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硫化カルボニルの四種硫黄同位体比に注目した、成層圏硫酸エアロゾル生成過程の解明

Research Project

Project/Area Number 10J07563
Research Category

Grant-in-Aid for JSPS Fellows

Allocation TypeSingle-year Grants
Section国内
Research Field Environmental dynamic analysis
Research InstitutionTokyo Institute of Technology

Principal Investigator

服部 祥平  東京工業大学, 大学院・総合理工学研究科, 助教

Project Period (FY) 2010 – 2012
Project Status Completed (Fiscal Year 2012)
Budget Amount *help
¥2,100,000 (Direct Cost: ¥2,100,000)
Fiscal Year 2012: ¥700,000 (Direct Cost: ¥700,000)
Fiscal Year 2011: ¥700,000 (Direct Cost: ¥700,000)
Fiscal Year 2010: ¥700,000 (Direct Cost: ¥700,000)
Keywords成層圏硫酸エアロゾル / 硫化カルボニル / 二酸化硫黄 / 硫黄同位体 / 質量非依存分別 / 波長依存同位体分別 / プルームモデル / 寒冷化 / 質量非依存同位体分別 / 硫黄循環 / 吸収断面積 / 光化学チャンバー
Research Abstract

本年度は、前年度までに達成した硫化カルボニル(OCS)の消失反応である光解離、酸素ラジカル、OHラジカルによる同位体分別を学術論文に発表し、さらに素過程における分別を考慮したモデルを用いて成層圏大気化学を考察した。その結果、同位体のマスバランスより、バックグラウンド成層圏硫酸エアロゾルの起源としてOCSは矛盾しないことを明らかにした。また、前年度に実験によって求めたOCSの光解離における波長依存同位体分別を、第一原理計算を用いた再現することに成功し、結果として発表した実験結果と相補的な結果を得た。さらに、理論計算からもOCS光解離は質量非依存分別を引き起こさないことも明らかとなり、現世の酸化的大気で観測される硫黄の質量非依存分別にはOCS由来の硫黄化合物は関与していないことが示唆された。
また、大規模火山噴火の際に生じる成層圏硫酸エアロゾルに関する研究でも成果を得た。本年度は、二酸化硫黄(SO_2)の光励起領域の紫外線吸収断面積の計測結果を共同で学術誌に発表した。その結果を組み込んだ火山噴煙のプルームモデルを用いることで、成層圏での大気化学反応により硫酸の硫黄安定同位体比が変化するメカニズムの解明に成功した。この結果、SO_2の光励起反応によって引き起こされる質量非依存分別によって極域の雪やアイスコアの記録を初めて再現した。今後、硫黄同位体記録を用いた火山噴火の規模や気候への影響の定量的な復元への展開が期待される。以上の結果を米国アカデミー紀要に発表し、プレスリリースを行った。

Report

(3 results)
  • 2012 Annual Research Report
  • 2011 Annual Research Report
  • 2010 Annual Research Report
  • Research Products

    (37 results)

All 2013 2012 2011 2010 Other

All Journal Article (11 results) (of which Peer Reviewed: 11 results) Presentation (25 results) Remarks (1 results)

  • [Journal Article] SO_2 photoexcitation mechanism links mass-independent sulfur isotopic fractionation in cryospheric sulfate to climate impacting volcanism2013

    • Author(s)
      Hattori, et al.
    • Journal Title

      Proc. Natl. Acad. Sci. USA

      Volume: (印刷中) Issue: 44 Pages: 4-5

    • DOI

      10.1073/pnas.1213153110

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Hydrogen and carbon isotope fractionation by thermophilic hydrogenotrophic methanogens from a deep aquifer under coculture with fermenters2012

    • Author(s)
      Hattori, et al.
    • Journal Title

      GEOCHEMICAL JOURNAL

      Volume: 46 Issue: 3 Pages: 193-200

    • DOI

      10.2343/geochemj.1.0161

    • NAID

      10030973363

    • ISSN
      0016-7002, 1880-5973
    • Year and Date
      2012-06-20
    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Isotope Effect in the Carbonyl Sulfide Reaction with O(^3P)2012

    • Author(s)
      Hattori, et al.
    • Journal Title

      J. Phys. Chem. A

      Volume: 116 Issue: 14 Pages: 3521-3526

    • DOI

      10.1021/jp2120884

    • Related Report
      2012 Annual Research Report 2011 Annual Research Report
    • Peer Reviewed
  • [Journal Article] An isotope analysis of ionising radiation as a source of sulphuric acid2012

    • Author(s)
      Enghoff, et al.
    • Journal Title

      Atmos. Chem. Phys.

      Volume: 12 Issue: 12 Pages: 5319-5327

    • DOI

      10.5194/acp-12-5319-2012

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Seasonal change, in microbial sulfur cycling in monomictic Lake Fukami-ike, Japan,2012

    • Author(s)
      Nakagawa, et al.
    • Journal Title

      Limnol. Oceanogr.

      Volume: 57(4) Issue: 4 Pages: 974-988

    • DOI

      10.4319/lo.2012.57.4.0974

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Photoabsorption cross-section measurements of ^<32>S, ^<33>S, ^<34>S and ^<36>S sulfur dioxide for the B^1B_1-X^1A_1 absorption band2012

    • Author(s)
      Danielache, et al.
    • Journal Title

      J. Geophys. Res. Atmos.

      Volume: 117

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] OCS photolytic isotope effects from first principles: sulfur and carbon is otopes, temperature dependence and implications for the stratosphere2012

    • Author(s)
      Schmidt, et al.
    • Journal Title

      Atmos. Chem. Phys.

      Volume: 13 Issue: 3 Pages: 1511-1520

    • DOI

      10.5194/acp-13-1511-2013

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] An isotope view on ionising radiation as a source of sulphuric acid2012

    • Author(s)
      Enghoff, et al
    • Journal Title

      Atmospheric Chemistry and Physics Discussions

      Volume: 12 Pages: 5039-5064

    • DOI

      10.5194/acpd-12-5039-2012

    • Related Report
      2011 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Prediction of the sulfur and carbon kinetic isotope effects in the OH+OCS reaction2012

    • Author(s)
      Schimidt, et al
    • Journal Title

      Chemical Physics Letter

      Volume: 531 Pages: 64-69

    • DOI

      10.1016/j.cplett.2012.02.049

    • Related Report
      2011 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Ultraviolet absorption cross sections of carbonyl sulfide isotopologues OC^<32>S, OC^<33>S, OC^<34>S, and O^<13>CS : isotopic fractionation in photolysis and at mospheric implications2011

    • Author(s)
      Shohei Hattori, et al
    • Journal Title

      Atmospheric Chemistry and Physics

      Volume: 11 Issue: 19 Pages: 10293-10303

    • DOI

      10.5194/acp-11-10293-2011

    • Related Report
      2011 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Isotopomer analysis of production and consumption mechanisms of N_2O and CH_4 in an advanced wastewater treatment system2011

    • Author(s)
      Sakae Toyoda, Yuuri Suzuki, Shohei Hattori, Keita Yamada, Ayako Fujii, Naohiro Yoshida, Rina, Kouno, Kouki Murayama, Hiroshi Shiomi
    • Journal Title

      Environmental Science and Technology

      Volume: 45 Pages: 917-922

    • Related Report
      2010 Annual Research Report
    • Peer Reviewed
  • [Presentation] 二酸化硫黄の光励起反応は大規模火山噴火後の成層圏硫酸エアロゾルに見られる硫黄-MIFを説明できるか2012

    • Author(s)
      服部祥平、ヨハンシュミット、マシュージョンソン、セバスチアンダニエラチエ、山田明憲、上野雄一郎、吉田尚弘
    • Organizer
      第59回日本地球化学会年会
    • Place of Presentation
      九州大学、福岡
    • Year and Date
      2012-09-13
    • Related Report
      2012 Annual Research Report
  • [Presentation] Vertical distribution of concentration and isotopomer ratios of N2O in tea field in Shizuoka,Japan2012

    • Author(s)
      Zou, et al.
    • Organizer
      第59回日本地球化学会年会
    • Place of Presentation
      九州大学、福岡
    • Year and Date
      2012-09-12
    • Related Report
      2012 Annual Research Report
  • [Presentation] 土壌凍結地帯における土壌中でのN_2O生成動態の解明2012

    • Author(s)
      柳井洋介、山崎哲明、服部祥平、豊田栄、吉田尚弘、岩田幸良、廣田知良
    • Organizer
      日本土壌肥料学会全国大会
    • Place of Presentation
      鳥取大学、鳥取
    • Year and Date
      2012-09-05
    • Related Report
      2012 Annual Research Report
  • [Presentation] SEASONALCHANGE IN MICROBIAL SULFUR CYCLING IN MONOMICTIC LAKE FUKAMI-IKE, JAPAN2012

    • Author(s)
      Nakagawa, et al.
    • Organizer
      Aquatic Sciences Meeting
    • Place of Presentation
      琵琶湖、滋賀県
    • Year and Date
      2012-07-11
    • Related Report
      2012 Annual Research Report
  • [Presentation] Isotopic fractionation in OCS sink reactions and implication for the source of background stratospheric sulfate aerosols2012

    • Author(s)
      Hattori, et al.
    • Organizer
      6th International Symposium on Isotopomers
    • Place of Presentation
      Washington D.C.
    • Year and Date
      2012-06-22
    • Related Report
      2012 Annual Research Report
  • [Presentation] Accurate photolytic isotope effects from first principles2012

    • Author(s)
      Schimidt, et al.
    • Organizer
      6th International Symposium on Isotopomers
    • Place of Presentation
      Washington D.C.
    • Year and Date
      2012-06-22
    • Related Report
      2012 Annual Research Report
  • [Presentation] Ultraviolet spectroscopy of 32S, 33S, 34S and 36S sulfur dioxide: fractionation by photoexcitation2012

    • Author(s)
      Danielache, et al.
    • Organizer
      6th International Symposium on Isotopomers
    • Place of Presentation
      Washington D.C.
    • Year and Date
      2012-06-22
    • Related Report
      2012 Annual Research Report
  • [Presentation] An isotope view on ionizing radiation as a source of sulphuric acid2012

    • Author(s)
      Enghoff, et al.
    • Organizer
      6th International Symposium on Isotopomers
    • Place of Presentation
      Washington D.C.
    • Year and Date
      2012-06-22
    • Related Report
      2012 Annual Research Report
  • [Presentation] Isotopomer analysis of N2O accumulated in teac field soil in Shizuoka, Central Japan2012

    • Author(s)
      Zou, et al.
    • Organizer
      6th International Symposium on Isotopomers
    • Place of Presentation
      Washington D.C.
    • Year and Date
      2012-06-22
    • Related Report
      2012 Annual Research Report
  • [Presentation] SO_2 photoexcitation explains mass-independent fractionation in present-day stratospheric sulfate2012

    • Author(s)
      Hattori, et al.
    • Organizer
      6th International Symposium on Isotopomers
    • Place of Presentation
      Washington D.C.
    • Year and Date
      2012-06-21
    • Related Report
      2012 Annual Research Report
  • [Presentation] An isotope view on ionising radiation as a source of sulphuric acid2012

    • Author(s)
      Enghoff, Bork, 服部祥平
    • Organizer
      地球惑星連合大会
    • Place of Presentation
      幕張メッセ、千葉(招待講演)
    • Year and Date
      2012-05-25
    • Related Report
      2012 Annual Research Report
  • [Presentation] An isotope view on ionising radiation as a source of sulphuric acid2012

    • Author(s)
      Enghoff M., et al
    • Organizer
      The 2^<nd> Nagoya Workshop on the Relationship between Solar Activity and Climate Changes
    • Place of Presentation
      名古屋大学
    • Year and Date
      2012-01-16
    • Related Report
      2011 Annual Research Report
  • [Presentation] 硫化カルボニルの分解時同位体分別から考える、成層圏硫酸エアロゾルへの寄与2011

    • Author(s)
      Shohei Hattori, et al
    • Organizer
      第17回大気化学討論会
    • Place of Presentation
      京都大学
    • Year and Date
      2011-10-19
    • Related Report
      2011 Annual Research Report
  • [Presentation] 大気光化学リアクターを用いた硫化カルボニルと酸素ラジカル(O(^3P))の反応とその同位体分別2011

    • Author(s)
      Shohei Hattori, et al
    • Organizer
      第17回大気化学討論会
    • Place of Presentation
      京都大学
    • Year and Date
      2011-10-19
    • Related Report
      2011 Annual Research Report
  • [Presentation] 硫化カルボニルの光解離反応における波長依存同位体分別、その理論的な理解と大気への応用2011

    • Author(s)
      Shohei Hattori, et al
    • Organizer
      日本地球化学会第58回年会
    • Place of Presentation
      北海道大学
    • Year and Date
      2011-09-15
    • Related Report
      2011 Annual Research Report
  • [Presentation] 硫化カルボニルの酸素ラジカル(O(^3P))による分解時同位体分別2011

    • Author(s)
      Shohei Hattori, et al
    • Organizer
      日本地球化学会第58回年会
    • Place of Presentation
      北海道大学
    • Year and Date
      2011-09-15
    • Related Report
      2011 Annual Research Report
  • [Presentation] Ultraviolet absorption cross sections of carbonyl sulfide isotopologues : Sulfur isotopic fractionation and its implication2011

    • Author(s)
      Shohei Hattori, et al
    • Organizer
      Tenth Informal Conference on Atmospheric and Molecular Science
    • Place of Presentation
      Copenhagen, Denmark
    • Year and Date
      2011-06-09
    • Related Report
      2011 Annual Research Report
  • [Presentation] Sulfur isotope fractionations in carbonyl sulfide sink reations in atmosphere2011

    • Author(s)
      Shohei Hattori, et al
    • Organizer
      地球惑星連介大会2011
    • Place of Presentation
      幕張、千葉
    • Year and Date
      2011-05-23
    • Related Report
      2011 Annual Research Report
  • [Presentation] Ultraviolet absorption cross sections of isotopically substituted carbonyl sulfide species : OC^<32>S, OC^<33>S, OC^<34>S, and O^<13>CS2011

    • Author(s)
      Shohei Hattori, et al
    • Organizer
      European Geoscience Union General Assembly
    • Place of Presentation
      Vienna, Austria
    • Year and Date
      2011-04-05
    • Related Report
      2011 Annual Research Report
  • [Presentation] 硫化カルボニルの硫黄同位体比及び分解時同位体分別係数に着目した、成層圏硫酸エアロゾル生成過程の推定2010

    • Author(s)
      服部祥平、上野雄一郎、ダニエラチェ セバスチアン、豊田栄、中川麻悠子、ジョンソンSマット、吉田尚弘
    • Organizer
      第16回大気化学討論会
    • Place of Presentation
      首都大学東京
    • Year and Date
      2010-11-17
    • Related Report
      2010 Annual Research Report
  • [Presentation] 成層圏エアロゾル2010

    • Author(s)
      Sebastian Danielache、服部祥平、吉川知里、上野雄一郎、Matthew Johnson、吉田尚弘
    • Organizer
      日本地球化学会2010年会
    • Place of Presentation
      立正大学熊谷キャンパス
    • Year and Date
      2010-09-08
    • Related Report
      2010 Annual Research Report
  • [Presentation] Isotopomer analysis of production/consumption mechanisms of nitrous oxide2010

    • Author(s)
      Sakae Toyoda, Yuuri Suzuki, Shohei Hattori, Keita Yamada, Ayako Fujii, Naohiro Yoshida, Rina Kouno, Kouki Murayama, Hiroshi Shiomi
    • Organizer
      5^<th> International Symposium on Isotopomers
    • Place of Presentation
      オランダ アムステルダム
    • Year and Date
      2010-06-23
    • Related Report
      2010 Annual Research Report
  • [Presentation] Hydrogen and carbon isotope fractionation by thermophilic hydrogenotrophic methanogens from a geothermal aquifer under coculture with fermenters2010

    • Author(s)
      Shohei Hattori, Hiroaki Nashimoto, Hiroyuki Kimura, Keisuke Koba, Keita Yamada, Mikio Shimizu, Hiroshi Watanabe, Muneoki Yoh, Naohiro Yoshida
    • Organizer
      5^<th> International Symposium on Isotopomers
    • Place of Presentation
      オランダ アムステルダム
    • Year and Date
      2010-06-22
    • Related Report
      2010 Annual Research Report
  • [Presentation] Sulfur mass balances and microbial metabolisms in a sulfur rich monomictic lake : A case study of the Lake Fukami-ike2010

    • Author(s)
      Mayuko Nakagawa, Yuichiro Ueno, Shohei Hattori, Maki Umemura, Akihiko Yagi, Ken Takai, Keisuke Koba, Akiko Makabe, Yuji Sasaki, Naohiro Yoshida
    • Organizer
      5^<th> International Symposium on Isotopomers
    • Place of Presentation
      オランダ アムステルダム
    • Year and Date
      2010-06-22
    • Related Report
      2010 Annual Research Report
  • [Presentation] Isotopomer analysis of N_2O emitted from a sesonally frozen soil,(凍結土壌から生じるN_2Oの安定同位体解析)2010

    • Author(s)
      Tetsuaki Yamazaki, Shohei Hattori, Yosuke Yanai, Sakae Toyoda, Naohiro Yoshida
    • Organizer
      International Symposium : Technology and Policy for Low Carbon Society,低炭素社会への道『省エネルギー、排出削減の技術と政策』国際シンポジウム
    • Place of Presentation
      Tsinghua University, Beijing, China
    • Related Report
      2010 Annual Research Report
  • [Remarks] 研究最前線「地球寒冷化を引き起こす大規模火山噴火の特定が可能に」

    • URL

      http://www.titech.ac.jp/topics/news/detail_3593.html

    • Related Report
      2012 Annual Research Report

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Published: 2010-12-03   Modified: 2024-03-26  

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