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Formation Mechanism and Emission Control of Persistent Organohalogen Compounds at Low Temperatures

Research Project

Project/Area Number 17H01891
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field Environmental engineering and reduction of environmental burden
Research InstitutionHokkaido University

Principal Investigator

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

Project Period (FY) 2017-04-01 – 2020-03-31
Project Status Completed (Fiscal Year 2019)
Budget Amount *help
¥18,200,000 (Direct Cost: ¥14,000,000、Indirect Cost: ¥4,200,000)
Fiscal Year 2019: ¥4,680,000 (Direct Cost: ¥3,600,000、Indirect Cost: ¥1,080,000)
Fiscal Year 2018: ¥4,680,000 (Direct Cost: ¥3,600,000、Indirect Cost: ¥1,080,000)
Fiscal Year 2017: ¥8,840,000 (Direct Cost: ¥6,800,000、Indirect Cost: ¥2,040,000)
Keywords環境技術 / 環境対応 / 有害化学物質 / 表面・界面物性
Outline of Final Research Achievements

To understand the formation mechanism of organic chlorides by the reaction of HCl with carbonaceous particles, we used molecular orbital calculations for three carbon active site models (Armchair, Zigzag, and Tip types) to examine the effect of Zn doping on HCl adsorption. The molecular models of the carbon materials with or without Zn doping showed that the presence of Zn element increased the number of carbon active sites available for the chemical adsorption of HC. Furthermore, Zn doping changed the electronic state of the activesite of the carbon particle in the direction in which HCl was readily adsorbed. We also examined the HCl removal performance of cheap natural soda ash loaded on a honeycomb support as a hot gas cleanup method. The honeycomb-supported soda ash improved HCl removal extent at the 1-ppm breakthrough time compared to the result without the support. Under the present conditions, the removal extent was maximized at 500℃.

Academic Significance and Societal Importance of the Research Achievements

本研究では、分子軌道計算法を用いZnをドープした炭素のモデル構造の電子状態を調べ、Znにより電子が局在化する部分を特定する一方、HCl吸着種の安定性を明らかにし、また、有機塩素種の塩素源の1つであるHClの除去を目的に、安価で資源量が豊富な天然ソーダ灰をハニカムに担持したNaベース吸収剤を製造し、その高いHCl除去性能を見出した。本成果により、HClによる未燃炭素粒子からの有機塩素化合物の発生を防止する手法の開発や有害化合物を発生させない添加剤などの開発が可能となり、学術的にも社会的にも意義の高い研究と言える。

Report

(4 results)
  • 2019 Annual Research Report   Final Research Report ( PDF )
  • 2018 Annual Research Report
  • 2017 Annual Research Report
  • Research Products

    (30 results)

All 2020 2019 2018 2017 Other

All Int'l Joint Research (1 results) Journal Article (15 results) (of which Int'l Joint Research: 1 results,  Peer Reviewed: 9 results) Presentation (13 results) (of which Int'l Joint Research: 6 results,  Invited: 1 results) Remarks (1 results)

  • [Int'l Joint Research] モンゴル国立大学(モンゴル)

    • Related Report
      2017 Annual Research Report
  • [Journal Article] Removal of Hydrogen Chloride Gas Using Honeycomb-Supported Natural Soda Ash2020

    • Author(s)
      Naoto Tsubouchi, Natsumi Matsuoka, Ken Fukuyama, Yuuki Mochizuki
    • Journal Title

      Chemical Engineering Research and Design

      Volume: 156 Pages: 138-145

    • DOI

      10.1016/j.cherd.2020.01.012

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] High Performance of Honeycomb-Supported Natural Soda Ash in the Removal of Hydrogen Chloride Gas2020

    • Author(s)
      Naoto Tsubouchi, Natsumi Matsuoka, Ken Fukuyama, Yuuki Mochizuki
    • Journal Title

      Abstracts of Papers of the American Chemical Society

      Volume: 259

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] ハニカム担持天然ソーダ灰を用いる石炭ガス化燃料ガス中の塩化水素ガスの除去2020

    • Author(s)
      望月友貴、福山健、松岡夏実、坪内直人
    • Journal Title

      第20回北海道エネルギー資源環境研究発表会論文集

      Volume: 20 Pages: 29-30

    • Related Report
      2019 Annual Research Report
  • [Journal Article] Quantum Chemical Study on Adsorption of Hydrogen Chloride with Zn-Doped Carbon Materials2019

    • Author(s)
      Yuji Shinohara, Naoto Tsubouchi
    • Journal Title

      Abstracts of the 18th Asian Pacific Confederation of Chemical Engineering Congress

      Volume: 18

    • Related Report
      2019 Annual Research Report
  • [Journal Article] ハニカム担持天然ソーダ灰を用いる燃料ガス中の塩化水素ガスの除去2019

    • Author(s)
      望月友貴、福山健、松岡夏実、坪内直人
    • Journal Title

      第56回石炭科学会議発表論文集

      Volume: 56 Pages: 84-85

    • Related Report
      2019 Annual Research Report
  • [Journal Article] Formation of Surface Chlorine Species by Low Temperature Reaction of HCl with Metal-Doped Carbon2019

    • Author(s)
      Naoto Tsubouchi, Yuuki Mochizuki, Yuji Shinohara, Akiyuki Kawashima, Yasuo Ohtsuka
    • Journal Title

      Fuel

      Volume: 246 Pages: 51-59

    • DOI

      10.1016/j.fuel.2019.02.084

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 塩化水素とZnドープ炭素物質の反応に関する量子化学的研究2019

    • Author(s)
      篠原祐治、坪内直人
    • Journal Title

      第19回北海道エネルギー資源環境研究発表会論文集

      Volume: 19 Pages: 51-52

    • Related Report
      2018 Annual Research Report
  • [Journal Article] Low-Temperature Reactions of HCl with Metal-Doped Carbon2018

    • Author(s)
      Naoto Tsubouchi, Yuuki Mochizuki, Yuji Shinohara, Akiyuki Kawashima, Yasuo Ohtsuka
    • Journal Title

      Energy & Fuels

      Volume: 32 Issue: 6 Pages: 6970-6977

    • DOI

      10.1021/acs.energyfuels.8b01165

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Some Factors Controlling the Formation of Hexachlorobenzene in the Process of Electric Arc Furnace Steelmaking2018

    • Author(s)
      Naoto Tsubouchi, Yasuo Ohtsuka
    • Journal Title

      Abstracts of Papers of the American Chemical Society

      Volume: 256

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Removal of Hydrogen Chloride Gas Using Natural Soda Ash2018

    • Author(s)
      Naoto Tsubouchi, Natsumi Matsuoka, Yuuki Mochizuki
    • Journal Title

      Proceedings of the 14th Japan-China Symposium on Coal and C1 Chemistry

      Volume: 14

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] ナトリウム担持褐炭に対する量子化学的検討2018

    • Author(s)
      篠原祐治、坪内直人
    • Journal Title

      第18回北海道エネルギー資源環境研究発表会論文集

      Volume: 18 Pages: 21-22

    • Related Report
      2017 Annual Research Report
  • [Journal Article] Catalytic Performance of Limonite Ores in the Decomposition of Model Compounds of Biomass-Derived Tar2017

    • Author(s)
      Naoto Tsubouchi, Yuuki Mochizuki, Enkhsaruul Byambajav, Satoko Takahashi, Yuu Hanaoka, Yasuo Ohtsuka
    • Journal Title

      Energy & Fuels

      Volume: 31 Issue: 4 Pages: 3898-3904

    • DOI

      10.1021/acs.energyfuels.7b00192

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Halogen Chemistry in Coal Utilization2017

    • Author(s)
      Naoto Tsubouchi
    • Journal Title

      Proceedings of the 2nd ISIJ-VDEh-Jernkontoret Joint Symposium

      Volume: 2 Pages: 119-123

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Release and Retention of the Chlorine in Coal during Pyrolysis and Gasification Processes2017

    • Author(s)
      Javzandolgor Bud, Yuuki Mochizuki, Naoto Tsubouchi
    • Journal Title

      Proceedings of the 17th Asian Pacific Confederation of Chemical Engineering Congress

      Volume: 17 Pages: 72-72

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 石炭乾留時における塩化水素の生成に及ぼす諸因子の検討2017

    • Author(s)
      坪内直人、望月友貴
    • Journal Title

      材料とプロセス

      Volume: 174 Pages: 662-662

    • Related Report
      2017 Annual Research Report
  • [Presentation] High Performance of Honeycomb-Supported Natural Soda Ash in the Removal of Hydrogen Chloride Gas2020

    • Author(s)
      Naoto Tsubouchi, Natsumi Matsuoka, Ken Fukuyama, Yuuki Mochizuki
    • Organizer
      The 259th American Chemical Society National Meeting
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] ハニカム担持天然ソーダ灰を用いる石炭ガス化燃料ガス中の塩化水素ガスの除去2020

    • Author(s)
      望月友貴、福山健、松岡夏実、坪内直人
    • Organizer
      第20回北海道エネルギー資源環境研究発表会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Quantum Chemical Study on Adsorption of Hydrogen Chloride with Zn-Doped Carbon Materials2019

    • Author(s)
      Yuji Shinohara, Naoto Tsubouchi
    • Organizer
      The 18th Asian Pacific Confederation of Chemical Engineering Congress
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 塩化水素と亜鉛ドープ炭素物質の反応による有機塩素種の生成に関する量子化学的研究2019

    • Author(s)
      篠原祐治、坪内直人
    • Organizer
      第9回エネルギー・マテリアル融合領域シンポジウム
    • Related Report
      2019 Annual Research Report
  • [Presentation] ハニカム担持天然ソーダ灰を用いる燃料ガス中の塩化水素ガスの除去2019

    • Author(s)
      望月友貴、福山健、松岡夏実、坪内直人
    • Organizer
      第56回石炭科学会議
    • Related Report
      2019 Annual Research Report
  • [Presentation] 塩化水素とZnドープ炭素物質の反応に関する量子化学的研究2019

    • Author(s)
      篠原祐治、坪内直人
    • Organizer
      第19回北海道エネルギー資源環境研究発表会
    • Related Report
      2018 Annual Research Report
  • [Presentation] Some Factors Controlling the Formation of Hexachlorobenzene in the Process of Electric Arc Furnace Steelmaking2018

    • Author(s)
      Naoto Tsubouchi, Yasuo Ohtsuka
    • Organizer
      The 256th American Chemical Society National Meeting
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Removal of Hydrogen Chloride Gas Using Natural Soda Ash2018

    • Author(s)
      Naoto Tsubouchi, Natsumi Matsuoka, Yuuki Mochizuki
    • Organizer
      The 14th Japan-China Symposium on Coal and C1 Chemistry
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] ナトリウム担持褐炭に対する量子化学的検討2018

    • Author(s)
      篠原祐治、坪内直人
    • Organizer
      第18回北海道エネルギー資源環境研究発表会
    • Related Report
      2017 Annual Research Report
  • [Presentation] 地球環境問題の解決を目指した次世代型石炭利用法の開発2018

    • Author(s)
      坪内直人
    • Organizer
      第7回エネルギー・マテリアル融合領域シンポジウム
    • Related Report
      2017 Annual Research Report
  • [Presentation] Halogen Chemistry in Coal Utilization2017

    • Author(s)
      Naoto Tsubouchi
    • Organizer
      The 2nd ISIJ-VDEh-Jernkontoret Joint Symposium
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Release and Retention of the Chlorine in Coal during Pyrolysis and Gasification Processes2017

    • Author(s)
      Javzandolgor Bud, Yuuki Mochizuki, Naoto Tsubouchi
    • Organizer
      The 17th Asian Pacific Confederation of Chemical Engineering Congress
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 石炭乾留時における塩化水素の生成に及ぼす諸因子の検討2017

    • Author(s)
      坪内直人、望月友貴
    • Organizer
      日本鉄鋼協会第174回秋季講演大会
    • Related Report
      2017 Annual Research Report
  • [Remarks] エネルギー変換システム設計研究室ホームページ

    • URL

      https://labs.eng.hokudai.ac.jp/labo/carem/lcec/

    • Related Report
      2019 Annual Research Report 2018 Annual Research Report 2017 Annual Research Report

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Published: 2017-04-28   Modified: 2021-02-19  

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