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酸化チタン/ゼオライト光触媒系による二酸化炭素の水による還元固定化反応

Research Project

Project/Area Number 15033263
Research Category

Grant-in-Aid for Scientific Research on Priority Areas

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

Principal Investigator

安保 正一  大阪府立大学, 工学研究科, 教授 (70094498)

Co-Investigator(Kenkyū-buntansha) 松岡 雅也  大阪府立大学, 工学研究科, 講師 (80305648)
竹内 雅人  大阪府立大学, 工学研究科, 助手 (90382233)
ザンペイソフ ノルボシン  大阪府立大学, 工学研究科, 助手 (10326275)
山下 弘巳  大阪大学, 大学院・工学研究科, 教授 (40200688)
Project Period (FY) 2003 – 2004
Project Status Completed (Fiscal Year 2004)
Budget Amount *help
¥5,000,000 (Direct Cost: ¥5,000,000)
Fiscal Year 2004: ¥2,500,000 (Direct Cost: ¥2,500,000)
Fiscal Year 2003: ¥2,500,000 (Direct Cost: ¥2,500,000)
Keywords光触媒 / 二酸化炭素還元固定化 / 可視光利用 / ゼオライト / イオン注入 / メタノール生成 / 表面疎水化 / 高分散酸化チタン / メソポーラスゼオライト
Research Abstract

本研究では、ゼオライト骨格中にTiを含有した触媒を合成し、この系にイオン注入法を適用することで、酸化チタン光触媒の電子状態の制御を行い、可視光を吸収し二酸化炭素を水により還元固定化できる光触媒プロセスの実現を検討した。また、触媒の薄膜化や疎水化処理により触媒活性と選択性の向上を試みた。Ti含有ゼオライト光触媒上でのメタノール生成の選択性の向上を図るため、F^-イオンを含有するテンプレートを用い、疎水性Betaゼオライト(Ti-Beta(F))を合成した。FT-IR測定により、OH^-イオンを含有するテンプレートを用いて合成したBetaゼオライト(Ti-Beta(OH))と比較してTi-Beta(F)では表面OH基の減少が確認された。実際、室温でのH_2O吸着等温線測定によりTi-Beta(F)ではH_2Oの吸着量は減少し、表面の疎水化が確認できた。これらを光触媒として二酸化炭素の水による還元反応を検討した結果、Ti-Beta(F)は触媒活性は低いものの、Ti-Beta(OH)と比較して高い選択性でメタノールを生成できることを見出した。
さらに、光透過性が高く大表面積を有するTi含有メソポーラスシリカ薄膜を合成した。溶媒抽出法により合成したTi含有メソポーラスシリカ薄膜を二酸化炭素と水の存在下で紫外光照射すると、メタンおよびメタノールが生成した。透明なTi含有メソポーラスシリカ薄膜を粉末状にすると光触媒活性が低下することから、透明な薄膜光触媒の高い光触媒反応性が触媒の薄膜化による光吸収効率の向上に密接に関連することがわかった。
また、Ti含有メソポーラスシリカ光触媒上にVイオンを注入するとUV-Vis吸収スペクトルは注入イオン量に依存して長波長側にシフトし、可視光を吸収することがわかった。このように可視光吸収が可能な光触媒を用いると、390nmより長波長の光照射下で二酸化炭素の水による還元固定化反応が進行し、メタンおよびメタノールが生成することを見いだした。

Report

(2 results)
  • 2004 Annual Research Report
  • 2003 Annual Research Report
  • Research Products

    (28 results)

All 2004 Other

All Journal Article (6 results) Book (1 results) Publications (21 results)

  • [Journal Article] Preparation, characterization, and reactivities of highly functional titanium oxide-based photocatalysts able to operate under UV-visible light2004

    • Author(s)
      M.Anpo
    • Journal Title

      Bull.Chem.Soc.Jpn. 77

      Pages: 1427-1442

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Preparation of TiO_2 Photocatalysts by Multi-gelation Method and Their Photocatalytic Reactivity for the Degradation of 2-propanol2004

    • Author(s)
      B.Neppolian, H.Yamashita, Y.Okada, H.Nishijima, M.Anpo
    • Journal Title

      Chem.Lett. 33

      Pages: 268-269

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Hydrogen Bonding versus Coordination of Adsorbate Molecules on Ti-silicalites2004

    • Author(s)
      N.U.Zhanpeisov, M.Anpo
    • Journal Title

      J.Am.Chem.Soc. 120

      Pages: 9439-9444

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Intrinsic Band Gap Shift in Ti silicalites Modified by V Ion Implantation : Ab initio and Density Functional Theory Study2004

    • Author(s)
      N.U.Zhanpeisov, Y.Kanazawa, H.Yamashita, M.Anpo
    • Journal Title

      Inter.J.Quant.Chem. 96

      Pages: 9439-9444

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Visible-Light-Sensitive Photocatalysts2004

    • Author(s)
      H.Yamashita, M.Takeuchi, M.Anpo
    • Journal Title

      Encyclop.Nanosci.Nanotech. 10

      Pages: 639-654

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Application of an Ion Beam Technique for the Design of Visible Light-Sensitive, Highly Efficient and Highly Selective Photocatalysts2004

    • Author(s)
      H.Yamashita, M.Anpo
    • Journal Title

      Catal.Surv.Asia 8

      Pages: 35-45

    • Related Report
      2004 Annual Research Report
  • [Book] 高機能な酸化チタン光触媒 -環境浄化・材料開発から規格化・標準化まで-2004

    • Author(s)
      安保正一監修
    • Total Pages
      499
    • Publisher
      NTS
    • Related Report
      2004 Annual Research Report
  • [Publications] Y.Hu, G.Martra, S.Higashimoto, JL.Zhang, M.Matsuoka, S.Coluccia, M.Anpo: "The Relationship between the Local Structures and Photocatalytic Reactivity of Ti-MCM-41 Catalysts"Stud.Surf.Sci.Catal.. 146. 593-596 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] Y.Shioya, K.Ikeue, M.Ogawa, M.Anpo: "Synthesis of Transparent Ti-containing Mesoporous Silica Thin Film Materials and Their Unique Photocatalytic Activity for the Reduction of CO_2 with H_2O"Appl.Catal.A : General. 254. 251-259 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] K.Iino, M.Anpo: "Atomic Level Characterization by Synchrotron Radiation for the Design of High Performance Catalysts"Res.Chem.Intermed.. 29. 773-782 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] M.Anpo, M.Takeuchi: "The Design and Development of Highly Reactive Titanium Oxide Photocatalysts Operating under Visible Light Irradiation"J.Catal.. 216. 505-516 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] M.Anpo, H.Yamashita, N.U.Zhanpeisov, M.Matsuoka, Y.Kanazawa, M.Okazaki: "Design and Development of Environmentally-Harmonious Ti/Zeolite Photocatalysts"Proc.4th Intern.Symp.on Eco-Mater.Process & Design. 63-66 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] M.Matsuoka, M.Anpo: "Local structures, Excited states, and Photocatalytic Reactivities of Highly Dispersed Catalysts Constructed within Zeolites"J.Photochem.Photobiol.C : Photochem.Rev.. 3. 225-252 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] S.Dohshi, M.Takeuchi, M.Anpo: "Effect of the Local Structure of Ti-oxide Species on the Photocatalytic Reactivity and Photoinduced Super-hydrophilic Properties of Ti/Si and Ti/B Binary Oxide Thin Films"Catal.Today. 85. 199-206 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] H.Yamashita, K.Maekawa, Y.Nakatani, J.-J.Park, M.Anpo: "Photocatalytic Degradation of 2-Propanol Diluted in Water with TiO_2 Photocatalyst Loaded on Si_3N_4"Chem.Lett.. 10. 930-931 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] J.Zhang, H.Xu, H.Chen, M.Anpo: "Study on the Formation of H_2O_2 on TiO_2 Photocatalysts and Their Activity for the Photocatalytic Degradation of X-GL dye"Res.Chem.Intermed.. 29. 839-848 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] M.Takeuchi, S.Dohshi, T.Eura, M.Anpo: "Preparation of Titanium-Silicon Binary Oxide Thin Film Photocatalysts by an Ionized Clust Beam Deposition Method. Their Photocatalytic Activity and Photoinduced Super-Hydrophilici"J.Phys.Chem.B. 107. 14278-14282 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] M.Takeuchi, K.Tsujimaru, K.Sakamoto, M.Matsuoka, H.Yamashita, M.Anpo: "Effect of Pt Loading on the Photocatalytic Reactivity of Titanium Oxide Thin Films Prepared by Ion Engineering Techniques"Res.Chem.Intermed. 29. 619-629 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] H.Yamashita, M.Harada, J.Misaka, H.Nakao, M.Takeuchi, M.Anpo: "Application of Ion Beams for Preparation of TiO_2 Thin Film Photocatalysts Operatable under Visible Light Irradiation : Ion-assisted Deposition and Metal Ion-implantation"Nuclear Instrument and Method in Physics Research B. 206. 889-892 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] H.Yamashita, H.Nakao, M.Okazaki, M.Anpo: "Preparation of Hydrophobic Ti-containing Mesoporous Silica by the F-modificatio and Their Photocatalytic Degradation of Organic Pollutant Diluted in Water"Stud.Surf.Sci.Catal.. 795-798 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] H.Yamashita, K.Kida, K.Ikeue, Y.Kanazawa, K.Yoshizawa, M.Anpo: "Photocatalytic Epoxidation of Propene with Molecular Oxygen under Visible Light Irradiation on V Ion-implanted Ti-HMS and Cr-HMS Mesoporous Molecular Sieve"Stud.Surf.Sci.Catal. 597-600 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] S.C.Moon, Y.Matsumura, M.Kitano, M.Matsuoka, M.Anpo: "Hydrogen production using semiconducting oxide photocatalysts"Res.Chem.Intermed. 29. 233-256 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] Y.Hu, S.Higashimoto, G.Martra, JL.Zhang, M.Matsuoka, S.Coluccia, M.Anpo: "Local Structures of Active Sites on Ti-MCM-41 and Their Photocatalytic Reactivity for the Decomposition of NO"Catal.Lett. 90. 161-163 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] H.Yamashita, M.Harada, J.Misaka, M.Takeuchi, B.Neppolian, M.Anpo: "Photocatalytic Degradation of Organic Compounds Diluted in Water using Visible Light-responsive Metal Ion-implanted TiO2 Catalysts : Fe Ion-implanted TiO2"Catal.Today. 84. 191-196 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] Y.Hu, JL.Zhang, M.Minagawa, T.Ayusawa, M.Matsuoka, H.Yamashita, M.Anpo: "The Origin of the Decline in the Photocatalytic Activity of TiO_2 in the Decomposition of NO : TPD Spectra of the Adsorbed NO Species"Res.Chem.Intermed. 29. 125-136 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] M.Anpo, M.Takeuchi, H.Yamashita, S.Kishiguchi, A.Davidson, M.Che: "Semiconductor Photochemistry and Photophysics "Design and Development of New Titanium Dioxide Semiconductor Photocatalysts"(Eds. by V.Ramamurthy and K.S.Schanze)"Marcel Dekker, New York. 283-299 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] 安保正一(分担執筆): "先端科学シリーズI"可視光応答型の高機能な酸化チタン光触媒の開発"(日本化学会編)"丸善. 170-179 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] 安保正一: "イオン工学ハンドブック"環境調和型触媒としての光触媒""イオン工学研究所. 955-964 (2003)

    • Related Report
      2003 Annual Research Report

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Published: 2003-04-01   Modified: 2018-03-28  

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