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Analysis of carbon deposition behavior in methane reforming in order to evaluate the catalyst life

Research Project

Project/Area Number 10555276
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section展開研究
Research Field 触媒・化学プロセス
Research InstitutionUniversitiy of Tsukuba (2001)
The University of Tokyo (1998-2000)

Principal Investigator

TOMISHIGE Keiichi  University of Tsukuba, Institute of Materials Science, Lecturer, 物質工学系, 講師 (50262051)

Project Period (FY) 1998 – 2001
Project Status Completed (Fiscal Year 2001)
Budget Amount *help
¥13,100,000 (Direct Cost: ¥13,100,000)
Fiscal Year 2001: ¥1,100,000 (Direct Cost: ¥1,100,000)
Fiscal Year 2000: ¥1,800,000 (Direct Cost: ¥1,800,000)
Fiscal Year 1999: ¥1,900,000 (Direct Cost: ¥1,900,000)
Fiscal Year 1998: ¥8,300,000 (Direct Cost: ¥8,300,000)
KeywordsNatural Gas / Methane / Carbon dioxide / Reforming / Synthesis Gas / Carbon deposition / Solid Solution Catalyst / リフォーミング / 活性劣化 / 反応器閉塞 / 触媒寿命 / リフォーミング反応 / ニッケル触媒 / メタン分解 / 不均化反応
Research Abstract

In methane reforming, one of the most serious problems is carbon deposition during the reaction. However the investigation of the route of carbon formation and the structure of formed carbon is not enough. Especially, in the development for the long-life catalyst, the information is very important. The research of the purpose is the elucidation of the relation between the catalyst life and carbon deposition behavior.
I investigated the methane reforming with CO_2, steam and CO_2+steam over various catalysts. The activity test, reaction temperature dependence, space velocity dependence, and total pressure dependence have been investigated. As a result, NiO-MgO solid solution catalysts showed excellent performance. Especially, the solid solution catalyst with low surface area exhibited much higher resistance to carbon deposition that that with high surface area. From the analysis ol the carbon deposition at various position of the catalyst bed, it is found that the carbon deposition at the inlet of the catalyst bed was inhibited. This indicates that the carbon formation from the methane decomposition is inhibited. Furthermore, the effect of other metal addition is also investigated. At present, the addition of Sn inhibited the carbon deposition.
The excellent catalyst is also applied to the fluidized reactor system for the methane reforming with internal heat supply using oxygen introduction with the reforming agents. Fluidization reaction system enhanced the methane conversion and it is found that the carbon deposition is not observed at all under highly pressurized condition. This is caused by the in-situ reproduction ol the active catalyst in the reactor.

Report

(5 results)
  • 2001 Annual Research Report   Final Research Report Summary
  • 2000 Annual Research Report
  • 1999 Annual Research Report
  • 1998 Annual Research Report
  • Research Products

    (21 results)

All Other

All Publications (21 results)

  • [Publications] K.Tomishige et al.: "Comparative study between fluidized bed and fixed bed reactors in methane reforming combined with methane combustion for the interval heat supply under pressured condition"Appl. Catal. A : General. 223. 225-238 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K.Tomishige et al.: "Effective methane reforming with CO_2 and O_2 under pressurized Conditions Using NiO-MgO and fluidized be reactor"Catal. Commun.. 2. 11-15 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K.Tomishige et al.: "Catalytic performance and carbon deposition behavior of NiO-MgO solid solution in methane reforming with carbon dioxide under pressurized condition"Ind. Eng. Chem. Res.. 39. 1891-1897 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K.Tomishige et al.: "Studies on Carbon deposition in Co_2 reforming of methane over Nickel-magnesia solid solution catalysts"J. Catal.. 181. 91-103 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K.Tomishige et al.: "Catalytic Performance and catalyst structure of nickel-magnesia catalysts for CO_2 reformnig of methane"J. Catal.. 184. 479-490 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Keiichi Tomishige, Yuichi Matsuo, Yusuke Yoshinaga, Yasushi Sekine, Mohammad Asadullah, Kaoru Fujimoto: "Comparative study between fluidized bed and fixed bed reactors in methane reforming combined with methane combustion for the internal heat supply under pressuri zed condition"Applied Catalysis A : General. 223. 225-238 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Keiichi Tomishige, Yuichi Matsuo, Yasushi Sekine, Kaoru Fujimoto: "Effective Methane Reforming with CO_2 and O_2 under Pressurized Conditions Using NiO-MgO and Fluidized Bed Reactor"Catalysis Communications. 2. 11-15 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Keiichi Tomishige, Yoshiyuki Himeno, Yuichi Matsuo, Kaoru Fujimoto: "Catalytic performance and carbon deposition behavior of NiO-MgO solid solution in methane reforming with carbon dioxide under pressurized condition"Ind. Eng. Chem. Res.. 39. 1891-1897 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Keiichi Tomishige, Yangguang Chen, Kaoru Fujimoto: "Studies on Carbon Deposition in CO_2 Reforming of CH_4 over Nickel-magnesia Solid Solution Catalysts"J. Catal.. 181. 91-103 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Yang-guang Chen, Keiichi Tomishige, Kota Yokoyama, Kaoru Fujimoto: "Catalytic performance and catalyst structure of nickel-magnesia catalysts for CO_2 reforming of methane"J. Catal.. 184. 479-490 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] 冨重圭一 他: "メタンの炭酸ガスリフォーミング反応による合成ガス製造における触媒特性と炭素析出挙動"石油学会誌. 44. 65-79 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Tomishige, et al.: "Effective Methane Reforming with CO_2 and O_2 under Pressurized Conditions Using NiO-MgO and Fluidized Bed Reactor"Catalysis Communications. 2. 11-15 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Tomishige, et al.: "Comparative Study between Fluidized bed and fixed bed Peactors in methane Reforming combined with methane combustion for the internal heat supply"Applied Catalysis A:General. 223. 225-238 (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] 冨重 et al: "メタンの炭酸ガスリフォーミング反応による合成ガス製造における触媒特性と炭素析出挙動解析-NiO-MgO固溶体触媒の開発-"石油学会誌. (印刷中).

    • Related Report
      2000 Annual Research Report
  • [Publications] K.Tomishige et al.: "Studies on Carbon Depositon in CO_2 reforming of methane over Nickel Magnesia Solid Solution Catalysts"J.Catalysis. 181. 91-103 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] 姫野嘉之,冨重圭一 et al.: "NiO-Mgo 固溶体触媒上の高圧条件化でのメタンの炭酸ガスリフォーミング反応における反応特性と炭素析出挙動"石油学会誌. 42. 252-257 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] Y.Chen,K.Tomishige et al.: "Catalytic Perfomance and catalyst structure of nickel-magnesia catalysts for CO_2 reforminjg of methane"J.Catalysis. 184. 479-490 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] K.Tomishige et al.: "Development of New Generation Reforming Catalyst-Catalytic Performance and Carbon Deposition Behavior on Nickel-magnesia Catalysts"Kinetics and Catalysis. 40. 388-394 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] K.Tomishige et.al.: "Development of Active and Stable Nickel-Magnesia Solid Solution Catalysts for CO_2 reforming of methane" Stud.Surf.Sci.Catal.114. 375-378 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] K.Tomishige et al: "Development of Ultra-Stable ni catalysts for CO_2 reforming of Methane" Catalysis Today. 45. 35-39 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] K.Tomishige: "Carbon-free CH_4-CO_2 and CH_4-H_2O Reforming Catalysts - Structure and Mechanism" Stud.Surf.Sci.Catal.119. 861-866 (1998)

    • Related Report
      1998 Annual Research Report

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Published: 1998-04-01   Modified: 2016-04-21  

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