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Development of Technique for Chemical Conversion of Natural Gas

Research Project

Project/Area Number 01470079
Research Category

Grant-in-Aid for General Scientific Research (B)

Allocation TypeSingle-year Grants
Research Field 工業物理化学
Research InstitutionTokyo Institute of Technology

Principal Investigator

MORIKAWA Akira  Tokyo Institute of Technology Professor, 工学部, 教授 (00016396)

Co-Investigator(Kenkyū-buntansha) KOMATSU Takayuki  Research Associate, 工学部, 助手 (40186797)
HATANO Masaharu  Research Associate, 工学部, 助手 (50202255)
WADA Yuji  Research Associate, 工学部, 助手 (40182985)
OTSUKA Kiyoshi  Associate Professor, 工学部, 助教授 (60016532)
Project Period (FY) 1989 – 1990
Project Status Completed (Fiscal Year 1990)
Budget Amount *help
¥7,400,000 (Direct Cost: ¥7,400,000)
Fiscal Year 1990: ¥1,500,000 (Direct Cost: ¥1,500,000)
Fiscal Year 1989: ¥5,900,000 (Direct Cost: ¥5,900,000)
KeywordsNatural gas / Alkane / Oxidative coupling / Oxygenated / Methane / Fuel cell / Peroxide / Solid catalyst / 燃料電池 / 過酸化ナトリウム / 部分酸化 / 部分酸化物 / アルデヒド
Research Abstract

It has been found that LiNO_3-doped NiO was a catalyst effective for oxidative coupling of methane to produce ethane and ethylene. This catalyst was identified as a compound, LiNiO_2. When methane was brought into contact with LiNiO_2, methane was converted to ethylene and ethane and LiNiO_2 was changed into a mixture of Li_2O and NiO. LiNiO_2 was restored when oxygen gas was added to the system. From the Kinetic and spectroscopic studies of this catalytic system, it has been concluded that oxidative coupling of methane on LiNiO_2 proceeds through the reaction of methane with the catalyst and reoxidation of the reduced catalyst.
LiClーdoped NiO was a catalyst effective for selective formation of ethylene during oxidative coupling of methane. LiCl suppressed deep oxidation of methane and enhanced the successive oxidative dehydrogenation of ethane to ethylene.
Two effective catalysts for formation of oxygenated compounds in oxidation of alkanes with molecular oxygen have been found. One was B_2O_3-Al_2O_3, which gave acetaldehyde from ethane. The main products on this catalyst were acetaldehyde and ethylene. A mechanism including the common intermediate for the formations of the two products were proposed. Another was B_2O_3-P_2O_5, on which propane was converted to propionaldehyde, acetone, acetaldehyde, and propylene.
Oxidative coupling of methane into ethylene and ethane over LiNiO_2 was enhanced when oxygen was removed electrochemically from the catalyst through a stabilized zirconia oxygen-anion conductor. On the other hand, the same enhancement was observed over LiCl-doped NiO when oxygen was pumped to the catalyst. The mechanisms of the new catalytic systems controlled electrochemically were proposed.

Report

(3 results)
  • 1990 Annual Research Report   Final Research Report Summary
  • 1989 Annual Research Report
  • Research Products

    (35 results)

All Other

All Publications (35 results)

  • [Publications] K.Otsuka: "Electrochemical enhancement of oxidative coupling of methane over LiClーdoped NioO using stabilized zirconia electrolyte" Catalysis Letters. 1. 423-428 (1988)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] M.Hatano: "Alkali metalーdoped transition metal oxides active for oxidative conpling of methane" Inorganica Chimica Acta. 146. 243-247 (1988)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] T.Komatsu: "LiCl doped cobalt oxide is an active catalyst for the formation of ethylene in the oxidative coupling of methane" Catalysis Letters. 3. 317-322 (1989)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] M.Hatano: "The oxidative coupling of methane on lithium nickelate(III)" J.Chem.Soc.,Faraday Trans.1. 85. 199-206 (1989)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] K.Otsuka: "Synthesis of C_2H_4 by partial oxidation of CH_4 over LiCl/NiO" Catalysis Today. 4. 409-419 (1989)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] K.Otsuka: "Oxidative of methane applying a solid oxide fuel cell system" Catalysis Today. 6. 587-592 (1990)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] K. Otsuka, K. Suga, I. Yamanaka: "Electrochemical Control for Oxidative Coupling of Methane over LiNiO_2 Using Solid Electrolytes" Chem. Lett.,. 317-318, (1988)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] K. Otsuka, K. Suga, I. Yamanaka: "Electrochemical Enhancement of Oxidative Coupling of Methane over LiClーDoped NiO Using Stabilized Zirconia Electrolyte" Catal. Lett.,. 1. 423-428

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] M. Hatano, K. otsuka: "Alkali Metal-Doped Transition Metal Oxides Active for Oxidative Coupling of Methane" Inorg. Chim. Acta,. 146,. 243-247 (1988)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] K. Otsuka, M. Hatano, T. Komatsu: "Synthesis of C_2H_4 by Partial Oxidation of CH_4 over Transition Metal Oxides with Alkali-Chlorides." Methane Coversion, Elsevier,. 383-387, (1988)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] K. Otsuka: "Activation and Partial Oxidation of Methane" Shokubai (Catalyst),. 30,. 248-254, (1988)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] K. Otsuka, T. Komatsu, K. Jinno, Y. Uragami, A. Morikawa: "Activation of Methane and Synthesis of Formaldehyde by Partial Oxidation" Proc. 9th Intern. Cong. Catal.,. 2,. 915-922, (1988)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] K. Otsuka, T. Komatsu, Y. Shimizu: "The Cerium Oxide Based Catalysts Active for Oxidative Coupling of Methane" Successful Design of Catalysts, Elsevier,. 43-50, (1988)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] T. Komatsu, Y. Uragami, K. Otsuka: "Partial Oxidation of Propane over B-P Mixed Oxide Catalysts" Chem. Lett.,. 1903-1906, (1988)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] T. Komatsu, T. Amaya, K. Otsuka: "LiCl Doped Cobalt Oxide is an Active Catalyst for the Formation of Ethylene in the Oxidative Coupling of Methane" Catal. Lett.,. 3,. 317-322, (1989)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] M. Hatano, K. Otsuka: "The Oxidative Coupling of Methane on Lithium Nickelate (III)" J. Chem. Soc., Faraday Trans.1, 8,. 199-206, (1989)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] K. Otsuka, Y. Murakami, Y. Wada, A. A. Said, A. Morikawa: "Oxidative Coupling of Methane, Ethane, and Propane with Sodium Peroxide at Low Temperatures" J. Catal.,. 121,. 122-130, (1990)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] Y. Murakami, K. Otsuka, Y. Wada, A. Morikawa: "Partial Oxidation of Ethane over Boron Oxide Added Catalysts" Chem. Lett.535-538, (1989)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] K. Otsuka, M. Hatano, T. Komatsu: "Synthesis of C_2 H_4 by Partial Oxidation of CH_4 over LiCl/NiO" Catal. Today,. 4,. 409-419, (1989)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] K. Otsuka, K. Hosokawa, I. Yamanaka, Y. Wada, A. Morikawa,: "Oneーstep Oxidation of Benzene to Phenol Applying a Fuel Cell System" Electrochimica Acta,. 34,. 1485-1488, (1989)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] K. Otsuka, M. Inaida, Y. Wada, T. Komatsu, A. Morikawa: "Isotopic Studies on Oxidative Methane Coupling over Samarium Oxide" Chem. Lett.,. 1531-1534, (1989)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] Y. Murakami, K. Otsuka, T. Wada, A. Morikawa: "The Partial Oxidation of Ethane over a B_2O_3-Al_2O_3 Catalyst" Bull. Chem. Soc. Jpn.,. 63,. 340-346, (1990)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] K. Otsuka, K. Suga, I. Yamanaka: Catal. Today,. 6,. 587-592, (1990)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1990 Final Research Report Summary
  • [Publications] K.Otsuka: "Electrochemical enhancement of oxidative coupling of methane over LiClーdoped NiO using stabilized zirconia electrolyte" Catalysis Letters. 1. 423-428 (1988)

    • Related Report
      1990 Annual Research Report
  • [Publications] M.Hatano: "Alkali metalーdoped transition metal oxides active for oxidative coupling of methane" Inorganica Chimica Acta. 146. 243-247 (1988)

    • Related Report
      1990 Annual Research Report
  • [Publications] T.Komatsu: "LiCl doped cobalt oxide is an active catalyst for the formation of ethylene in the oxidative coupling of methane" Catalysis Letters. 3. 317-322 (1989)

    • Related Report
      1990 Annual Research Report
  • [Publications] M.Hatano: "The oxidative coupling of methane on lithium nickelate(III)" J.Chem.Soc.,Faraday Trans.1. 85. 199-206 (1989)

    • Related Report
      1990 Annual Research Report
  • [Publications] K.Otsuka: "Synthesis of C_2H_4 by partial oxidation of CH_4 over LiCl/NiO" Catalysis Today. 4. 409-419 (1989)

    • Related Report
      1990 Annual Research Report
  • [Publications] K.Otsuka: "Oxidative coupling of methane applying a solid oxide fuel cell system" Catalysis Today. 6. 587-592 (1990)

    • Related Report
      1990 Annual Research Report
  • [Publications] T.Komatsu: "Partial oxidation of propane over B-P mixed oxide catalysts" Chemistry Letters. 1988. 1903-1906 (1988)

    • Related Report
      1989 Annual Research Report
  • [Publications] Y.Murakami: "Partial oxidation of ethane over boron oxide added catalysts" Chemistry Letters. 1989. 535-538 (1989)

    • Related Report
      1989 Annual Research Report
  • [Publications] K.Otsuka: "Isotopic studies on oxidative methane coupling over samarium oxide" Chemistry Letters. 1989. 1531-1534 (1989)

    • Related Report
      1989 Annual Research Report
  • [Publications] K.Otsuka: "Partial oxidation of methane over solid catalysts:Reaction mechanismand active oxygen species" Preprints of 3B symposium on methane activation,conversion and utilization(PACIFICHEM'89). 88-10 (1989)

    • Related Report
      1989 Annual Research Report
  • [Publications] K.Otsuka: "Oxidative coupling of methane,ethane,and propane with sodium peroxide at low termperatures" Journal of Catalysis. 121. 122-130 (1990)

    • Related Report
      1989 Annual Research Report
  • [Publications] Y.Murakami: "The partial oxidation of ethane over a B_2O_3-Al_2O_3 catalyst" Bulletin of the Chemical Society of Japan. 63. 340-346 (1990)

    • Related Report
      1989 Annual Research Report

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Published: 1989-04-01   Modified: 2016-04-21  

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