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Reactions of Hydrogen Halides with Carbonaceous Materials during High Temperature Processes and the Formation of Halogenated Organic Compounds

Research Project

Project/Area Number 26281035
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypePartial Multi-year Fund
Section一般
Research Field Environmental engineering and reduction of environmental burden
Research InstitutionHokkaido University

Principal Investigator

TSUBOUCHI Naoto  北海道大学, 工学(系)研究科(研究院), 准教授 (90333898)

Co-Investigator(Renkei-kenkyūsha) MOCHIZUKI YUUKI  北海道大学, 大学院工学研究院, 特任助教 (90546087)
Project Period (FY) 2014-04-01 – 2017-03-31
Project Status Completed (Fiscal Year 2016)
Budget Amount *help
¥16,250,000 (Direct Cost: ¥12,500,000、Indirect Cost: ¥3,750,000)
Fiscal Year 2016: ¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2015: ¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2014: ¥7,930,000 (Direct Cost: ¥6,100,000、Indirect Cost: ¥1,830,000)
Keywords炭素系資源 / 高温プロセス / ハロゲン化水素 / 炭素活性サイト / 金属種 / 二次的反応 / 有機ハロゲン化合物 / 石炭 / 熱分解 / 燃焼 / ガス化 / フッ化水素 / 有機フッ素化合物 / 環境技術 / 環境対応 / 有害化学物質 / 表面・界面物性 / 塩化水素 / 有機塩素 / 微粉炭燃焼 / フライアッシュ / 有機フッ素種 / 表面カルシウム
Outline of Final Research Achievements

To elucidate secondary reactions of HCl during high-temperature industrial processes, a model carbon prepared from phenol resin is first O2-activated at 500℃ and then impregnated with CH3COOK, (CH3COO)2CaH2O, (CH3COO)2Cu or (CH3COO)2Zn2H2O. When the sample is exposed to a stream of 100 ppm HCl/N2 at 500℃, HCl can readily react with all carbon samples to produce surface chlorine species, and the extent of the reaction increases by metal doping. The X-ray photoelectron spectroscopy (XPS) measurements of the HCl-treated samples exhibit the distinct Cl 2p spectra, which can be identified to organic chlorine with pure carbon and to organic and inorganic chlorine with the Ca-, Cu- and Zn-doped carbons. These observations suggest that HCl evolved during high-temperature industrial processes may react secondarily with carbon active sites and mineral components (for example, Ca, Cu and Zn) in carbonaceous materials (for example, unburned carbon) to form organic and inorganic chlorine.

Report

(4 results)
  • 2016 Annual Research Report   Final Research Report ( PDF )
  • 2015 Annual Research Report
  • 2014 Annual Research Report
  • Research Products

    (15 results)

All 2016 2015

All Journal Article (8 results) (of which Peer Reviewed: 7 results,  Acknowledgement Compliant: 8 results) Presentation (7 results) (of which Int'l Joint Research: 3 results,  Invited: 1 results)

  • [Journal Article] Significant Evolution of Hydrogen Fluoride from Coal Chars after Apparently Complete Release of Carbon Dioxide2016

    • Author(s)
      Naoto Tsubouchi
    • Journal Title

      Energy & Fuels

      Volume: 30 Issue: 5 Pages: 4381-4383

    • DOI

      10.1021/acs.energyfuels.6b00591

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Fluorine Release and Retention during Fixed Bed Combustion of Pyrolyzed Coal Chars2016

    • Author(s)
      Naoto Tsubouchi
    • Journal Title

      Abstracts of Papers of the American Chemical Society

      Volume: 61 Pages: 750-751

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Fluorine Release and Retention in the Fixed Bed Combustion of Pyrolyzed Chars2016

    • Author(s)
      Naoto Tsubouchi
    • Journal Title

      Proceedings of the 11th European Conference on Coal Research and Its Applications

      Volume: 11

    • NAID

      110008067355

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Reactions of Hydrogen Chloride with Carbonaceous Materials and the Formation of Surface Chlorine Species2016

    • Author(s)
      Naoto Tsubouchi
    • Journal Title

      Energy & Fuels

      Volume: 30 Issue: 3 Pages: 2320-2327

    • DOI

      10.1021/acs.energyfuels.6b00015

    • Related Report
      2015 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Evolution of Hydrogen Fluoride during Coal Pyrolysis and Subsequent Char Combustion2015

    • Author(s)
      Naoto Tsubouchi
    • Journal Title

      Abstracts of Papers of the American Chemical Society

      Volume: 60 Pages: 583-584

    • NAID

      110007520659

    • Related Report
      2015 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] 塩化水素と炭素質物質の反応による表面塩素種の生成2015

    • Author(s)
      坪内 直人
    • Journal Title

      日本化学会北海道支部2015年夏季研究発表会講演要旨集

      Volume: 2015 Pages: 72-72

    • Related Report
      2015 Annual Research Report
    • Acknowledgement Compliant
  • [Journal Article] Chemical Characterization of Unburned Carbon in Coal Fly Ashes by Use of TPD/TPO and LRS Methods2015

    • Author(s)
      Naoto Tsubouchi
    • Journal Title

      Environmental Science & Technology

      Volume: 49 Issue: 8 Pages: 5189-5194

    • DOI

      10.1021/es506023r

    • Related Report
      2014 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Functional Forms of the Unburned Carbon Present in Coal Fly Ashes: Role of Surface Oxygen Species in the Formation of Organic Fluorine Forms on the Carbon Surface2015

    • Author(s)
      Naoto Tsubouchi
    • Journal Title

      Abstracts of Papers of the American Chemical Society

      Volume: 249

    • Related Report
      2014 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Presentation] Fluorine Release and Retention in the Fixed Bed Combustion of Pyrolyzed Chars2016

    • Author(s)
      Naoto Tsubouchi
    • Organizer
      The 11th European Conference on Coal Research & Its Applications
    • Place of Presentation
      University of Sheffield (UK)
    • Year and Date
      2016-09-05
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Fluorine Release and Retention during Fixed Bed Combustion of Pyrolyzed Coal Chars2016

    • Author(s)
      Naoto Tsubouchi
    • Organizer
      The 252nd American Chemical Society National Meeting (Division of Energy & Fuels)
    • Place of Presentation
      Pennsylvania Convention Center (USA)
    • Year and Date
      2016-08-22
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 石炭利用時の窒素と塩素の挙動2016

    • Author(s)
      坪内直人
    • Organizer
      日本鉄鋼協会製銑部会発表会
    • Place of Presentation
      新日鐵住金株式会社鹿島製鐵所人材育成センター (茨城県)
    • Year and Date
      2016-07-14
    • Related Report
      2016 Annual Research Report
    • Invited
  • [Presentation] Evolution of Hydrogen Fluoride during Coal Pyrolysis and Subsequent Char Combustion2015

    • Author(s)
      Naoto Tsubouchi
    • Organizer
      The 250th American Chemical Society National Meeting (Division of Energy & Fuels)
    • Place of Presentation
      Boston Convention & Exhibition Center (USA)
    • Year and Date
      2015-08-18
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 塩化水素と炭素質物質の反応による表面塩素種の生成2015

    • Author(s)
      坪内 直人
    • Organizer
      日本化学会北海道支部2015年夏季研究発表会
    • Place of Presentation
      北海道教育大学函館校 (北海道)
    • Year and Date
      2015-07-18
    • Related Report
      2015 Annual Research Report
  • [Presentation] Functional Forms of the Unburned Carbon Present in Coal Fly Ashes: Role of Surface Oxygen Species in the Formation of Organic Fluorine Forms on the Carbon Surface2015

    • Author(s)
      Naoto Tsubouchi
    • Organizer
      The 249th American Chemical Society National Meeting (Division of Environmental Chemistry)
    • Place of Presentation
      Colorado Convention Center (USA)
    • Year and Date
      2015-03-25
    • Related Report
      2014 Annual Research Report
  • [Presentation] Functional Forms of the Unburned Carbon Present in Coal Fly Ashes: Role of Surface Oxygen Species in the Formation of Organic Fluorine Forms on the Carbon Surface2015

    • Author(s)
      Naoto Tsubouchi
    • Organizer
      The 249th American Chemical Society National Meeting (Sci-Mix)
    • Place of Presentation
      Colorado Convention Center (USA)
    • Year and Date
      2015-03-23
    • Related Report
      2014 Annual Research Report

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Published: 2014-04-04   Modified: 2018-03-22  

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