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A Novel Method of Removal of Nitrogen and Sulfur by Use of Nanoparticles Containing Composites Produced from Inexpensive Raw Materials

Research Project

Project/Area Number 11218202
Research Category

Grant-in-Aid for Scientific Research on Priority Areas

Allocation TypeSingle-year Grants
Review Section Science and Engineering
Research InstitutionTohoku University

Principal Investigator

OHTSUKA Yasuo  Tohoku University, IMRAM, Professor, 多元物質研究所, 教授 (20091663)

Co-Investigator(Kenkyū-buntansha) KIKUCHI Takemitsu  Tohoku Univ., IMRAM, Research Associate, 多元物質研究所, 助手 (30169825)
TSUBOUCHI Naoto  Tohoku Univ., IMRAM, Research Associate, 多元物質研究所, 助手 (90333898)
王 野  東北大学, 反応化学研究所, 助手 (40292304)
Project Period (FY) 1999 – 2002
Project Status Completed (Fiscal Year 2002)
Budget Amount *help
¥31,600,000 (Direct Cost: ¥31,600,000)
Fiscal Year 2002: ¥5,200,000 (Direct Cost: ¥5,200,000)
Fiscal Year 2001: ¥7,800,000 (Direct Cost: ¥7,800,000)
Fiscal Year 2000: ¥9,600,000 (Direct Cost: ¥9,600,000)
Fiscal Year 1999: ¥9,000,000 (Direct Cost: ¥9,000,000)
KeywordsNanoparticles / Carbon composites / Nitrogen removal / Sulfur removal / Hot gas cleanup / ナノ微粒子複合体 / 石炭
Research Abstract

This project has been performed to develop a novel method of removing nitrogen and sulfur by using nanoparticles containing composites, which are produced from inexpensive raw materials, from a viewpoint of hot gas cleanup for an integrated gasification combined cycle process. The main achievements are summarized as follows :
(1) Nanoscale Fe particles on coal chars, prepared by carbonizing brown coals with externally added Fe ions, show higher activity in the catalytic decomposition of NH_3 to N_2 than Fe catalyst loaded on a commercial activated carbon, when 2000 ppm NH_3 diluted with He is fed at a high space velocity of 45000 1/h.
(2) The TEM, XRD and TPD measurements strongly suggest that the highly dispersed Fe particles play the crucial role in NH_3 decomposition and catalyze this reaction through a cycle mechanism involving α-Fe and the nitride species
(3) Some chars, prepared by simply pyrolyzing low rank coals with significant amounts of Fe and Ca cations naturally present as minerals, also work efficiently as the catalysts, and there is a strong correlation between NH_3 conversion and Fe content in char.
(4) The char with the largest content (2 wt%) of inherent Fe provides the stable conversion of 80% during 25 h reaction at 750℃ and achieves complete decomposition of NH_3 at 850℃.
(5) When NH_3 decomposition is carried out in the presence of 2000 ppm H_2S, CaO in the char is completely deactivated to form CaS, but Fe particles in it are still active, showing that the char can realize the removal of sulfur compounds and the catalytic decomposition of NH_3 simultaneously.
(6) The coexistence of syngas, a mixture of CO and H_2 with the molar ratio of 2 : 1, lowers the activity of the Fe catalyst, whereas the addition of C0_2 to syngas restores the performance to the original state without syngas, which suggests that some chars can be utilized in an actual hot gas cleanup process.

Report

(5 results)
  • 2002 Annual Research Report   Final Research Report Summary
  • 2001 Annual Research Report
  • 2000 Annual Research Report
  • 1999 Annual Research Report
  • Research Products

    (12 results)

All Other

All Publications (12 results)

  • [Publications] Y.Ohtsuka, C.Xu, D.Kong, N.Tsubouchi: "Decomposition of ammonia with iron and calcium catalysts supported on coal chars"Fuel. 82(In press). (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Y.Ohtsuka, C.Xu, D.Kong, N.Tsubouchi: "High catalytic performances of low rank coal chars in ammonia decomposition at high temperatures"Amer. Chem. Soc. Div. Fuel Chem.. 48・1. 304-305 (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Y.Ohtsuka, C.Xw, D.Kong, N.Tsubouchi: "Catalytic decomposition of ammonia with iron nanoparticles supported on carbons"Amer. Chem. Soc. Div. Fuel Chem.. 46・1. 151-153 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] 多賀谷英幸, 進藤隆世志, 大塚康夫, 玉井康文, 門川淳一: "有機資源化学"朝倉書店. 150 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Y. Ohtsuka, C. Xu, D. Kong, N. Tsubouchi: "Decomposition of ammonia with iron and calcium catalysts supported on coal chars"Fuel. 82, in press. (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Y. Ohtsuka, C. Xu, D. Kong, N. Tsubouchi: "High catalytic performances of low rank coal chars in ammonia decomposition at high temperatures"Amer. Chem. Soc. Div. Fuel Chem.. 48(1). 304-305 (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Y. Ohtsuka, C. Xu, D. Kong, N. Tsubouchi: "Catalytic decomposition of ammonia with iron nanoparticles supported on carbons"Amer. Chem. Soc. Div. Fuel Chem.. 46(1). 151-153 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] H. Tagaya, T. Shindo, Y. Ohtsuka, Y. Tamai, J. Kadokawa: "Asakura Shoten"Organic Resources Chemistry. 150 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Y.Ohtsuka: "High catalytic performances of low rank coal chars in ammonia decomposition at high temperatures"Amer.Chem.Soc.Div. Fuel Chem.. 48(In press). (2003)

    • Related Report
      2002 Annual Research Report
  • [Publications] Y.Ohtsuka: "High temperature decomposition of ammonia with low rank coal chars"Amer. Chem. Soc. Div. Fuel Chem.. 47(2)(To be presented). (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] Y.Ohtsuka: "Catalytic decomposition of ammonia with iron nanoparticles supported on carbons"Amer. Chem. Soc. Div. Fuel Chem.. 46(1). 151-153 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] Y.Ohtsnka: "Catalytic decomposition of ammonia with iron rawpatzloy Supported on corbons"ACS,Dir.Frel Chem.. 46(in press). (2001)

    • Related Report
      2000 Annual Research Report

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Published: 1999-04-01   Modified: 2018-03-28  

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