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Crucial factors controlling the formation of halogenated organic compounds during high-temperature combustion proc esse s

Research Project

Project/Area Number 21681008
Research Category

Grant-in-Aid for Young Scientists (A)

Allocation TypeSingle-year Grants
Research Field Environmental technology/Environmental materials
Research InstitutionHokkaido University (2011)
Tohoku University (2009-2010)

Principal Investigator

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

Project Period (FY) 2009 – 2011
Project Status Completed (Fiscal Year 2011)
Budget Amount *help
¥25,870,000 (Direct Cost: ¥19,900,000、Indirect Cost: ¥5,970,000)
Fiscal Year 2011: ¥6,110,000 (Direct Cost: ¥4,700,000、Indirect Cost: ¥1,410,000)
Fiscal Year 2010: ¥7,280,000 (Direct Cost: ¥5,600,000、Indirect Cost: ¥1,680,000)
Fiscal Year 2009: ¥12,480,000 (Direct Cost: ¥9,600,000、Indirect Cost: ¥2,880,000)
Keywords高温プロセス / 塩化水素 / フッ化水素 / 炭素活性サイト / 有機ハロゲン化合物 / 鉱物質 / 微量金属 / 二次的反応 / 残留性有害有機ハロゲン化合物 / 炭紫活性サイト
Research Abstract

Six dust samples recovered from bag filters of electric arc furnaces for steelmaking or six fly ashes recovered from electrostatic precipitators in pulverized coal-fired power plants are characterized by use of XRD, SEM-EPMA, XPS and TPD techniques to examine several factors controlling the formation of organic halogen compounds in the steelmaking or coal combustion process, respectively. The dust samples contain 2. 1-6. 4 wt%-dry of carbon element, and some of the C can release CO_2 in the TPD up to 300℃to provide carbon active sites. The number is related closely to hexachlorobenzene(HCB) concentration of each dust. Further, it is suggested that the Zn present in the samples consists of ZnFe_2O_4, ZnO and surface ZnCO_3, and the dust with a larger content of the ZnCO_3 has a higher concentration of HCB. On the other hand, the ashes include 20-130цg/gg-dry and 0. 5-4. 2 wt%-dry of F and C elements, respectively, and these components are enriched at the outermost layer of the ash surface. The F consists of both inorganic and organic functionalities, and the proportion of the latter is as high as 84-93 mol%. The C has different types of surface oxygen species, such as carboxyl, lactone/acid anhydride and phenolic groups, and most of these groups decompose into CO_2 or CO up to 800℃to give carbon active sites. When the amount of the O-functional forms increases, the content of organic CF forms tends to increase almost linearly.

Report

(4 results)
  • 2011 Annual Research Report   Final Research Report ( PDF )
  • 2010 Annual Research Report
  • 2009 Annual Research Report
  • Research Products

    (39 results)

All 2012 2011 2010 2009

All Journal Article (23 results) (of which Peer Reviewed: 13 results) Presentation (16 results)

  • [Journal Article] Catalytic decomposition of N-containing heterocyclic compounds with highly dispersed iron nanoparticles on carbons2012

    • Author(s)
      Matsuyama, T.; Tsubouchi, N.; Ohtsuka, Y
    • Journal Title

      Journal of Molecular Catalysis A : Chemical

      Volume: 356 Pages: 14-19

    • Related Report
      2011 Final Research Report
    • Peer Reviewed
  • [Journal Article] Iron-catalyzed nitrogen removal as N_2 from PAN-derived activated carbon2012

    • Author(s)
      Ohshima, Y.; Tsubouchi, N.; Ohtsuka, Y
    • Journal Title

      Applied Catalysis B : Environmental

      Volume: 111-112 Pages: 614-620

    • Related Report
      2011 Final Research Report
    • Peer Reviewed
  • [Journal Article] Functional forms of nitrogen and sulfur in coals and fate of heteroatoms during coal carbonization2012

    • Author(s)
      Tsubouchi, N.; Mochizuki, Y.; Ono, Y.; Uebo, K
    • Journal Title

      Tetsu to Hagane-Journal of the Iron and Steel Institute of Japan

      Volume: 98 Pages: 161-169

    • NAID

      130002127290

    • Related Report
      2011 Final Research Report
    • Peer Reviewed
  • [Journal Article] Functional Forms of Nitrogen and Sulfur in Coals and Fate of Heteroatoms during Coal Carbonization2012

    • Author(s)
      Naoto Tsubouchi
    • Journal Title

      Tetsu-to-Hagane

      Volume: 98 Pages: 161-169

    • NAID

      130002127290

    • Related Report
      2011 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Catalytic Decomposition of Nitrogen-Containing Heterocyclic Compounds with Highly Dispersed Iron Nanoparticles on Carbons2012

    • Author(s)
      Tetsuya Matsuyama
    • Journal Title

      Journal of Molecular Catalysis A : Chemical

      Volume: 356 Pages: 14-19

    • Related Report
      2011 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Iron-Catalyzed Nitrogen Removal as N_2 from PAN-Derived Activated Carbon2012

    • Author(s)
      Yasuhiro Ohshima
    • Journal Title

      Applied Catalysis B : Environmental

      Volume: 111-112 Pages: 614-620

    • Related Report
      2011 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Decomposition of Pyrrole and Pyridine with Iron Catalysts Supported on Carbons2012

    • Author(s)
      Naoto Tsubouchi
    • Journal Title

      Preprints, American Chemical Society, Division of Fuel Chemistry

      Volume: 243(CD-ROM)

    • Related Report
      2011 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Chemical forms of the fluorine and carbon in fly ashes recovered from electrostatic precipitators of pulverized coal-fired plants2011

    • Author(s)
      Tsubouchi, N.; Hayashi, H.; Kawashi ma, A.; Sato, M.; Suzuki, N.; Ohtsuka, Y
    • Journal Title

      Fuel

      Volume: 90 Pages: 376-383

    • Related Report
      2011 Final Research Report
    • Peer Reviewed
  • [Journal Article] Secondary Reactions of HCl during Coal Pyrolysis : Studies on Reactions of HCl with Model Carbons2011

    • Author(s)
      Naoto Tsubouchi
    • Journal Title

      Proceedings, International Conference on Coal Science and Technology

      Volume: (CD-ROM)

    • Related Report
      2011 Annual Research Report
  • [Journal Article] Rapid In-Situ Steam Gasification of Low Rank Coal with Catalyst from Low-Cost Minerals2011

    • Author(s)
      Li-xin Zhang
    • Journal Title

      Proceedings, The 13th Cross Straits Symposium on Materials, Energy and Environmental Engineering

      Volume: 13(CD-ROM)

    • Related Report
      2011 Annual Research Report
  • [Journal Article] Catalytic Effects of Na and Ca from Inexpensive Materials on the Steam Gasification of Nascent Char from Rapid Pyrolysis of Low Rank Coal in a Drop Tube Reactor2011

    • Author(s)
      Li-xin Zhang
    • Journal Title

      Proceedings, The 11th China-Japan Symposium on Coal and C1 Chemistry

      Volume: 11(CD-ROM)

    • Related Report
      2011 Annual Research Report
  • [Journal Article] Catalytic Steam Gasification of Low Rank Coals Using Inexpensive Catalyst Resources2011

    • Author(s)
      Li-xin Zhang
    • Journal Title

      Proceedings, The 7th International Conference on Clean Coal Technology and Fuel Cells

      Volume: 7(CD-ROM)

    • Related Report
      2011 Annual Research Report
  • [Journal Article] Chemical Forms of the Fluorine and Carbon in Fly Ashes Recovered from Electrostatic Precipitators of Pulverized Coal-Fired Plants2011

    • Author(s)
      Naoto Tsubouchi
    • Journal Title

      Fuel

      Volume: 90 Pages: 376-383

    • Related Report
      2010 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 石炭の熱分解ならびにチャーのガス化過程における塩素とフッ素の行方2011

    • Author(s)
      坪内直人
    • Journal Title

      第11回北海道エネルギー資源環境研究発表会講演予稿集

      Volume: 11 Pages: 41-42

    • Related Report
      2010 Annual Research Report
  • [Journal Article] Chemical characterization of dust particles recovered from bag filters of electric arc furnaces for steelmaking : some factors influencing the formation of hexachlorobenzene2010

    • Author(s)
      Tsubo uchi, N.; Hashimoto, H.; Ohtaka, N.; Ohtsuka, Y
    • Journal Title

      Journal of Hazardous Materials

      Volume: 183 Pages: 116-124

    • Related Report
      2011 Final Research Report
    • Peer Reviewed
  • [Journal Article] Chemical Characterization of Dust Particles Recovered from Bag Filters of Electric Arc Furnaces for Steelmaking : Some Factors Influencing the Formation of Hexachlorobenzene2010

    • Author(s)
      Naoto Tsubouchi
    • Journal Title

      Journal of Hazardous Materials

      Volume: 183 Pages: 116-124

    • Related Report
      2010 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Leaching Behavior of the Boron and Fluorine in Fly Ashes Formed in Pulverized Coal Combustion2010

    • Author(s)
      Naoto Tsubouchi
    • Journal Title

      Journal of the Japan Institute of Energy

      Volume: 89 Pages: 1164-1171

    • NAID

      130004540955

    • Related Report
      2010 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Steam Gasification of Low Rank Coals with Ion-Exchanged Sodium Catalysts Prepared Using Natural Soda Ash2010

    • Author(s)
      Yuu Hanaoka
    • Journal Title

      Proceedings, The 27^<th> Annual International Pittsburgh Coal Conference

      Volume: 27(CD-ROM)

    • Related Report
      2010 Annual Research Report
  • [Journal Article] 石炭利用時のハロゲンのケミストリーの解明:熱分解チャーの燃焼過程におけるフッ素の脱離と濃縮2010

    • Author(s)
      坪内直人
    • Journal Title

      第10回多元物質科学研究所研究発表会講演予稿集

      Volume: 10 Pages: 111-111

    • Related Report
      2010 Annual Research Report
  • [Journal Article] 循環流動床を用いる低炭化度炭の水蒸気ガス化におけるCa触媒の効果2010

    • Author(s)
      松岡浩一
    • Journal Title

      第47回石炭科学会議発表論文集

      Volume: 47 Pages: 104-105

    • Related Report
      2010 Annual Research Report
  • [Journal Article] 熱分解チャーの燃焼過程におけるフッ素の脱離と濃縮2010

    • Author(s)
      坪内直人
    • Journal Title

      第47回石炭科学会議発表論文集

      Volume: 47 Pages: 56-57

    • Related Report
      2010 Annual Research Report
  • [Journal Article] Effects of Metal Cations Present Naturally in Coal on the Fate of Coal-Bound Nitrogen in the Fixed-Bed Pyrolysis of 25 Coals with Different Ranks : Correlation between Inherent Fe Cations and N_2 Formation from Low-Rank Coals2009

    • Author(s)
      Yasuo Ohtsuka
    • Journal Title

      Energy & Fuels 23

      Pages: 4774-4781

    • Related Report
      2009 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Formation of Hydrogen Fluoride during Coal Pyrolysis and Subsequent Char Combustion2009

    • Author(s)
      Naoto Tsubouchi
    • Journal Title

      Proceedings, The 10th Japan-China Symposium on Coal and C1 Chemistry 10

      Pages: 1-2

    • Related Report
      2009 Annual Research Report
  • [Presentation] Decomposition of Pyrrole and Pyridine with Iron Catalysts Supported on Carbons2012

    • Author(s)
      Naoto Tsubouchi
    • Organizer
      The 243rd American Chemical Society National Meeting
    • Place of Presentation
      San Diego Convention Center (USA)
    • Year and Date
      2012-03-27
    • Related Report
      2011 Annual Research Report
  • [Presentation] 石炭中の窒素と硫黄の化学形態と乾留過程での行方2012

    • Author(s)
      坪内直人
    • Organizer
      日本鉄鋼協会高温プロセス部会資源・エネルギーフォーラム講演会
    • Place of Presentation
      日本鉄鋼協会(東京都)(招待講演)
    • Year and Date
      2012-02-07
    • Related Report
      2011 Annual Research Report
  • [Presentation] アルゴンヌ標準炭中の塩素のファンクショナリティと熱分解時の形態変化2012

    • Author(s)
      坪内直人
    • Organizer
      第12回北海道エネルギー資源環境研究発表会
    • Place of Presentation
      北海道大学学術交流会館.
    • Year and Date
      2012-01-31
    • Related Report
      2011 Final Research Report
  • [Presentation] Rapid In-Situ Steam Gasification of Low Rank Coal with Catalyst from Low-Cost Minerals2011

    • Author(s)
      Li-xin Zhang
    • Organizer
      The 13th Cross Straits Symposium on Materials, Energy and Environmental Engineering
    • Place of Presentation
      九州大学筑紫キャンパス(福岡県)
    • Year and Date
      2011-11-23
    • Related Report
      2011 Annual Research Report
  • [Presentation] Catalytic Steam Gasification of Low Rank Coals Using Inexpensive Catalyst Resources2011

    • Author(s)
      Li-xin Zhang
    • Organizer
      The 7th International Conference on Clean Coal Technology and Fuel Cells
    • Place of Presentation
      九州大学筑紫キャンパス(福岡県)
    • Year and Date
      2011-11-09
    • Related Report
      2011 Annual Research Report
  • [Presentation] CO_2排出量の削減を目指したクリーン・コール・テクノロジーの開発2011

    • Author(s)
      坪内直人
    • Organizer
      日本鉄鋼協会コークス部会発表会
    • Place of Presentation
      JFEスチール西日本製鉄所(岡山県)(招待講演)
    • Year and Date
      2011-10-28
    • Related Report
      2011 Annual Research Report
  • [Presentation] Secondary Reactions of HCl during Coal Pyrolysis : Studies on Reactions of HCl with Model Carbons2011

    • Author(s)
      Naoto Tsubouchi
    • Organizer
      International Conference on Coal Science and Technology 2011
    • Place of Presentation
      Conference and Exhibition Centre Ciudad de Oviedo (Spain)
    • Year and Date
      2011-10-11
    • Related Report
      2011 Annual Research Report
  • [Presentation] Catalytic Effects of Na and Ca from Inexpensive Materials on the Steam Gasification of Nascent Char from Rapid Pyrolysis of Low Rank Coal in a Drop Tube Reactor2011

    • Author(s)
      Li-xin Zhang
    • Organizer
      The 11th China-Japan Symposium on Coal and C1 Chemistry
    • Place of Presentation
      Ningxia Yuehai Hotel (China)
    • Year and Date
      2011-08-04
    • Related Report
      2011 Annual Research Report
  • [Presentation] 石炭の熱分解ならびにチャーのガス化過程における塩素とフッ素の行方2011

    • Author(s)
      坪内直人
    • Organizer
      第11回北海道エネルギー資源環境研究発表会
    • Place of Presentation
      札幌
    • Year and Date
      2011-02-01
    • Related Report
      2010 Annual Research Report
  • [Presentation] 石炭利用時のハロゲンのケミストリーの解明:熱分解チャーの燃焼過程におけるフッ素の脱離と濃縮2010

    • Author(s)
      坪内直人
    • Organizer
      第10回多元物質科学研究所研究発表会
    • Place of Presentation
      仙台
    • Year and Date
      2010-12-01
    • Related Report
      2010 Annual Research Report
  • [Presentation] Steam Gasification of Low Rank Coals with Ion-Exchanged Sodium Catalysts Prepared Using Natural Soda Ash2010

    • Author(s)
      Yuu Hanaoka
    • Organizer
      The 27^<th> Annual International Pittsburgh Coal Conference
    • Place of Presentation
      Istanbul (Turkey)
    • Year and Date
      2010-10-14
    • Related Report
      2010 Annual Research Report
  • [Presentation] ヘテロ界面を用いる劣質・未利用炭素資源のコークス化鼓術の検討2010

    • Author(s)
      坪内直人
    • Organizer
      劣質・未利用炭素資源コークス化技術研究会討論会
    • Place of Presentation
      札幌
    • Year and Date
      2010-09-28
    • Related Report
      2010 Annual Research Report
  • [Presentation] 熱分解チャーの燃焼時におけるフッ素の脱離と濃縮2010

    • Author(s)
      坪内直人,赤間佑紀,大塚康夫
    • Organizer
      第47回石炭科学会議
    • Place of Presentation
      岐阜県長良川国際会議場
    • Year and Date
      2010-09-22
    • Related Report
      2011 Final Research Report
  • [Presentation] 循環流動床を用いる低炭化度炭の水蒸気ガス化におけるCa触媒の効果2010

    • Author(s)
      松岡浩一
    • Organizer
      第47回石炭科学会議
    • Place of Presentation
      岐阜
    • Year and Date
      2010-09-22
    • Related Report
      2010 Annual Research Report
  • [Presentation] 熱分解チャーの燃焼過程におけるフッ素の脱離と濃縮2010

    • Author(s)
      坪内直人
    • Organizer
      第47回石炭科学会議
    • Place of Presentation
      岐阜
    • Year and Date
      2010-09-22
    • Related Report
      2010 Annual Research Report
  • [Presentation] Formation of Hydrogen Fluoride during Coal Pyrolysis and Subsequent Char Combustion2009

    • Author(s)
      Naoto Tsubouchi
    • Organizer
      The 10th Japan-China Symposium on Coal and C1 Chemistry
    • Place of Presentation
      つくば国際会議場(茨城)
    • Year and Date
      2009-07-28
    • Related Report
      2009 Annual Research Report

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Published: 2009-04-01   Modified: 2016-04-21  

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