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Development of radioactive ^<35>S and ^3H pulse tracer methods-Elucidation of behaviors of sulfur and hydrogen on sulfided catalysts

Research Project

Project/Area Number 08455371
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field 触媒・化学プロセス
Research InstitutionTokyo University of Agriculture and Technology

Principal Investigator

KABE Toshiaki  TUAT., Dept.of Appl.Chem., Professor, 工学部, 教授 (50092482)

Co-Investigator(Kenkyū-buntansha) GODO Masazumi  TUAT., Dept.of Appl.Chem., Research Assistant, 工学部, 助手 (80262244)
ISHIHARA Atsushi  TUAT., Dept.of Appl.Chem., Associate Professor, 工学部, 助教授 (60212908)
Project Period (FY) 1996 – 1997
Project Status Completed (Fiscal Year 1997)
Budget Amount *help
¥8,200,000 (Direct Cost: ¥8,200,000)
Fiscal Year 1997: ¥2,500,000 (Direct Cost: ¥2,500,000)
Fiscal Year 1996: ¥5,700,000 (Direct Cost: ¥5,700,000)
Keywordsradioactive tracer method / Hydrodesulfurization / Sulfur behavior / Labile sulfur / Structure of sulfided catalysts / Hydrogen behavior / Hydrodesulfurization mechanism / Deep hydrodesulfurization of light gas oil / 触媒 / 水素化 / 脱硫 / 石炭液化 / ラジオアイソトープトレーサー法 / トリチウム / ^<35>S / 反応機構
Research Abstract

This research was supported by grants from the Ministry of Education, Science, Sports and Culture as Grant-in-Aid for Scientific Research (B) (2) with the project number 08455371 in the two years (1996-1997). This report summarized the study results on the structure of sulfided catalysts and the mechanism of deep hydrodesulfurization of a light gas oil using ^<35>S and ^3H radioisotope pulse tracer methods. Many basic point on the structure of HDS catalyst and the mechanism have still remained to be clarified although a number of studies on elucidation of HDS mechanisms using conventional characterization technique and the kinetic analysis method were reported. Especially, there have been few examples clarifying the behavior of sulfur on the working-catalyst. In order to develop the new catalysts continuously, it is essential to know in more detail the hydrodesulfurization mechanism. On the other hand, the tracer method has been considered to enable us quantify the behavior of sulfur o … More n the working catalyst and hydrogen behavior in the practical hydrodesulfurization reaction. Therefore, in this study, a ^<35>S and ^3H radioisotope pulse tracer method was developed and was applied to several aspects as follows : 1) Presulfidation mechanism of No-based desulfurization catalysts ; 2) Hydrodesulfurization kinetics of dibenzothiophenes on Mo-based catalysts ; 3) Retarding effect of H_2S and solvent on hydrodesulfurization reaction ; 4) Elucidation of sulfur mobility on Mo-based catalysts in hydrodesulfurization by ^<35>S pulse tracer method : 5) Deep desulfurization mechanism of light gas oil ; 6) Novel desulfurization catalysts using supported metal carbonyl complexes as catalytic precursors. From these studies, a lot of new information on the structure of sulfided catalysts, the insight of active sites and the mechanism of hydrodesulfurization was obtained. This makes us gain a good deal of enlightenment for development of new catalysts appropriated to the dep hydrodesulfurization of light gas oil. Less

Report

(3 results)
  • 1997 Annual Research Report   Final Research Report Summary
  • 1996 Annual Research Report
  • Research Products

    (51 results)

All Other

All Publications (51 results)

  • [Publications] Q.Zhang: "Deep Desulfurizaltion of Light Oil.4.Hydyo desulfurigation of Methyl-sufstituted Dibenzo thiopheues Catalyiecl by Various CoMc/OZOD_5 and NaMo/AbO_2,cotaly" Sekiyu Gakkaishi. 39. 410-417 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] T.Kabe: "Sulfur exchange on CoMo/AhO_3 hydrochesalfariycztion catalyst using^<35>S raolioisotope tracer." Catal.Today. 29. 197-202 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] A.Ishihara: "(Part 4)Hgdnodesulgarizaltion Catalysts prepared from alumina and silica-alumina supporaitod molybdenum and cobaltcarbomyls." Sekiyu Gakkaishi. 39. 26-33 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] A.Ishihara: "Part 5. Cataly_8t_3 for nydrodesulfurization prepared from alumina-supgorted ruthenium carboml-alkali metal rydroxade system" Sekiyu Gakkaishi. 39. 211-221 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] A, Ishihara: "Part 6.Effect of supports on cectivilies of HDS catalyzts prepazecl from supported rutheriam carborgl-cesium hydroxido systems" Sekiyu Gakkaishi. 39. 403-409 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] T.Kabe: "Sulgidation of molybdena-based alumina catolyzts using a radioisotope tracer method" J.chem.Soc.Faraday Trans.93. 3709-3713 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] A.Ishihara: "Elucidetion of Sulfur Behavior on Alumina-sapported Ruthenium Sultide-Casium Catalysts Using Radioactive ^<35>S as a Tracer" Chem.Lett.743-744 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Q.Zhang: "The Role of Cobalt of Hydrodesulfurization and Hydrogenation of Dibenzo-thiophene and 4,6-Dimethyldibenzothiophene Catalyzed by Co-Mo/Al_2O_3" J.Jpn.Petrol.Inst.(Sekiyu Gakkaishi). 40. 408-414 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Q.Zhang: "Effect of H_2S on Hydrodesulfurization of Dibenzothiophene and 4,6-Dimethyl dibenzothiophene" J.Jpn.Petrol.Inst.(Sekiyu Gakkaishi). 40. 185-191 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] T.Kabe: "Elucidation of Hydrodesulfurization Meehanism Using ^<35>S Redioisotope Pulse Traeer Methods" Catalysis Today. 1107. 1-10 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] W.Qian: "Elucidation of Molybdenum-based Catalysts Using a Redioisotope Tracer Method (Part 1)Hydrodesulfarization Activity and Structure of Sulfided Molybdena-Alumina Catalysts" J.Chem.Soc.Faraday Trans. 93. 1821-1826 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] W.Qian: "(Part 2)Promotion Effect of cobalt for Molybdena-Alumina Catalysts" J.Chem.Soc.Faraday Trans.93. 4395-4400 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] W.Qian: "Elucidafion of Behavior of Sulfur on Sulfided.Co-Mo/Al_2O_3 Catalyst Using a ^<35>S Radioisotope Pulse Tracer Method" J.Catal. 170. 286-294 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Q.Zhang: "(Rart 5)Hydrodesulfurization of Methyl-substituted Benzothicphenes and Pibenzothiophenes in Light gas oil Catalyzed by Various Sultided Co-Mo/Al_2O_3 and Ni-Mo/Al_2O_3 Catalysts" J.Jpn.Petrol.Inst.(Sekiyu Gakkaishi). 40. 29-34 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] A.Ishihara: "(Part 7)Hydrodesulfurization Catalysts Prepared from Alumina-sapported Ruthenium Carbonyl-Alkaline-earth Metal Hydroxide System" J.Jpn.Petrol.Inst.(Sekiyu Gakkaishi). 40. 516-523 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Q.Zhang, A.Ishihara, and T.Kabe: "Deep Desulfurization of Light Oil. 4. Hydrodesulfurization of Methyl-substituted Dibenzothiophenes Catalyzed by Various Co-Mo/Al_2O_3 and Ni-Mo/Al_2O_3 Catalysts." J.Jpn.Petrol, Inst.(Sekiyu Gakkaishi). 39(6). 410-417 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] T.Kabe, W.Qian, W.Wang, and A.Ishihara: "Sulfur Exchange on Co-Mo/Al_2O_3 Hydrodesulfurization Catalyst Using ^<35>S Radiosotope Tracer" Catal.Today.29. 197-202 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] A.Ishihara, M.Matsushita, K.Shirouchi, Q.Zhang, and T.Kabe: "Hydrodesulfurization of Dibenzothiophene Catalyzed by Supported Metal Carbonyls Complexes (Part 4)Hydrodesulfurization Catalysts Prepared from Alumina and Silica-Alumina Supported Molybdenum and Cobalt Carbonyls." J.Jpn.Petrol, Inst.(Sekiyu Gakkaishi). 39(1). 26-33 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] A.Ishihara, M.Nomura, N.Takahama, K.Hamaguchi, and T.Kabe: "Hydrodesulfurization of Dibenzothiophene Catalyzed by Supported Metal Carbonyl Complexes (Part 5). Catalysts for Hydrodesulfurization Prepared from Alumina-supported Ruthenium Carbonyl-Alkali Metal Hydroxide Systems." J.Jpn.Petrol, Inst.(Sekiyu Gakkaishi). 39(3). 211-221 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] A.Ishihara, M.Nomura, K.Shirouchi, and T.Kabe: "Hydrodesulfurization of Dibenzothiophene Catalyzed by Supported Metal Carbonyls Complexes (Part 6). Effect of Supports on Activities of HDS Catalysts Prepared from Supported Ruthenium Carbonyl-Cesium Hydrode Systems." J.Jpn.Petrol, Inst.(Sekiyu Gakkaishi). 39(6). 403-409 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] A.Ishihara, M.Yamaguchi, H.Godo, W.Qian, M.Godo, and T.Kabe: "Elucidation of Sulfur Behavior on Alumina-Supported Ruthenium Sulfide-Cesium Catalysts Using Radioactive ^<35>S as a Tracer." Chem.Lett.743-744 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] T.Kabe, W.Qian, K.Tanihata, A.Ishihara, and M.Godo: "Sulfidation of Molybdena-Based Alumina Catalysts Using a Radioisotope Tracer method." J.Chem.Soc.Faraday Trans.93(20). 3709-3713 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Q.Zhang, W.Qian, S.Oshima, A.Ishihara, and T.Kabe: "The Role of Cobalt on Hydrodesulfurization and Hydrogenation of Dibenzo-thiophene and 4,6-Dimenthyl-dibenzothiophene Catalyzed Co-Mo/Al_2O_3" J.Jpn.Petrol, Inst.(Sekiyu Gakkaishi). 40(5). 408-414 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Q.Zhang, W.Qian, A.Ishihara, and T.Kabe: "Effect of H_2S on Hydrodesulfurizationof Dibenzothiophene and 4,6-Dimethyldibensothiophene" J.Jpn.Petrol, Inst.(Sekiyu Gakkaishi). 40(3). 185-191 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] T.Kabe, W.Qian, and A.Ishihara: "Elucidation of Hydrodesulfurization Mechanism Using ^<35>S Radioisotope Pulse Tracer Methods" Catalysis Today. 1107. 1-10 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] W.Qian, Q.Zhang, Y.Okushi, A.Ishihara, and T.Kabe: "Eluciadation of Molybdenum-based Catalysts Using a Radioisotope Tracer Method. Part 1.Hydrodesulfurization Activity and Structure of Sulfided Molybdena-Alumina Catalysts." J.Chem.Soc.Faraday Trans.93(9). 1821-1826 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] W,Qian, A.Ishihara, Y.Okoshi, W.Nakakami, M.Godo, and T.Kabe: "Elucidation of Molybdenum-based Catalysts Using a Radioisotope Tracer Method. Part 2. Promotion Effect of Cobalt for Molybdena-Alumina Catalysts." J.Chem.Soc.Faraday Trans.93(24). 4395-4400 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] W,Qian, A.Ishihara, G.Wang, T.Tsuzuki, M.Godo, and T.Kabe: "Elucidation of Behavior of Sulfur on Sulfided Co-Mo/Al_2O_3 Catalysts Using a ^<35>S Radioisotope Pulse Tracer Method" J.Catal.170. 286-294 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Q.Zhang, A.Ishihara, H.Yashima, W.Qian, H.Tsutsui, and T.Kabe: "Deep Desulfurization of Light Oil (Part 5) Hydrodesulfurization of Methyl-Substituted Benzothiophenes and Dibenzothiophenes in Light Gs Oil Catalyzed by Various Sulfided Co-Mo/Al_2O_3 and Ni-Mo/Al_2O_3 Catalysts." J.Jpn.Petrol, Inst.(Sekiyu Gakkaishi). 40(1). 29-34 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] A.Ishihara, K.Hamaguchi, and T.Kabe: "Hydrodesulfurization of Dibenzothiophene Catalyzed by Supported Metal Carbonyl Complexes (Part 7). Hydrodesulfurization Catalysts Prepared from Alumina-supported Ruthenium Carbony-Alkaline-earth Metal Hydroxide Systems." J.Jpn.Petrol, Inst.(Sekiyu Gakkaishi). 40(6). 516-523 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Q.zhang: "Deep Desulfurization of Light oil.4.Hydrodesulf urization of Methy-substituted Diben zothiophenes Catalyzed by various Co-Mo/Al_2O_3 and Mi-Mo/Al_2O_3 Catnlyses" Sekiyu Gakkaishi. 39. 410-417 (1996)

    • Related Report
      1997 Annual Research Report
  • [Publications] T.Kabe: "Sulfur exchange on CoMo/Al_2O_3 hydrodesulfurization Catalyst using ^<35>S radioisotope tracer" Catal. Today. 29. 197-202 (1996)

    • Related Report
      1997 Annual Research Report
  • [Publications] A.Ishihara: "(Part4) Hydrodesulfurization Catalysts prepared from alumina and Silica-alumina supported molybdcnum and cobalt carbonyls" Sekiyu Gakkaishi. 39. 26-33 (1996)

    • Related Report
      1997 Annual Research Report
  • [Publications] A.Ishihara: "Part5 Catalysts for hydrodesulfurization prepared from alumina-supported nothenium Carbonyl-alkali metal hydroxide system" Sekiyu Gakkaishi. 39. 211-221 (1996)

    • Related Report
      1997 Annual Research Report
  • [Publications] A.Ishihara: "Part6 effect of supports on activities of HDS Catalysts prepared from supported ruthenium carbonyl-Cesium hydroxide systems" Sekiyu Gakkaishi. 39. 403-409 (1996)

    • Related Report
      1997 Annual Research Report
  • [Publications] T.Kabe: "Sulfidation of molybdenium-based alumina Catalysts using a radioisotope tracer method" J.Chem. Soc.Faraday trans. 93. 3709-3713 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] A.Ishihara: "Elucidation of Sulfur Bcluir on Alumina-supported Ruthenium sulfide-cosium Catalyets using Radioactive ^<35>S as a Traces" Chem.Lett. 743-744 (1996)

    • Related Report
      1997 Annual Research Report
  • [Publications] Q.zhang: "The role of Cabalt of Hydrodesulfurization and Hydrogenation of Diben20t nline and 4,6-Dimethyldiben20thiophene Cataly2ed by Co-Mo/Al_2O" J.Jpn. Petrol.Inst.(Sekiyu Gakkaishi). 40. 408-414 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] Q.zhang: "Effect of ths on Hydrodesulfurization of Diben 20 thiophene and 4.6-Dimethyl diben20thiophene" J.Jpn.Petiol.Insi (Sekiyu Gakkaishi). 40. 185-191 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] T.Kabe: "Elucideition of Hydrodesulfurization Mechanism Using ^<35>S Radioisotope Pulse Tracer Methods" Catalysis Today. 1107. 1-10 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] W.Qian: "Elucidation of Molybdenum-based Catalysts Using a Radioisotope Tracer Method (Part1) Hydrodesulfurization Activitly and siucture of Sulfided Molybdena-Alumina Cal" J.Chem.Soc.Faraday Trans. 93. 1821-1826 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] W.Qian: "(Part2) Promotion Effect of Cobalt for Molybdena-Alumina catalysts" J.Chem.Soc.Faraday Trans. 93. 4395-4400 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] W.Qian: "Elucidation of Bchanior of sulfur on sulfided CO-MO/Al_2O_3 Catalysts using a ^<35>S Radioisotope pulse Tracer Method" J.Catal. 170. 286-294 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] Q.Zhang: "(Part5) Hydrodesulfarization of Methy-subsrituted Banzothiopenes and Dibenzo-phene in Light gas oil Catalyzed by various sulfided CO-MO/Al_2O_3 and Nl-MO/Al_2O_3 Catalysts" J.Jpn.Petrol.Ict (Sekiyu Gakkaishi). 40. 29-34 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] A.Ishihara: "(Part7) Hydrodesulturization Catalysts prepared from Alumina-supported Ruthenium Carbonyh-Alkaline-earth Metal Hydroxide system" J.Jpn.Petrol.Inst (Sekiyu Gakkaishi). 40. 516-523 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] Toshiaki Kabe: "Sulfur exchange on Co-Mo/Al_2O_3 hydrodesulfurization catalyst using ^<35>S radloisotope tracer" CATALYSIS TODAY. 29. 197-202 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] Atsushi Ishihara: "Hydrodesulfurization of Dibenzothiophene Catalyzed by Supported Metal Carbonyl Complexes (Part 5)" J.Jpn.Petrol.Inst.39(3). 211-221 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] Atsushi Ishihara: "Elucidation of Behavior of Sulfur on Catalysts Derived from Aumina-Supported Ruthenium Carbonyls-Cesium Hydroxide Systems Using ^<35>S as a Tracer" Chem.Lett.743-744 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] Atsushi Ishihara: "Hydrodesulfurization of Dibenzothiophene Catalyzed by Supported Metal Carbonyl Complexes (Part 6)" J.Jpn.Petrol.Inst.39(6). 403-409 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] Qing Zhang: "Deep Desulfurization of Light Oil (Part 4)" J.Jpn.Petrol.Inst.39(6). 410-417 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] Qing Zhang: "Deep Desulfurization of Light Oil (Part 5)" J.Jpn.Petrol.Inst.40(1). 29-34 (1997)

    • Related Report
      1996 Annual Research Report

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Published: 1996-04-01   Modified: 2016-04-21  

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