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Compound-specific stable hydrogen isotope analysis of natural samples in nano-molar levels and its application to earth environmental sciences

Research Project

Project/Area Number 12359003
Research Category

Grant-in-Aid for Scientific Research (A)

Allocation TypeSingle-year Grants
Section展開研究
Research Field 広領域
Research InstitutionTOKYO METROPOLITAN UNIVERSITY

Principal Investigator

NARAOKA Hiroshi  TOKYO METROPOLITAN UNIVERSITY, Dept. Of Chemistry, Assoc.Prof. (20198386)

Co-Investigator(Kenkyū-buntansha) ブリンカット デビット  東京都立大学, 理学研究科, 助手 (60301412)
Project Period (FY) 2000 – 2002
Project Status Completed (Fiscal Year 2002)
Budget Amount *help
¥33,040,000 (Direct Cost: ¥31,900,000、Indirect Cost: ¥1,140,000)
Fiscal Year 2002: ¥2,080,000 (Direct Cost: ¥1,600,000、Indirect Cost: ¥480,000)
Fiscal Year 2001: ¥2,860,000 (Direct Cost: ¥2,200,000、Indirect Cost: ¥660,000)
Fiscal Year 2000: ¥28,100,000 (Direct Cost: ¥28,100,000)
KeywordsHydorgen isotope / Organic compounds / Sub-nano molar / Analytical development / Natural samples / Lipid molecules / Vegetation / Meteorite / 有機分子レベル / 堆積物 / アルカン / 脂肪酸 / アルコール / 多環芳香族炭化水素 / 水素同位体 / n-アルカン / 陸上高等植物 / 熱分解 / 拡張型同位体比質量分析計
Research Abstract

Compound-specific hydrogen isotope measurement has been developed at sub-nano molar level using gas chromatography/pyrolysis/isotope ratio mass spectrometry (GC/pyrolysis/IRMS). Isotopic calibration and sample preparation including derivatization of unvolatile compounds and separation of co-eluted compounds by silica gel chromatography were also established for more precise isotope measurement. Finally, it is successful to determine a OD value of natural samples with precision of less than 5‰ using ・0ng hydrogen-containing organic compound. We applied the established method to determine δD values of n-alkanes, n-alkanoic acids, n-alkanols and sterols of biological materials and sediments, in order to discuss their isotope fractionation mechanisms during different biosynthetic pathways as well as their source, diagenetic effects and transportation processes in sediments. We also conducted the δD measurement of polycyclic aromatic hydrocarbons such as pyrene and fluoranthene in carbonaceous chondrites to find different the δD value in spite of their structural isomers each other (C_<16>H_<10>). In addition, hydrogen isotope exchange of pyrene and fluoranthene occurred in hydrothermal solutions under acidic condition, where where hydrogens have exchanged more easily between pyrene and water relative to between fluoranthene and water. The kinetically different behavior between pyrene and fluoranthene coincides with the two-series (pyrene-series and fluoranthene-series) PAH formation mechanisms in carbonaceous chondrites inferred from carbon isotopic compositions of PAH.
Originally this reserch project was planned for 4 years (2000-2003 FY). However, since this project has successfully continued to a new research project as titled "Multi-stable isotope systematics of individual organic compounds in cosmogeochemical samples", this project ended up to make a final report.

Report

(4 results)
  • 2002 Annual Research Report   Final Research Report Summary
  • 2001 Annual Research Report
  • 2000 Annual Research Report
  • Research Products

    (31 results)

All 2003 2002 Other

All Journal Article (12 results) Book (1 results) Publications (18 results)

  • [Journal Article] Geochemical and organic carbon isotope studies across the continental Permian-Triassic boundary of Ranigay Basirn2003

    • Author(s)
      A.Sarkar, H.Yoshioka, ら
    • Journal Title

      Palaeogeogr. Palaeoclimat. Palaeoecol. 191

      Pages: 1-14

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Journal Article] Glacial-interglacial changes in organic carpon, nitrogen and sulfur accomulation in Lake Baikal sediment2003

    • Author(s)
      T.Watanabe, H.Naraoka, ら
    • Journal Title

      Geochemical Journal 37

      Pages: 493-502

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Journal Article] A different behavior of hydrogen isotope exchange petureen two PAH isomers (fluoranthene and pyrene)2003

    • Author(s)
      Y.Oba, H.Naraoka
    • Journal Title

      Res.Org.Geochem. 18

      Pages: 29-35

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Journal Article] Geochemical and organic carbon isotope studies across the continental Permean-Triassic boundary of Raniganj Basin, eastern India.2003

    • Author(s)
      A.Sarkar, H.Yoshioka, M.Ebihara, H.Naraoka
    • Journal Title

      Palaeogeogr. Palaeoclimat. Palaeoecol. 191

      Pages: 1-14

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Journal Article] Glacial- interglacial changes in organic carbon, nitrogen and sulfur accumulation in Lake Baikal sediment over the past 250 kyr.2003

    • Author(s)
      T.Watanabe, H.Naraoka, M.Kinoshita, M.Nishimura, T.Kawai
    • Journal Title

      Geochem.J. 37

      Pages: 493-502

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Journal Article] A different behavior of hydrogen isotope exchange between two PAH isomers (fluoranthene and pyrene).2003

    • Author(s)
      Y.Oba, H.Naraoka
    • Journal Title

      Res.Org.Geochem. 18

      Pages: 29-35

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Journal Article] Carbon isotope fractionation during permanganate oxidation of chlorinated ethylenes (cDCE. TCE. PCE)2002

    • Author(s)
      S.R.Poulson., H.Naraoka
    • Journal Title

      Environ, Science and Technology 36

      Pages: 3270-3274

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Journal Article] Vertical distributions and δ^<13>C Isotopic compositions of PAHs in Chidorigafuchi Moat sediment, Japan2002

    • Author(s)
      T.Okuda, H.Kumata, ら
    • Journal Title

      Organic Geochemistry 33

      Pages: 843-848

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Journal Article] 有機分子レベル安定水素同位体比測定と地球環境科学への応用2002

    • Author(s)
      奈良岡浩, 力石嘉人
    • Journal Title

      Radioisotopes 51

      Pages: 249-250

    • NAID

      10008637289

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Journal Article] Carbon isotope fractionation during permanganate oxidation of chlorinated ethylenes (cDCE, TCE, PCE).2002

    • Author(s)
      S.R.Poulson, H.Naraoka
    • Journal Title

      Environ.Sci.Tech. 36

      Pages: 3270-3274

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Journal Article] Vertical distributions and δ13^C isotopic compositions of PAHs in Chidorigafuchi Moat sediment, Japan.2002

    • Author(s)
      T.Okuda, H.Kumata, H.Naraoka, R.Ishiwatari, H.Takada
    • Journal Title

      Org.Geochem. 33

      Pages: 843-848

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Journal Article] Compound-specific hydrogen isotope analysis its application to earth environmental sciences (in Japanese).2002

    • Author(s)
      H.Naraoka, Y.Chikaraishi
    • Journal Title

      Radioisotopes. 51

      Pages: 249-250

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Book] 地球化学講座第4巻「有機地球化学」(分担)

    • Author(s)
      奈良岡浩
    • Publisher
      培風館(印刷中)
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] H.Naraoka, H.Mita: "δD of individual PAHs from the Murchison and an Antarctic carbonaceous chondrite"Geochim. Cosmochim. Acta, Spec. Suppl.. 66. A546 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] S.R.Poulson, H.Naraoka: "Carbon isotope fractionation during permanganate oxidation of chlorinated ethylenes (cDCE, TCE, PCE)"Enriromental Science and Technology. 36. 3270-3274 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] Y.Chikaraishi, H.Naraoka: "Compound-specific δD-δ^<13>C analyses of n-alkanes extracted from terrestrial and aquatic plants"Phytochemistry. (印刷中). (2003)

    • Related Report
      2002 Annual Research Report
  • [Publications] Y.Chikaraishi, H.Naraoka: "Hydrogen and carbon isotope fraqtionation during lipid biosynthesis of terrestrial plants"Geochim. Cosmochim. Acta, Spec. Suppl.. 66. A139 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] T.Okuda, H.Kumata: "Vertical distributions and δ^<13>C isotopic compositions of PAHs in Chidorigafuchi Moat sediment, Japan"Organic Geochemistry. 33. 843-848 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] 奈良岡浩, 力石嘉人: "分子レベル安定水素同位体比測定と地球環境科学への応用"Radio isotopes. 51. 249-250 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] 奈良岡浩(分担): "「地球化学講座」第8巻「地球化学実験法」A1章"培風館(印刷中). (2003)

    • Related Report
      2002 Annual Research Report
  • [Publications] Y.Chikaraishi, H.Naraoka: "Organic hydrogen-carbon isotope signatures of terrestrial higher plants during biosynthesis for distinctive photosynthetic pathways"Geochemical Journal. 35. 451-458 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] 奈良岡浩: "陸・海洋系における有機分子の安定炭素同位体組成とその起源"月刊海洋「現代海洋化学II」. 号外25. 210-215 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] T.Okuda: "Source identification of Malaysian atmospheric polycyclic aromatic hydrocarbons nearby forest fires using molecular and isotopic compositions"Atmospheric Environment. 36. 611-618 (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] Y.Chikaraishi, H.Naraoka: "Sources of long-chain n-alkanes at lake Haruna(Japan) based on their individuall stable hydrogen and carbon isotopic conpositions"Organic Geochemistry. (印刷中). (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] 奈良岡 浩: "「地球化学講座」第4巻「有機地球化学」第7章"培風館(印刷中). (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] H.Naraoka,A.Shimoyama ら: "Isotopic evidence from an Antarctic carbonaceous chondrite for two reaction pathways of extraterrestrial PAH formation"Earth and Planetary Science Letters. 184. 1-7 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] H.Naraoka,R,Ishiwatari: "Molecular and isotopic abundances of long-chain n-fatty acids in open marine sediments of the western north Pacific"Chemical Geology. 165. 23-36 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] H.Naraoka,K.Yamada ら: "Recent sedimentary hopanoids in the north western Pacific alongside Japanese Islands"Organic Geochemistry. 31. 1023-1029 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] D.Brincat,K.Yamada ら: "Molecular-isotopic stratigraphy of long chain n-alkanes in Lake Baikal Holocene and glacial age sediments"Organic Geochemistry. 31. 287-294 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] T.Okuda,H.Naraoka ら: "Separation of PAHs in environmental samples by use of solid-phase extraction system for carbon isotope analysis"J.Mass Spectrom.Soc.Japan. 48. 387-394 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] 力石嘉人,内藤卓,奈良岡浩: "有機物の水素-炭素同位体組成と地球化学サイクル"月刊海洋. 32. 570-575 (2000)

    • Related Report
      2000 Annual Research Report

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Published: 2000-04-01   Modified: 2016-04-21  

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