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CVD調整による新規メソポーラス窒化物触媒の細孔内反応機構の解析と高活性化

Research Project

Project/Area Number 09555244
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 InstitutionTokyo University of Agriculture and Technology

Principal Investigator

永井 正敏  東京農工大学, 大学院・生物システム応用科学研究科, 助教授 (20111635)

Co-Investigator(Kenkyū-buntansha) 馬 光輝  東京農工大学, 大学院・生物システム応用科学研究科, 助手 (90262245)
萩原 洋一  東京農工大学, 総合情報処理センター, 講師 (40218392)
尾見 信三  東京農工大学, 大学院・生物システム応用科学研究科, 教授 (70016393)
高山 正夫  日揮ユニバーサル株式会社, 中央研究所, 室長
Project Period (FY) 1997 – 1998
Project Status Completed (Fiscal Year 1998)
Budget Amount *help
¥12,000,000 (Direct Cost: ¥12,000,000)
Fiscal Year 1998: ¥5,200,000 (Direct Cost: ¥5,200,000)
Fiscal Year 1997: ¥6,800,000 (Direct Cost: ¥6,800,000)
KeywordsCVD触媒 / タングステン窒化物 / モリブデン窒化物 / 水素化脱硫反応 / フラクタル / ニオブ窒化物 / メソ細孔 / フラクタル次元
Research Abstract

(1)熱CVD法によりタングステンおよびニオブを各種担体に担持した窒化物触媒を調整し、ジベンゾチオフェンの水素化硫反応に対する選択性と活性を検討した。具体的には、CVD法によりアルミナ上にポーラスな窒化ニオブ薄膜を合成した。反応時間1.5時間の触媒において、経時時間140分を境に活性が低下から増加へ変化した。反応後のXPS測定から、反応後の硫黄の堆積は認められないことから、この活性上昇の原因は触媒上での硫化物の形成によるものではないことが分かった。
(2)その他のコバルト,モリブデン窒化物触媒をCVD法および昇温窒化法により調整し、CO_2の水素化、CO_2によるCH_4の改質反応を行った。またカルバゾールの水素化脱窒素反応に対する活性を研究した。
(3)反応工学的・工業的検討としてモリブデン窒化物の水素化脱硫反応に対する触媒劣化機構と触媒劣化を劣化関数を導出してシミュレーションによる寿命予測を行った。
(4)触媒表面の構造と触媒の表面反応性を拡散FTIR,TEM,SEM,XPS等で検討し、反応に高選択・高活性な触媒の表面構造と反応性の相関関係を考察し、反応データを反応工学的見地から解析する。
(5)物質を変えた吸着実験から触媒表面のフラクタル構造について検討し現在学会誌への投稿を準備している。シリウスによるフラクタルシミュレーションは成果を論文として提出するまでには至らなかった。

Report

(3 results)
  • 1998 Annual Research Report   Final Research Report Summary
  • 1997 Annual Research Report
  • Research Products

    (26 results)

All Other

All Publications (26 results)

  • [Publications] M.Nagai、A.Irisawa、S.Omi: "XPS Study of the Deactivation and Sulfiding of Nitrided Molybdena-Alumina Catalyst during the Hydrodesulfurization of Dibenzothiophene"J.Phys.Chem.B. 102. 7619-7626 (1998)

    • Related Report
      1998 Final Research Report Summary
  • [Publications] M.Nagai、Y.Goto、K.Oshikawa、K.Hada、S.Omi: "Temperature-programmed Reduction and XRD Studies of Ammonia-Treated Molybdeum Oxide and Its Activity for Carbazole Hydrodenitrogenation"J.Catal.. 182. 292-301 (1999)

    • Related Report
      1998 Final Research Report Summary
  • [Publications] M.Nagai、T.Suda、K.Oshikawa、N.Hirano、S.Omi: "CVD Preparation of Alumina-Supported Tungsten Nitride and Its Activity for Thiophene Hydrodesulfurization"Catal.Today. 50. 29-37 (1999)

    • Related Report
      1998 Final Research Report Summary
  • [Publications] M.Nagai、J.Takada、S.Omi、: "XPS Study of Nitrided Molybdena/Titania Catalyst for the Hydrodesulfurization of Dibenzothiophene"J.Phys.Chem.B. 103. 10180-10188 (1999)

    • Related Report
      1998 Final Research Report Summary
  • [Publications] M.Nagai、M.Kiyoshi、A.Irisawa、S.Omi: "Hydrodesulfurization of Dibenzothiophene on Ammonia-treated Molybdenum Oxide Catalyt"Studies in Surface Science and Catalysis. 122. 373-378 (1999)

    • Related Report
      1998 Final Research Report Summary
  • [Publications] M.Magai、H.Koyama、S.Sakamoto、S.Omi: "The nitrided CoMo Catalysts for Hydrodesulfurization and Hydrodenitrogenation"Studies in Surface Science and Catalysis. 127. 195-202 (1999)

    • Related Report
      1998 Final Research Report Summary
  • [Publications] M.Nagai、Y.Goto、H.Ishii、S.Omi: "XPS and TPSR Study of Nitrided Molybdena-alumina Catalyst for the Hydrodesulfurization of Dibenzothiophene"Appl.Catal.Gen.. 192. 189-199 (2000)

    • Related Report
      1998 Final Research Report Summary
  • [Publications] M.Nagai、T.Nakauchi、Y.Ono、S.Omi: "CVD Preparation of Alumina-supported Niobium Nitride and Its Activity for Thiophene Hydrodesulfurization"Catal.Today. 57. 299-306 (2000)

    • Related Report
      1998 Final Research Report Summary
  • [Publications] K.Hada、S.Omi、M.Nagai: "XPS and TPR Studies of Nitrided Molybdena-alumina"J.Phys.Chem.B. 104. 2090-2098 (2000)

    • Related Report
      1998 Final Research Report Summary
  • [Publications] M.Nagai,K.Oshikawa,T.Kurakami,T.Miyao,S.Omi: "Surface Properties of Carbided Molybdena-Alumina and Its Activity for CO_2 Hydrogenation" J.Catal.180. 14-23 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] M.Nagai,A.Irisawa,S.Omi: "XPS Study of the Deactivation and Sulfiding of Nitrided Molybdena-Alumina Catalyst during the Hydrodesulfurization of Dibenzothiophene" J.Phys.Chem.B. 102. 7619-7626 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] M.Nagai,T.Kurakami,S.Omi: "Activity of carbided molybdena-alumina for CO_2 hydrogenation" Catal.Today. 45. 237-241 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] M.Nagai,Y.Goto,O.Uchino,S.Omi: "TPD study and carbazole hydrodenitrogenation activity of nitrided molybdena-alumina" Catal.Today. 45. 337-342 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] M.Nagai,Y.Goto,O.Uchino,S.Omi: "TPD and XRD Studies on Molybdenum Nitride and Its Activity for Hydrodenitrogenation of Carbazole" Catal.Today. 43. 249-259 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] M.Nagai,K.Koizumi,S.Omi: "Hydrodesulfurization of Thiophene on Ru/Al_2O_3 Catalyst-Effect of Ru particles size on Activity and Selectivity" J.Japan Petrol.Inst.42(1). 12-21 (1999)

    • Related Report
      1998 Annual Research Report
  • [Publications] S.Omi, T.Taguch, M.Nagai, G-H.Ma: "Synthesis of 100μm Uniform Porous by SPG Emulsification with Subsequent Swelling of the Droplets" J.Appl.Polym.Sci.63. 934-942 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] M.Nagai, K.Koizumi, S.Omi: "NH_3-TPD and XPS Studies of Ru/Al_2O_3 Catalyst and HDS Activity" Catalysis Today. 35. 393-405 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] M.miyao, K.Oshikawa, S.Omi, M.nagai: "Surface Property of Amunina-Supported Mo Carbide and its Acticity for HDN" Studies in Surface Science and Catalysis. 106. 255-262 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] M.Nagai, O.Uchino, T.Kusagaya, S.Omi: "Infrared Study on the Acid Sites of Nitrided Molybdena-alumina Catalysts" Studies in Surface Science and Catalysis. 106. 541-546 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] M.Nagai, K.Koizumi, S.Omi: "Surface Properties and Activity of Ru/Al_2O_3 Catalysts for Hydrodesulfurization of Thiophene" J.Petroleum Institute of Jpn. 39(4). 272-281 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] M.Nagai, Y.Goto, H.Sasuga, S.Omi: "Hydrodesulfurization of Dibenzothiophene on Nitrided Mo/Al_2O_3 Catalysts" J.European Ceramic Soc. 17. 1983-1987 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] M.Nagai, A.Miyata, T.Miyao, S.Omi: "Hydrodenitrogenation of Carbazole on Nitrided Molybdena-alumina Catalyst" J.Petroleum Inst.Jpn. 40(6). 500-509 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] T.Miyao, I.Shishikura, M.Matsuoka, M.Nagai, S.T.Oyama: "Preparation and Characterization of Alumina-supported Molybdenum Carbide" Applied Catalysis. (in press). (1998)

    • Related Report
      1997 Annual Research Report
  • [Publications] M.Nagai, Y.Goto, H.Sasuga, S.Omi: "Hydrodesulfurization of Dibenzothiophene on a Nitrided Supported Molybdena-Alumina Catalyst" Studies in Surface Science and Catalysis 111,Catalyst Deactivati on 1997,Elsevier Science-NL. 439-445 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] S.T.Oyama, 永井正敏: "遷移金属窒化物・炭化物を用いた新規材料の開発" ペトロテック. 20(9). 762-766 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] M.Nagai, T.Suda, S.Omi: "Preparation of Alumina-Supported Tungsten Nitride and its HDS Activity" Preprints,Division Petrolem..Chem,ACS. 42(3). 555-557 (1997)

    • Related Report
      1997 Annual Research Report

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Published: 1997-04-01   Modified: 2016-04-21  

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