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Design and preparation of dinitrogen complexes bearing an arsenic-containing ANA-type pincer ligand and their application to catalytic dinitogen fixation

Research Project

Project/Area Number 24750083
Research Category

Grant-in-Aid for Young Scientists (B)

Allocation TypeMulti-year Fund
Research Field Synthetic chemistry
Research InstitutionThe University of Tokyo

Principal Investigator

TANABE Yoshiaki  東京大学, 工学(系)研究科(研究院), 研究員 (20384737)

Co-Investigator(Renkei-kenkyūsha) NISHIBAYAHI Yoshiaki  東京大学, 大学院工学系研究科, 准教授 (40282579)
Project Period (FY) 2012-04-01 – 2014-03-31
Project Status Completed (Fiscal Year 2013)
Budget Amount *help
¥4,680,000 (Direct Cost: ¥3,600,000、Indirect Cost: ¥1,080,000)
Fiscal Year 2013: ¥2,340,000 (Direct Cost: ¥1,800,000、Indirect Cost: ¥540,000)
Fiscal Year 2012: ¥2,340,000 (Direct Cost: ¥1,800,000、Indirect Cost: ¥540,000)
Keywords窒素固定 / ヒ素 / アルシン / ピンサー型配位子 / ANA型配位子 / モリブデン / アンモニア / 触媒 / 窒素錯体 / タングステン
Research Abstract

A new catalytic system to convert molecular dinitrogen directly into ammonia has been achieved using a dinitrogen-bridged dimolybdenum complex with a PNP-type pincer ligand as a catalyst. Thus the use of an arsenic-containing ANA-type pincer ligand where phosphines in the PNP-type pincer ligand are substituted for arsines has been focuse on in this reserch, for arsines are known to have similar coordination modes to phosphines, but are also recognized to be more reluctant to oxidation, sterically bulkier, and poorer s-donors and p-acceptors compared to phosphines.
Novel mono- and dimolybdenum-dinitrogen complexes bearing an arsenic-containing ANA-type pincer ligand are prepared and characterized by X-ray analyses. These complexes afford a stoichiometric amount of ammonia by treatment with sulfuric acid at room temperature.

Report

(3 results)
  • 2013 Annual Research Report   Final Research Report ( PDF )
  • 2012 Research-status Report
  • Research Products

    (19 results)

All 2014 2013 2012 Other

All Journal Article (10 results) (of which Peer Reviewed: 8 results) Presentation (8 results) Remarks (1 results)

  • [Journal Article] Preparation and reactivity of molybdenum–dinitrogen complexes bearing an arsenic-containing ANA-type pincer ligand2013

    • Author(s)
      Tanabe Yoshiaki, Kuriyama Shogo, Arashiba Kazuya, Miyake Yoshihiro, Nakajima Kazunari, Nishibayashi Yoshiaki
    • Journal Title

      Chemical Communications

      Volume: 49 (81) Pages: 9290-9292

    • Related Report
      2013 Final Research Report
    • Peer Reviewed
  • [Journal Article] Design and Preparation of Molybdenum-Dinitrogen Complexes Bearing Ferrocenyldiphosphine and Pentamethylcyclopentadienyl Moieties as Auxiliary Ligands2013

    • Author(s)
      Miyazaki Takamasa, Tanabe Yoshiaki, Yuki Masahiro, Miyake Yoshihiro, Nakajima Kazunari, Nishibayashi Yoshiaki
    • Journal Title

      Chemistry–A European Journal

      Volume: 19 (36) Pages: 11874-11877

    • Related Report
      2013 Final Research Report
    • Peer Reviewed
  • [Journal Article] Developing more sustainable process for ammonia synthesis2013

    • Author(s)
      Tanabe Yoshiaki, Nishibayashi Yoshiaki
    • Journal Title

      Coordination Chemistry Reviews

      Volume: 257 (17–18) Pages: 2551-2564

    • Related Report
      2013 Final Research Report
    • Peer Reviewed
  • [Journal Article] 穏和な条件下での触媒的アンモニア合成法の開拓を目指して2013

    • Author(s)
      田辺資明, 西林仁昭
    • Journal Title

      月刊ファインケミカル

      Volume: 42 (7) Pages: 42-48

    • Related Report
      2013 Final Research Report
  • [Journal Article] Synthesis, Structure, and Reactivity of Group VI Metal Complexes Bearing Group IV Metallocenyldiphosphine Moieties and a Pentamethylcyclopentadienyl Ligand2013

    • Author(s)
      Miyazaki Takamasa, Tanabe Yoshiaki, Yuki Masahiro, Miyake Yoshihiro, Nishibayashi Yoshiaki
    • Journal Title

      Organometallics

      Volume: 32 (6) Pages: 2007-2013

    • Related Report
      2013 Final Research Report
    • Peer Reviewed
  • [Journal Article] Preparation and Reactivity of Molybdenum-Dinitrogen ComplexesBearing an Arsenic-Containing ANA-Type Pincer Ligand2013

    • Author(s)
      Yoshiaki Tanabe, Shogo Kuriyama, Kazuya Arashiba, Yoshihiro Miyake, Kazunari Nakajima, Yoshiaki Nishibayashi
    • Journal Title

      Chemical Communications

      Volume: 49 Issue: 81 Pages: 9290-9292

    • DOI

      10.1039/c3cc45228j

    • Related Report
      2013 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Developing more sustainable process for ammonia synthesis2013

    • Author(s)
      Tanabe, Yoshiaki; Yoshiaki Nishibayashi
    • Journal Title

      Coordination Chemistry Reviews

      Volume: 257 Issue: 17-18 Pages: 2551-2564

    • DOI

      10.1016/j.ccr.2013.02.010

    • Related Report
      2013 Annual Research Report 2012 Research-status Report
    • Peer Reviewed
  • [Journal Article] Design and Preparation of Molybdenum-Dinitrogen Complexes Bearing Ferrocenyldiphosphine and Pentamethylcyclopentadienyl Moieties as Auxiliary Ligands2013

    • Author(s)
      Takamasa Miyazaki, Yoshiaki Tanabe, Masahiro Yuki, Yoshihiro Miyake, Kazunari Nakajima, Yoshiaki Nishibayashi
    • Journal Title

      Chem. Eur. J. 2013, 19, 11874-11877

      Volume: 19 Issue: 36 Pages: 11874-11877

    • DOI

      10.1002/chem.201302700

    • Related Report
      2013 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Synthesis, Structure, and Reactivity of Group VI Metal Complexes Bearing Group IV Metallocenyldiphosphine Moieties and a Pentamethylcyclo pentadienyl Ligand2013

    • Author(s)
      Takamasa Miyazaki, Yoshiaki Tanabe, Masahiro Yuki, Yoshihiro Miyake, Yoshiaki Nishibayashi
    • Journal Title

      Organometallics

      Volume: 32 Issue: 6 Pages: 2007-2013

    • DOI

      10.1021/om400088d

    • Related Report
      2013 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 穏和な条件下での触媒的アンモニア合成法の開拓を目指して2013

    • Author(s)
      田辺資明、西林仁昭
    • Journal Title

      ファインケミカル

      Volume: 42

    • Related Report
      2012 Research-status Report
  • [Presentation] 含ヒ素ANA型ピンサー配位子を有するルテニウム錯体の合成と触媒能2014

    • Author(s)
      田辺資明, 栗山翔吾, 荒芝和也, 中島一成, 西林仁昭
    • Organizer
      日本化学会第94春季年会
    • Place of Presentation
      名古屋大学東山キャンパス(名古屋)(1F2-39)
    • Year and Date
      2014-03-27
    • Related Report
      2013 Final Research Report
  • [Presentation] フェロセニルジホスフィン配位子を有するモリブデン–二トリド錯体の特異な反応性2013

    • Author(s)
      宮崎貴匡, 田辺資明, 結城雅弘, 三宅由寛, 西林仁昭
    • Organizer
      日本化学会第93春季年会
    • Place of Presentation
      立命館大学びわこ・くさつキャンパス(草津)(1B6-11)
    • Year and Date
      2013-03-22
    • Related Report
      2013 Final Research Report
  • [Presentation] 含ヒ素ピンサー型配位子を有するモリブデン窒素錯体の合成と反応性2012

    • Author(s)
      田辺資明, 栗山翔吾, 荒芝和也, 三宅由寛, 西林仁昭
    • Organizer
      第39回有機典型元素化学討論会
    • Place of Presentation
      いわて県民情報交流センター(盛岡)(O-22)
    • Year and Date
      2012-12-06
    • Related Report
      2013 Final Research Report
  • [Presentation] Synthesis and Reactivity of Molybdenum Dinitrogen Complexes Bearing Ferrocenyl Diphosphine and Cyclopentadienyl Moieties2012

    • Author(s)
      Miyazaki Takamasa, Tanabe Yoshiaki, Yuki Masahiro, Miyake Yoshihiro, Nishibayashi Yoshiaki
    • Organizer
      The 25th International Conference on Organometallic Chemistry
    • Place of Presentation
      Lisbon University Campus (リスボン)(PB.14)
    • Year and Date
      2012-09-06
    • Related Report
      2013 Final Research Report
  • [Presentation] Synthesis and Reactivity of Coordinatively Unsaturated Diruthenium Complex Bridged by Hybrid Phosphido and Sulfido Ligands2012

    • Author(s)
      Tanabe Yoshiaki, Miyake Yoshihiro, Moriyama Taichi, Endo Satoshi, Nishibayashi Yoshiaki
    • Organizer
      The 25th International Conference on Organometallic Chemistry
    • Place of Presentation
      Lisbon University Campus (リスボン)(PA.5)
    • Year and Date
      2012-09-04
    • Related Report
      2013 Final Research Report
  • [Presentation] 含ヒ素ANA型ピンサー配位子を有するルテニウム錯体の合成と触媒能

    • Author(s)
      田辺資明, 栗山翔吾, 荒芝和也, 中島一成, 西林仁昭
    • Organizer
      日本化学会第94春季年会
    • Place of Presentation
      名古屋大学東山キャンパス, 愛知県
    • Related Report
      2013 Annual Research Report
  • [Presentation] 含ヒ素ピンサー型配位子を有するモリブデン窒素錯体の合成と反応性

    • Author(s)
      田辺資明、栗山翔吾、荒芝和也、三宅由寛、西林仁昭
    • Organizer
      第39回有機典型元素化学討論会
    • Place of Presentation
      盛岡
    • Related Report
      2012 Research-status Report
  • [Presentation] フェロセニルジホスフィン配位子を有するモリブデン–二トリド錯体の特異な反応性

    • Author(s)
      宮崎貴匡、田辺資明、結城雅弘、三宅由寛、西林仁昭
    • Organizer
      日本化学会第93春季年会
    • Place of Presentation
      草津
    • Related Report
      2012 Research-status Report
  • [Remarks]

    • URL

      http://webpark1495.sakura.ne.jp/index.htm

    • Related Report
      2013 Final Research Report

URL: 

Published: 2013-05-31   Modified: 2019-07-29  

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