥8,450,000 (Direct Cost: ¥6,500,000、Indirect Cost: ¥1,950,000); Fiscal Year 2017: ¥5,330,000 (Direct Cost: ¥4,100,000、Indirect Cost: ¥1,230,000); Fiscal Year 2016: ¥5,330,000 (Direct Cost: ¥4,100,000、Indirect Cost: ¥1,230,000); Fiscal Year 2015: ¥4,550,000 (Direct Cost: ¥3,500,000、Indirect Cost: ¥1,050,000)
• Keywords: エアロゾル / 界面 / 表面 / 大気化学 / 気候変動 / PM2.5 / 毒性 / 中間体 / 質量分析法 / 地球温暖化 / 大気汚染 / 光化学 / ラジカル / 健康影響 / 反応 / イオン / クリーギー / レーザー / オゾン / 不均一反応 / 環境化学

Outline of Final Research Achievements

We have successfully elucidated the reaction mechanisms involving peroxyl radicals, Criegee intermediates, and carbocations occuring at the gas-liquid aerosol, that help us to understand atmospheric multiphase chemistry. We published 24 papers including: Qiu et al. Environ. Sci. Technol., 2019, DOI:　10.1021/acs.est.9b00364., Enami et al. J. Phys. Chem. Lett., 2017, 8, 1615, Enami et al. J. Phys. Chem. Lett., 2017, 8, 3888, Enami et al. Environ. Sci. Technol., 2016, 50, 1834, Enami et al. J. Phys. Chem. Lett., 2015, 6, 3935, Enami et al. J. Phys. Chem. Lett., 2015, 6, 527. These results will have impact on elucidation of aging processes of atmospeheric aerosol.

Academic Significance and Societal Importance of the Research Achievements

地球の気候変動に重要な影響を与えている空気中に浮遊する微粒子（エアロゾル）は気相の反応物と気液界面で反応を起こし、その結果、エアロゾルの放射強制力（気候に対して与える放射の大きさ）や生体への毒性が常に変化している。これまで測定できなかった気液界面に生成する中間体を検出できる新規手法を用いて、大気エアロゾルの光化学的エイジングのメカニズムを解明することに成功した。その結果、地球の気候変動予測の精度向上とPM2.5(Particulate Matter 2.5, 粒径が2.5マイクロメートル以下の粒子状物質)のヒトへの毒性評価の向上に大きく貢献した。

Research Products

• [Int'l Joint Research] Caltech(米国)
• [Int'l Joint Research] Caltech(米国)
• [Int'l Joint Research] Caltech(米国)
• [Journal Article] Detecting Intermediates and Products of Fast Heterogeneous Reactions on Liquid Surfaces via Online Mass Spectrometry (2019)
  • Author(s): Colussi Agustin、Enami Shinichi
  • Journal Title: Atmosphere Volume: 10 Issue: 2 Pages: 47-47
  • DOI: 10.3390/atmos10020047
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Chemical signatures of surface microheterogeneity on liquid mixtures (2019)
  • Author(s): Enami Shinichi、Ishizuka Shinnosuke、Colussi Agustin J.
  • Journal Title: The Journal of Chemical Physics Volume: 150 Issue: 2 Pages: 024702-024702
  • DOI: 10.1063/1.5055684
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Interfacial vs bulk ozonolysis of nerolidol (2019)
  • Author(s): Qiu Junting、Ishizuka Shinnosuke、Tonokura Kenichi、Enami Shinichi
  • Journal Title: Environmental Science and Technology Volume: in press Issue: 10 Pages: 5750-5757
  • DOI: 10.1021/acs.est.9b00364
  • Peer Reviewed / Open Access
• [Journal Article] OH-Radical Oxidation of Lung Surfactant Protein B on Aqueous Surfaces (2018)
  • Author(s): Enami Shinichi、Colussi Agustin J.
  • Journal Title: Mass Spectrometry Volume: 7 Issue: 2 Pages: 1-7
  • DOI: 10.5702/massspectrometry.S0077
  • NAID: 130007520489
  • ISSN: 2186-5116, 2187-137X
  • Year and Date: 2018-11-21
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Chain-propagation, chain-transfer, and hydride-abstraction by cyclic carbocations on water surface (2018)
  • Author(s): Shinnosuke Ishizuka, Akira Matsugi, Tetsuya Hama, and Shinichi Enami
  • Journal Title: Physical Chemistry Chemical Physics Volume: 20 Issue: 39 Pages: 25256-25267
  • DOI: 10.1039/c8cp04993a
  • Peer Reviewed
• [Journal Article] Reactivity of Monoterpene Criegee Intermediates at Gas-Liquid Interfaces (2018)
  • Author(s): Qiu Junting、Ishizuka Shinnosuke、Tonokura Kenichi、Colussi Agustin J.、Enami Shinichi
  • Journal Title: The Journal of Physical Chemistry A Volume: 122 Issue: 39 Pages: 7910-7917
  • DOI: 10.1021/acs.jpca.8b06914
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Reactions of Criegee Intermediates with Benzoic Acid at the Gas/Liquid Interface (2018)
  • Author(s): Qiu Junting、Ishizuka Shinnosuke、Tonokura Kenichi、Enami Shinichi
  • Journal Title: The Journal of Physical Chemistry A Volume: 122 Issue: 30 Pages: 6303-6310
  • DOI: 10.1021/acs.jpca.8b04995
  • Peer Reviewed
• [Journal Article] Controlling factors of oligomerization at the water surface: why is isoprene such a unique VOC? (2018)
  • Author(s): Shinnosuke Ishizuka, Tomihide Fujii, Akira Matsugi, Yosuke Sakamoto, Tetsuya Hama, and Shinichi Enami
  • Journal Title: Physical Chemistry Chemical Physics Volume: 20 Issue: 22 Pages: 15400-15410
  • DOI: 10.1039/c8cp01551a
  • Peer Reviewed
• [Journal Article] Efficient scavenging of Criegee intermediates on water by surface-active cis-pinonic acid (2017)
  • Author(s): Enami Shinichi、Colussi A. J.
  • Journal Title: Physical Chemistry Chemical Physics Volume: 19 Issue: 26 Pages: 17044-17051
  • DOI: 10.1039/c7cp03869k
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Reactions of Criegee Intermediates with Alcohols at Air-Aqueous Interfaces (2017)
  • Author(s): Enami Shinichi、Colussi A. J.
  • Journal Title: The Journal of Physical Chemistry A Volume: 121 Issue: 27 Pages: 5175-5182
  • DOI: 10.1021/acs.jpca.7b04272
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Criegee Intermediates React with Levoglucosan on Water (2017)
  • Author(s): Enami Shinichi、Hoffmann Michael R.、Colussi A. J.
  • Journal Title: The Journal of Physical Chemistry Letters Volume: 8 Issue: 16 Pages: 3888-3894
  • DOI: 10.1021/acs.jpclett.7b01665
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Aerosol Health Effects from Molecular to Global Scales (2017)
  • Author(s): Shiraiwa et al.
  • Journal Title: Environmental Science & Technology Volume: 51 Issue: 23 Pages: 13545-13567
  • DOI: 10.1021/acs.est.7b04417
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Criegee chemistry on aqueous organic surfaces (2017)
  • Author(s): S. Enami, A. J. Colussi
  • Journal Title: J. Phys. Chem. Lett. Volume: 8 Issue: 7 Pages: 1615-1623
  • DOI: 10.1021/acs.jpclett.7b00434
  • Peer Reviewed / Int'l Joint Research / Acknowledgement Compliant
• [Journal Article] Reactive uptake of gaseous sesquiterpenes on aqueous surfaces (2017)
  • Author(s): K. Matsuoka, Y. Sakamoto, T. Hama, Y. Kajii, S. Enami
  • Journal Title: J. Phys. Chem. A Volume: 121 Issue: 4 Pages: 810-818
  • DOI: 10.1021/acs.jpca.6b11821
  • Peer Reviewed / Acknowledgement Compliant
• [Journal Article] Extensive H-atom abstraction from benzoate by OH-radicals at the air-water interface (2016)
  • Author(s): S. Enami, M. R. Hoffmann, A. J. Colussi
  • Journal Title: Phys. Chem. Chem. Phys. Volume: 18 Issue: 46 Pages: 31505-31512
  • DOI: 10.1039/c6cp06652f
  • Peer Reviewed / Int'l Joint Research / Acknowledgement Compliant
• [Journal Article] “Sizing” heterogeneous chemistry in the conversion of gaseous dimethyl sulfide to atmospheric particulates (2016)
  • Author(s): S. Enami, Y. Sakamoto, K. Hara, K. Osada, M. R. Hoffmann, A. J. Colussi
  • Journal Title: Environ. Sci. Technol. Volume: 50 Issue: 4 Pages: 1834-1843
  • DOI: 10.1021/acs.est.5b05337
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] OH-radical specific addition to glutathione S-atom at the air-water interface – Relevance to the redox balance of the lung epithelial lining fluid (2015)
  • Author(s): S. Enami, M. R. Hoffmann, A. J. Colussi
  • Journal Title: J. Phys. Chem. Lett. Volume: 6 Issue: 19 Pages: 3935-3943
  • DOI: 10.1021/acs.jpclett.5b01819
  • NAID: 120005753866
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Presentation] Microheterogeneous Water Surfaces (2019)
  • Author(s): Shinichi Enami
  • Organizer: IMS Symposium: Water at Interfaces 2018
  • Int'l Joint Research / Invited
• [Presentation] Chemical Reactions at Microheterogeneous Aerosol Surfaces (2018)
  • Author(s): Shinichi Enami
  • Organizer: 1st International Symposium on Aerosol Chemistry and Related Reaction Dynamics
  • Int'l Joint Research / Invited
• [Presentation] Reactions of terpene Criegee intermediates with water, acids, alcohols, and saccharides at gas-liquid interfaces (2018)
  • Author(s): Shinichi Enami
  • Organizer: The 22nd East Asian Workshop on Chemical Dynamics
  • Int'l Joint Research / Invited
• [Presentation] Lung surface chemistry: Why air pollutants are "toxic"? (2018)
  • Author(s): Shinichi Enami
  • Organizer: Tsukuba Global Science Week 2018
  • Int'l Joint Research / Invited
• [Presentation] 生体内における不均一性と界面反応 (2018)
  • Author(s): Shinichi Enami
  • Organizer: 第８回日本分子状水素医学生物学会
  • Invited
• [Presentation] 新規質量分析法を用いた新しい界面科学の探求 (2018)
  • Author(s): Shinichi Enami
  • Organizer: Mass Spectrometry and Proteomics 2018
  • Invited
• [Presentation] 環境問題の解決に向けた分子科学的アプローチ (2018)
  • Author(s): Shinichi Enami
  • Organizer: 第67回中国四国産学連携化学フォーラム
  • Invited
• [Presentation] In-situ mass spectrometric monitoring of reactions at the gas-liquid interface (2018)
  • Author(s): Enami Shinichi
  • Organizer: Pittcon 2018
  • Int'l Joint Research / Invited
• [Presentation] Mass spectrometric measurements of fast radical reactions at the air-water interface (2018)
  • Author(s): Enami Shinichi
  • Organizer: 日本化学会第98春季年会アジア国際シンポジウム
  • Int'l Joint Research / Invited
• [Presentation] Atmospheric intermediates at the air-water interface (2017)
  • Author(s): S. Enami
  • Organizer: The 1st Workshop on Physical Chemistry in the Atmosphere
  • Place of Presentation: アカデミアシニカ(台北)
  • Year and Date: 2017-03-22
  • Int'l Joint Research / Invited
• [Presentation] Interfacial reactions of Criegee intermediates with water, acids, alcohols and sugars (2017)
  • Author(s): Enami Shinichi
  • Organizer: 3rd International Workshop on Heterogeneous Kinetics Related to Atmospheric Aerosols
  • Int'l Joint Research / Invited
• [Presentation] Reactions of Criegee intermediates at gas-aqueous interfaces (2017)
  • Author(s): Enami Shinichi
  • Organizer: 34th International Symposium on Free Radicals
  • Int'l Joint Research
• [Presentation] Reactions of Criegee intermediates at the gas-liquid interface (2017)
  • Author(s): Enami Shinichi
  • Organizer: 254th ACS National Meeting
  • Int'l Joint Research
• [Presentation] Experimental study on the reactions of Criegee intermediates at the gas-liquid interface (2017)
  • Author(s): Enami Shinichi
  • Organizer: 33rd Symposium on Chemical Kinetics and Dynamics
  • Int'l Joint Research
• [Presentation] Heterogeneous reactions of gaseous ozone with aqueous sesquiterpenes: The roles of Criegee intermediates (2017)
  • Author(s): Enami Shinichi、Colussi A. J.
  • Organizer: JpGU-AGU joint meeting 2017
  • Int'l Joint Research
• [Presentation] クリーギー中間体は大気エアロゾルの成長にどのように関与しているのか？ (2017)
  • Author(s): 江波進一
  • Organizer: 第23回大気化学討論会
• [Presentation] Heterogeneous Reactions of Atmospheric Radical/Atom with Aqueous Species (2016)
  • Author(s): S. Enami
  • Organizer: 2nd International Workshop on Heterogeneous Kinetics Related to Atmospheric
  • Place of Presentation: つくば国際会議場(茨城県)
  • Year and Date: 2016-11-12
  • Int'l Joint Research / Invited
• [Presentation] エアロゾルの表面で起こる不均一ハロゲンラジカル反応の研究 (2016)
  • Author(s): S. Enami
  • Organizer: 第22回大気化学討論会
  • Place of Presentation: 北海道大学工学部フロンティア応用科学研究棟 (北海道)
  • Year and Date: 2016-10-13
• [Presentation] OH-Radical Oxidation of Organic Species at the Air-Water Interface (2016)
  • Author(s): S. Enami
  • Organizer: 14th IGAC Science Conference
  • Place of Presentation: Beaver Run (米国コロラド州)
  • Year and Date: 2016-09-27
  • Int'l Joint Research
• [Presentation] 水の界面における不均一ハロゲンラジカル反応の研究 (2016)
  • Author(s): S. Enami
  • Organizer: 第10回分子科学討論会
  • Place of Presentation: 神戸ファッションマート(兵庫県)
  • Year and Date: 2016-09-13
• [Presentation] Radical chemistry at aqueous interfaces (2016)
  • Author(s): S. Enami
  • Organizer: 平成28年度化学系学協会東北大会
  • Place of Presentation: いわき明星大学(福島県)
  • Year and Date: 2016-09-11
  • Invited
• [Presentation] 雲核生成の鍵となるジメチルスルホキシドとOHラジカルの不均一反応の研究 (2016)
  • Author(s): S. Enami
  • Organizer: 日本地球惑星科学連合2016年大会
  • Place of Presentation: 幕張メッセ(千葉県)
  • Year and Date: 2016-05-25
• [Presentation] In-situ mass spectrometric detection of radical intermediates at the air-water interface (2015)
  • Author(s): S.Enami
  • Organizer: Pacifichem2015
  • Place of Presentation: Hawaii (USA)
  • Year and Date: 2015-12-15
  • Int'l Joint Research / Invited
• [Presentation] Reactions of reactive oxygen species with lung antioxidants at the air-water interface (2015)
  • Author(s): S. Enami
  • Organizer: Physicochemical properties of atmospheric aerosols and their effects on air quality and public health
  • Place of Presentation: Mainz (Germany)
  • Year and Date: 2015-11-25
  • Int'l Joint Research
• [Presentation] Elucidating the photochemical aging mechanism of aqueous organic aerosols (2015)
  • Author(s): S. Enami
  • Organizer: The 13th international conference on the Atmospheric Sciences and Application to Air Quality
  • Place of Presentation: 神戸
  • Year and Date: 2015-11-11
  • Int'l Joint Research
• [Presentation] 大気エアロゾルの光化学的エイジング過程の研究 (2015)
  • Author(s): S. Enami
  • Organizer: 第21回大気化学討論会
  • Place of Presentation: 東京
  • Year and Date: 2015-10-19
• [Presentation] 大気中及び生体中で起こる界面ラジカル反応機構の解明 (2015)
  • Author(s): S. Enami
  • Organizer: 第9回分子科学討論会
  • Place of Presentation: 東京
  • Year and Date: 2015-09-16
• [Presentation] Interfacial radical chemistry (2015)
  • Author(s): S. Enami
  • Organizer: 31st Symposium on Chemical Kinetics and Dynamics
  • Place of Presentation: 札幌
  • Year and Date: 2015-06-03
  • Int'l Joint Research
• [Book] Multiphase Environmental Chemistry in the Atmosphere (2018)
  • Author(s): Shinichi Enami
  • Total Pages: 13
  • Publisher: ACS
• [Remarks] 大気中の粒子成長の鍵となるプロセスを解明
  • URL: https://www.nies.go.jp/whatsnew/20170407/20170407.html