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photocatalytic dehydrogenation of methanol by nonprecious-metal-complex bearing redox-active aminochalcogenolato

Research Project

Project/Area Number 15K17834
Research Category

Grant-in-Aid for Young Scientists (B)

Allocation TypeMulti-year Fund
Research Field Inorganic chemistry
Research InstitutionChuo University

Principal Investigator

matsumoto takeshi  中央大学, 理工学部, 助教 (40564109)

Project Period (FY) 2015-04-01 – 2017-03-31
Project Status Completed (Fiscal Year 2016)
Budget Amount *help
¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2016: ¥1,300,000 (Direct Cost: ¥1,000,000、Indirect Cost: ¥300,000)
Fiscal Year 2015: ¥2,860,000 (Direct Cost: ¥2,200,000、Indirect Cost: ¥660,000)
Keywords非貴金属錯体 / メタノール / 脱水素化 / 光反応 / ホルムアルデヒド / 水素ラジカル / アミノフェノール / レドックス活性配位子 / 錯体 / 光脱水素化 / MeOH / 光脱水素 / 非貴金属触媒 / 室温駆動 / 水素発生量子収率
Outline of Final Research Achievements

Dehydrogenation of anhydrous methanol is of great importance, given its ubiquity as an intermediate for the production of a large number of industrial chemicals. Since dehydrogenation of methanol is an endothermic reaction, heterogeneous or homogeneous precious-metal-based catalysts and high temperatures are usually required for this reaction to proceed. Here we report the photochemical dehydrogenation of anhydrous methanol at room temperature catalysed by o-aminophenol (apH2), o-aminophenolate (apH-) and the non-precious metal complex trans-[FeII(apH)2(MeOH)2]. Under excitation at 289 nm and in the absence of additional photosensitizers, these photocatalysts generate hydrogen and formaldehyde from anhydrous methanol with external quantum yields of 2.9%, 3.7% and 4.8%, respectively, which are the highest values reported so far to the best of our knowledge. Mechanistic investigations reveal that the photo-induced formation of hydrogen radicals triggers the reaction.

Report

(3 results)
  • 2016 Annual Research Report   Final Research Report ( PDF )
  • 2015 Research-status Report
  • Research Products

    (12 results)

All 2017 2016 2015 Other

All Journal Article (3 results) (of which Int'l Joint Research: 1 results,  Peer Reviewed: 3 results,  Open Access: 1 results,  Acknowledgement Compliant: 1 results) Presentation (5 results) (of which Int'l Joint Research: 2 results) Remarks (4 results)

  • [Journal Article] Structural and spectroscopic studies on the interactions of ortho-phenylenediamine and Li+, Na+, Mg2+, or Ca2+ ions2017

    • Author(s)
      Takeshi Matsumoto, Junki Ishii, Masanori Wakizaka, Ho-Chol Chang
    • Journal Title

      Chem. Lett.

      Volume: 46 Issue: 2 Pages: 232-235

    • DOI

      10.1246/cl.160997

    • NAID

      130005317076

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Dehydrogenation of Anhydrous Methanol at Room Temperature by o-Aminophenol-based Photocatalysts2016

    • Author(s)
      Masanori Wakizaka, Takeshi Matsumoto, Ryota Tanaka, Ho-Chol Chang
    • Journal Title

      Nature Commun.

      Volume: 7 Issue: 1 Pages: 1-11

    • DOI

      10.1038/ncomms12333

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Highly Polar Solvent-induced Disproportionation of a Cationic Pt(II)-Diimine Complex Containing an o-Semiquinonato2016

    • Author(s)
      山田将太、松本剛、脇坂聖憲、張浩徹
    • Journal Title

      Dalton Transaction

      Volume: 45 Issue: 12 Pages: 4974-4977

    • DOI

      10.1039/c6dt00487c

    • Related Report
      2015 Research-status Report
    • Peer Reviewed / Int'l Joint Research / Acknowledgement Compliant
  • [Presentation] o-アミノフェノラート錯体が示すメタノールの光脱水素化反応2017

    • Author(s)
      金 穂香、田中 亮太、脇坂 聖憲、松本 剛、張 浩徹
    • Organizer
      日本化学会第97春季年会
    • Place of Presentation
      慶応大学日吉キャンパス
    • Year and Date
      2017-03-16
    • Related Report
      2016 Annual Research Report
  • [Presentation] Photochemical Hydrogen Evolution Catalyzed by Iron(II) Complexes with Redox-active Ligands2016

    • Author(s)
      Ho-Chol Chang, Takeshi Matsumoto
    • Organizer
      6th International IUPAC Conference On Green Chemistry
    • Place of Presentation
      ベネチア、イタリア
    • Year and Date
      2016-09-04
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research
  • [Presentation] ビスアミノフェノール骨格による無水メタノールの光脱水素化2016

    • Author(s)
      松本 剛、 田中 亮太、 金 穂香、脇坂 聖憲、 張 浩徹
    • Organizer
      第28回配位化合物の光化学討論会
    • Place of Presentation
      京都工芸繊維大学、松ヶ崎キャンパス
    • Year and Date
      2016-08-08
    • Related Report
      2016 Annual Research Report
  • [Presentation] Photochemical Hydrogen Evolution Based on the Nonprecious Metal Complexes with Redox-active Ligands2016

    • Author(s)
      Takeshi Matsumoto, Ho-Chol Chang
    • Organizer
      42nd International Conference on Coordination Chemistry
    • Place of Presentation
      ブレスト、フランス
    • Year and Date
      2016-07-03
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research
  • [Presentation] ビスo-アミノフェノラト鉄(II)錯体が示す MeOH中における光化学反応2015

    • Author(s)
      松本剛, 田中亮太, 脇坂聖憲, 張浩徹
    • Organizer
      第27回配位化合物の光化学討論会
    • Place of Presentation
      佐渡インフォメーションセンター(あいぽーと佐渡)
    • Year and Date
      2015-08-07
    • Related Report
      2015 Research-status Report
  • [Remarks] 中央大学理工学部応用化学科分子物性化学研究室website_原著論文リスト

    • URL

      http://www.chem.chuo-u.ac.jp/~chang/achievements_treatise.html

    • Related Report
      2016 Annual Research Report
  • [Remarks] 中央大学理工学部応用化学科分子物性化学研究室website_学会発表リスト

    • URL

      http://www.chem.chuo-u.ac.jp/~chang/achievements_meeting.html

    • Related Report
      2016 Annual Research Report
  • [Remarks] 中央大学理工学部応用化学科分子物性化学研究室website_原著論文リスト(松本分)

    • URL

      http://www.chem.chuo-u.ac.jp/~chang/member04.html

    • Related Report
      2016 Annual Research Report
  • [Remarks] 中央大学理工学部応用化学科分子物性化学研究室website

    • URL

      http://www.chem.chuo-u.ac.jp/~chang/index.html

    • Related Report
      2015 Research-status Report

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Published: 2015-04-16   Modified: 2018-03-22  

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