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Quantitative analysis of chemical reaction rates in deliquesced aerosol particles at high ionic strengths

Research Project

Project/Area Number 21K17876
Research Category

Grant-in-Aid for Early-Career Scientists

Allocation TypeMulti-year Fund
Review Section Basic Section 63010:Environmental dynamic analysis-related
Research InstitutionTohoku University (2022-2023)
Kanazawa University (2021)

Principal Investigator

Gen Masao  東北大学, 多元物質科学研究所, 助教 (50774535)

Project Period (FY) 2021-04-01 – 2024-03-31
Project Status Discontinued (Fiscal Year 2023)
Budget Amount *help
¥4,550,000 (Direct Cost: ¥3,500,000、Indirect Cost: ¥1,050,000)
Fiscal Year 2023: ¥1,040,000 (Direct Cost: ¥800,000、Indirect Cost: ¥240,000)
Fiscal Year 2022: ¥1,300,000 (Direct Cost: ¥1,000,000、Indirect Cost: ¥300,000)
Fiscal Year 2021: ¥2,210,000 (Direct Cost: ¥1,700,000、Indirect Cost: ¥510,000)
Keywordsエアロゾル / 大気化学反応 / NO2 / 不均一反応 / 多相反応 / 不均一/多相反応 / 大気化学 / 反応速度定数 / イオン強度
Outline of Research at the Start

エアロゾルに起因する気候変動および人への健康影響は、化学組成に強く依存するため、その反応速度定数を正確に見積もることが重要である。エアロゾル反応系の特徴である高イオン強度条件下では、その反応速度定数が変化すると予測されている。しかし従来の手法ではエアロゾル反応を直接測定するのは困難であるため、高イオン強度の影響は十分に解明されていない。
本研究では高イオン強度条件下における化学反応を定量的に評価する。申請者が独自に開発してきた単一粒子分光分析法を応用し、イオン強度とエアロゾルの反応速度定数の関係を数式化する。その関係式をモデルへ実装、「高イオン強度の影響」を考慮したエアロゾル反応系を再構築する。

Outline of Final Research Achievements

Nitrogen dioxide (NO2) hydrolysis in deliquesced aerosol particles forms nitrous acid and nitrate and thus impacts air quality, climate, and the nitrogen cycle. Traditionally, it is considered to proceed far too slowly in the atmosphere. However, the significance of this process is highly uncertain because kinetic studies have only been made in dilute aqueous solutions but not under high ionic strength conditions of the aerosol particles. Here, we use laboratory experiments, air quality models, and field measurements to examine the effect of the ionic strength on the reaction kinetics of NO2 hydrolysis. We find that high ionic strengths (I) enhance the reaction rate constants (kI) by more than an order of magnitude compared to that at infinite dilution (kI=0), yielding log10(kI/kI=0) = 0.04I.

Academic Significance and Societal Importance of the Research Achievements

エアロゾルの反応速度定数への高イオン強度の影響は未だ解明されず、従来の研究ではバルク反応領域から得られた速度定数がエアロゾルの反応速度定数として代用されてきた。本研究の成果では、高イオン強度条件の影響に係る実験的検討を行い、エアロゾル相での反応速度定数は、バルク溶液(イオン強度がゼロ)に比べて、何倍もから高いことを示した。この成果は、従来のバルク溶液から得られた反応速度論は大気エアロゾル中で起こる化学反応には適用できないことが示唆され、大気化学研究におけるイオン強度の重要性が高まると考えられる。

Report

(3 results)
  • 2023 Final Research Report ( PDF )
  • 2022 Annual Research Report
  • 2021 Research-status Report
  • Research Products

    (9 results)

All 2023 2022 Other

All Int'l Joint Research (3 results) Journal Article (4 results) (of which Int'l Joint Research: 4 results,  Peer Reviewed: 4 results,  Open Access: 3 results) Presentation (2 results)

  • [Int'l Joint Research] Tsinghua University/Nankai University(中国)

    • Related Report
      2022 Annual Research Report
  • [Int'l Joint Research] Max Planck Institute for Chemistry(ドイツ)

    • Related Report
      2022 Annual Research Report
  • [Int'l Joint Research] City University of Hong Kong(中国)

    • Related Report
      2021 Research-status Report
  • [Journal Article] Single-particle Raman spectroscopy for studying physical and chemical processes of atmospheric particles2022

    • Author(s)
      Liang Zhancong、Chu Yangxi、Gen Masao、Chan Chak K.
    • Journal Title

      Atmospheric Chemistry and Physics

      Volume: 22 Issue: 5 Pages: 3017-3044

    • DOI

      10.5194/acp-22-3017-2022

    • Related Report
      2022 Annual Research Report 2021 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Photochemical Reactions of Glyoxal during Particulate Ammonium Nitrate Photolysis: Brown Carbon Formation, Enhanced Glyoxal Decay, and Organic Phase Formation2022

    • Author(s)
      Zhang Ruifeng、Gen Masao、Liang Zhancong、Li Yong Jie、Chan Chak Keung
    • Journal Title

      Environmental Science & Technology

      Volume: 56 Issue: 3 Pages: 1605-1614

    • DOI

      10.1021/acs.est.1c07211

    • Related Report
      2022 Annual Research Report 2021 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Rapid hydrolysis of NO2 at high ionic strengths of deliquesced aerosol particles2022

    • Author(s)
      Gen Masao、Zheng Haotian、Sun Yele、Xu Wanyun、Ma Nan、Su Hang、Cheng Yafang、Wang Shuxiao、Xing Jia、Zhang Shuping、Xue Likun、Xue Chaoyang、Mu Yujing、Tian Xiao、Matsuki Atsushi、Song Shaojie
    • Journal Title

      Research Square

      Volume: -

    • DOI

      10.21203/rs.3.rs-2257102/v1

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Particulate nitrate photolysis in the atmosphere2022

    • Author(s)
      Gen Masao、Liang Zhancong、Zhang Ruifeng、Go Mabato Beatrix Rosette、Chan Chak K.
    • Journal Title

      Environmental Science: Atmospheres

      Volume: 2 Issue: 2 Pages: 111-127

    • DOI

      10.1039/d1ea00087j

    • Related Report
      2022 Annual Research Report 2021 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Presentation] Rapid hydrolysis of NO2 at high ionic strengths of deliquesced aerosol particles2023

    • Author(s)
      玄 大雄、Haotian Zheng、Yele Sun、Wanyun Xu、Nan Ma、Hang Su、Yafang Cheng、Shuxiao Wang、Jia Xing、Shuping Zhang、Likun Xue、Chaoyang Xue 、Yujing Mu、Xiao Tian、Atsushi Matsuki、Shaojie Song
    • Organizer
      日本地球惑星科学連合2023年大会
    • Related Report
      2022 Annual Research Report
  • [Presentation] NO2の加水分解反応へのエアロゾルのイオン強度の影響2022

    • Author(s)
      玄大雄, 佐々木結, Haotian Zheng, Shaojie Song
    • Organizer
      第39回エアロゾル科学・技術研究討論会
    • Related Report
      2022 Annual Research Report

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Published: 2021-04-28   Modified: 2025-01-30  

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