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規整表面上に精密集積した金属錯体触媒の開発

Publicly Offered Research

Project AreaMolecule Activation Directed toward Straightforward Synthesis
Project/Area Number 23105503
Research Category

Grant-in-Aid for Scientific Research on Innovative Areas (Research in a proposed research area)

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

Principal Investigator

原 賢二  北海道大学, 触媒化学研究センター, 准教授 (10333593)

Project Period (FY) 2011-04-01 – 2013-03-31
Project Status Completed (Fiscal Year 2012)
Budget Amount *help
¥7,020,000 (Direct Cost: ¥5,400,000、Indirect Cost: ¥1,620,000)
Fiscal Year 2012: ¥3,510,000 (Direct Cost: ¥2,700,000、Indirect Cost: ¥810,000)
Fiscal Year 2011: ¥3,510,000 (Direct Cost: ¥2,700,000、Indirect Cost: ¥810,000)
Keywords規整表面 / 単分子層 / イソシアニド / 金表面 / メソポーラスシリカ / 有機シリカ / ゼオライト鋳型炭素 / 白金 / 触媒調製 / 金 / ロジウム / 水素化
Outline of Annual Research Achievements

本研究課題では、触媒調製の新しいアプローチとして、構造が規整された表面上に分子レベルで精密に金属錯体を集積することによって特異かつ有用な触媒反応場を構築する手法の開発を試みている。今年度は、金表面上における種々の高密度なジイソシアニド金属錯体単分子層の形成とその触媒機能、および、規則性メソポーラス有機シリカ表面上における金属錯体高密度固定化について検討を行った。
有機化合物が表面上で高密度な自己組織化単分子層を形成する現象は種々の機能性材料の調製手法となる。この現象を触媒調製に利用した例は少ないが、特異的な触媒反応場の構築手法として展開できる可能性を秘めている。最も利用されている自己組織化単分子層は金表面上のチオール分子の系であるが、我々は新展開を図るべく、研究例の非常に限られたイソシアニド単分子層を触媒反応場の構築に利用することに着手した。今年度は、金表面上に新たに高密度なニッケルおよび鉄―ジイソシアニド単分子層の形成を行い、その触媒機能を精査した。
メソポーラスシリカは担持金属触媒の担体として広く用いられている。規則的なメソ細孔空間内に活性金属種を導入して特殊な触媒反応場として利用する試みが報告されているが、配位子分子を導入するために元来のメソ細孔の規則性が失われることが多い。そこで今年度の研究では、配位子分子が骨格内に組み込まれた規則性メソポーラス有機シリカを活用することとした。特に、特異な触媒機能の発現が期待される複核錯体構造としての高密度固定化を可能にする手法の確立を目指した。また、今年度の検討では、メソポーラスシリカおよびゼオライト鋳型炭素に担持した白金ナノ粒子がそれぞれ微量エチレンの低温酸化およびフェニルアセチレンの部分水素化において優れた触媒機能を有することを見出した。

Research Progress Status

24年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

24年度が最終年度であるため、記入しない。

Report

(2 results)
  • 2012 Annual Research Report
  • 2011 Annual Research Report
  • Research Products

    (44 results)

All 2013 2012 2011

All Journal Article (13 results) (of which Peer Reviewed: 13 results) Presentation (30 results) (of which Invited: 5 results) Book (1 results)

  • [Journal Article] Low-Temperature Oxidation of Ethylene over Platinum Nanoparticles Supported on Mesoporous Silica2013

    • Author(s)
      Chuanxia Jiang, Kenji Hara, Atsushi Fukuoka
    • Journal Title

      Angewandte Chemie International Edition

      Volume: 52巻(in press) Issue: 23 Pages: 6084-6087

    • DOI

      10.1002/anie.201300469

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] High-Yielding One-Pot Synthesis of Glucose from Cellulose Using Simple Activated Carbons and Trace Hydrochloric Acid2013

    • Author(s)
      H. Kobayashi, M. Yabushita, T.Komanoya, K. Hara, I. Fujita, A. Fukuoka
    • Journal Title

      ACS Catalysis

      Volume: 3 Issue: 4 Pages: 581-587

    • DOI

      10.1021/cs300845f

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Phase Change of Nickel Phosphide Catalysts in the Conversion of Cellulose into Sorbitol2012

    • Author(s)
      P. Yang, H. Kobayashi, K. Hara and A. Fukuoka
    • Journal Title

      ChemSusChem

      Volume: 5 Pages: 920-926

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 1-Butanol Synthesis from Ethanol over Strontium Phosphate Hydroxyapatite Catalysts with Various Sr/P Ratios2012

    • Author(s)
      S. Ogo, A. Onda, Y. Iwasa, K. Hara, A. Fukuoka,K. Yanagisawa
    • Journal Title

      Journal of Catalysis

      Volume: 296巻 Pages: 24-30

    • DOI

      10.1016/j.jcat.2012.08.019

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Selective and Efficient Silylation of Mesoporous Silica : A Quantitative Assessment of Synthetic Strategies by Solid-State NMR2012

    • Author(s)
      Hara, K.; Akahane, S.; Wiench, J.W.; Burgin, B.R.; Ishito, N.; Lin, V.S.-Y., Fukuoka, A.; Pruski, M
    • Journal Title

      J.Phys.Chem.C

      Volume: 116 Issue: 12 Pages: 7083-7090

    • DOI

      10.1021/jp300580f

    • Related Report
      2011 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Intrinsic Catalytic Role of Mesoporous Silica in Preferential Oxidation of Carbon Monoxide in Excess Hydrogen2012

    • Author(s)
      Huang, S.; Hara, K.; Fukuoka, A.
    • Journal Title

      Chem.Eur.J.

      Volume: 18 Issue: 15 Pages: 4738-4747

    • DOI

      10.1002/chem.201102256

    • Related Report
      2011 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Palladium (II)-exchanged hydroxyapatite-catalyzed Suzuki-Miyaura-type cross-coupling reactions with potassiumaryltrifluoroborates2012

    • Author(s)
      Yoshiro Masuyama, Yutaka Sugioka, Shiori Chonan, Masahiro Fujita, Noriyuki Suzuki, Kenji Hara, Atsushi Fukuoka
    • Journal Title

      Journal of Molecular Catalysis, A.Chemical

      Volume: 352 Pages: 81-85

    • DOI

      10.1016/j.molcata.2011.10.017

    • Related Report
      2011 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Remarkable Effect of Ordered Mesoporous Carbon Support in Tantalum Oxide-catalyzed Selective Epoxidation of Cyclooctene2011

    • Author(s)
      Lin, M.-L.; Hara, K.; Okubo, Y.; Yanagi, M.; Nambu, H.; Fukuoka, A.
    • Journal Title

      Catal.Comm.

      Volume: 12 Issue: 13 Pages: 1228-1230

    • DOI

      10.1016/j.catcom.2011.04.023

    • NAID

      120003242991

    • Related Report
      2011 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Hydroxyapatite-supported copper (II)-catalyzed azide-alkyne [3+2] cycloaddition with neither reducing agents nor bases in water2011

    • Author(s)
      Yoshiro Masuyama, Kazuki Yoshikawa, Noriyuki Suzuki, Kenji Hara, Atsushi Fukuoka
    • Journal Title

      Tetrahedron Letters

      Volume: 52 Issue: 51 Pages: 6916-6918

    • DOI

      10.1016/j.tetlet.2011.10.060

    • Related Report
      2011 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Hydrogenolysis of sugar beet fiber by supported metal catalyst2011

    • Author(s)
      S. K. Guha, H. Kobayashi, K. Hara, H.Kikuchi, T. Aritsuka, A. Fukuoka
    • Journal Title

      Catalysis Communications

      Volume: 12 Issue: 11 Pages: 980-983

    • DOI

      10.1016/j.catcom.2011.02.017

    • NAID

      120003118179

    • Related Report
      2011 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Catalysis and characterization of carbon-supported ruthenium for cellulose hydrolysis2011

    • Author(s)
      Tasuku Komanoya
    • Journal Title

      Applied Catalysis A : General

      Volume: 407 Issue: 1-2 Pages: 188-194

    • DOI

      10.1016/j.apcata.2011.08.039

    • Related Report
      2011 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Hydrodeoxygenation of Phenols as Lignin Models under Acid-Free Conditions withCarbon-Supported Platinum Catalysts2011

    • Author(s)
      H. Ohta, H. Kobayashi, K. Hara, A. Fukuoka
    • Journal Title

      Chemical Communications

      Volume: 47 Issue: 44 Pages: 12209-12211

    • DOI

      10.1039/c1cc14859a

    • Related Report
      2011 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Conversion of cellulose into renewable chemicals by supported metal catalysis2011

    • Author(s)
      H. Kobayashi, T. Komanoya, S. K.Guha, K. Hara, A. Fukuoka
    • Journal Title

      Applied Catalysis A: General

      Volume: 409-410(合併号) Pages: 13-20

    • DOI

      10.1016/j.apcata.2011.10.014

    • Related Report
      2011 Annual Research Report
    • Peer Reviewed
  • [Presentation] Densely Packed Monolayer of Metal-Diisocyanide on Gold Surface; Preparation and Application in Catalysis2013

    • Author(s)
      K. Hara, S .Jagtap Y. Kaji, W.J. Chun, A. Fukuoka
    • Organizer
      Collaborative Conference on Materials Research (CCMR) 2013
    • Place of Presentation
      Ramada Plaza Jeju Hotel(大韓民国)
    • Year and Date
      2013-06-24
    • Related Report
      2012 Annual Research Report
    • Invited
  • [Presentation] Surface Selective Silylation of Mesoporous Siica MCM-41; Precise Characterization and Cu Catalysis2013

    • Author(s)
      Kenji Hara, Saiko Akahane, Jerzy W. Wiench, Breina R. Burgin, Nobuhiro Ishito, Victor S.-Y. Lin, Atsushi Fukuoka, Marek Pruski
    • Organizer
      8th International Mesostructured Materials Symposium (IMMS-8, IMMS2013)
    • Place of Presentation
      淡路夢舞台国際会議場(淡路市)
    • Year and Date
      2013-05-20
    • Related Report
      2012 Annual Research Report
  • [Presentation] 高密度ジイソシアニド-金属錯体単分子層の特異な触媒機能とXAFS構造解析2013

    • Author(s)
      原 賢二、Sachin Jagtap、難波 光太郎、梶 義規、田 旺帝、朝倉 清高、福岡
    • Organizer
      第30回PFシンポジウム
    • Place of Presentation
      つくば国際会議場(つくば市)
    • Year and Date
      2013-03-15
    • Related Report
      2012 Annual Research Report
  • [Presentation] 規整表面上における高密度金属錯体単分子層の形成と触媒反応への応用2013

    • Author(s)
      原 賢二、Sachin Jagtap、難波 光太郎、梶 義規、福岡 淳
    • Organizer
      平成24年度日本表面科学会東北・北海道支部学術講演会
    • Place of Presentation
      日本大学工学部(郡山市)
    • Year and Date
      2013-03-11
    • Related Report
      2012 Annual Research Report
    • Invited
  • [Presentation] Densely Packed Monolayer of Metal-Diisocynide on Gold Surface as Highly Active and Selective Catalysis2012

    • Author(s)
      K. Hara, K. Namba, S. Jagtap, Y. Kaji, W.J. Chun, A. Fukuoka
    • Organizer
      2nd International Symposium on Molecular Activation
    • Place of Presentation
      東大寺総合文化センター(奈良市)
    • Year and Date
      2012-11-11
    • Related Report
      2012 Annual Research Report
  • [Presentation] Surface Selective Silylation of Mesoporous Siica MCM-41; Precise Characterization and Cu Catalysis2012

    • Author(s)
      Kenji Hara, Saiko Akahane, Jerzy W. Wiench, Breina R. Burgin, Nobuhiro Ishito, Victor S.-Y. Lin, Atsushi Fukuoka, Marek Pruski
    • Organizer
      International Conference on Emerging Advanced Nanomaterials (ICEAN) 2012
    • Place of Presentation
      Mercure Hotel(Australia)
    • Year and Date
      2012-10-22
    • Related Report
      2012 Annual Research Report
    • Invited
  • [Presentation] Densely Packed Monolayer of Rh- and Cu-Diisocynide on Gold Surface as Platforms for Highly Active and Selective Catalysis2012

    • Author(s)
      K. Hara, K. Namba, S. Jagtap, Y. Kaji, W.J. Chun, A. Fukuoka
    • Organizer
      Cambodian Malaysian Chemical Conference (CMCC) 2012
    • Place of Presentation
      Angkor Century Resort Spa(Cambodia)
    • Year and Date
      2012-10-19
    • Related Report
      2012 Annual Research Report
    • Invited
  • [Presentation] 金表面上におけるジイソシアニド銅錯体単分子層の作製と触媒反応への応用2012

    • Author(s)
      難波 光太郎, 原 賢二, 福岡 淳
    • Organizer
      第110回触媒討論会
    • Place of Presentation
      九州大学伊都キャンパス(福岡市)
    • Year and Date
      2012-09-24
    • Related Report
      2012 Annual Research Report
  • [Presentation] 金表面上におけるジイソシアニド銅錯体単分子層の作製と触媒反応への応用2012

    • Author(s)
      難波 光太郎, 原 賢二, 福岡 淳
    • Organizer
      第59回有機金属化学討論会
    • Place of Presentation
      大阪大学吹田キャンパス(吹田市)
    • Year and Date
      2012-09-13
    • Related Report
      2012 Annual Research Report
  • [Presentation] Monolayer of Diisocyanide on Gold Surface as a Platform for Rh-Catalyzed Selective Hydrogenation2012

    • Author(s)
      Kenji Hara, Sachin Jagtap, Yoshinori Kaji, Atsushi Fukuoka
    • Organizer
      The 6th International Conference on Gold Science, Technology and its Applications (Gold 2012)
    • Place of Presentation
      京王プラザホテル東京(東京都新宿区)
    • Year and Date
      2012-09-05
    • Related Report
      2012 Annual Research Report
  • [Presentation] Densely packed monolayer of metal complex on gold surface as platform for selective catalysis2012

    • Author(s)
      Kenji Hara, Sachin Jagtap, Yoshinori Kaji, Atsushi Fukuoka
    • Organizer
      International Symposium on Zeolite and Microporous Crystals (ZMPC) 2012
    • Place of Presentation
      アステールプラザ(広島市)
    • Year and Date
      2012-07-28
    • Related Report
      2012 Annual Research Report
  • [Presentation] Oxidation of ethylene over Pt nanoparticles supported on mesoporous silica2012

    • Author(s)
      Chuanxia Jiang, Kenji Hara, Atsushi Fukuoka
    • Organizer
      International Symposium on Zeolite and Microporous Crystals (ZMPC) 2012
    • Place of Presentation
      アステールプラザ(広島市)
    • Year and Date
      2012-07-28
    • Related Report
      2012 Annual Research Report
  • [Presentation] Monolayer of diisocyanide on Au surface as a platform for Rh catalysis of 1,4-hydrogenation of α,szlig;-unsaturated carbonyl compounds2012

    • Author(s)
      K. Hara, S. Jagtap, Y. Kaji, A. Fukuoka
    • Organizer
      15th International Congress on Catalysis 2012
    • Place of Presentation
      InternationaCongress Center Munich(ドイツ)
    • Year and Date
      2012-07-01
    • Related Report
      2012 Annual Research Report
  • [Presentation] 表面上での金属ジイソシアニド錯体単分子層の形成と有機分子変換反応への応用2012

    • Author(s)
      原 賢二
    • Organizer
      電気化学会北海道支部第18回若手研究者交流会
    • Place of Presentation
      おたる自然の家おこばち山荘(小樽市)
    • Year and Date
      2012-06-23
    • Related Report
      2012 Annual Research Report
    • Invited
  • [Presentation] Monolayer of diisocyanide on Au surface as a platform for Rh catalysis of 1,4-hydrogenation of α,szlig;-unsaturated carbonyl compounds2012

    • Author(s)
      K. Hara, S. Jagtap, Y. Kaji, A. Fukuoka
    • Organizer
      International Association of Colloid and Interface Scientists, Conference (IACIS) 2012
    • Place of Presentation
      仙台国際センター(仙台市)
    • Year and Date
      2012-05-14
    • Related Report
      2012 Annual Research Report
  • [Presentation] Complete Oxidation of Ethylene over Supported Pt Nanoparticles at Low Temperature2012

    • Author(s)
      Chuanxia Jiang, Kenji Hara, Atsushi Fukuoka
    • Organizer
      第109回触媒討論会
    • Place of Presentation
      東京工業大学(東京都目黒区)
    • Year and Date
      2012-03-28
    • Related Report
      2011 Annual Research Report
  • [Presentation] ジイソシアニド金属錯体単分子層の形成と触媒への応用2012

    • Author(s)
      難波光太郎、原賢二、福岡淳
    • Organizer
      化学系学協会北海道支部2012年冬季研究発表会
    • Place of Presentation
      北海道大学(札幌市)
    • Year and Date
      2012-01-31
    • Related Report
      2011 Annual Research Report
  • [Presentation] 二酸化炭素の化学変換を指向した固体触媒の開発2012

    • Author(s)
      石戸信広、原賢二、福岡淳
    • Organizer
      化学系学協会北海道支部2012年冬季研究発表会
    • Place of Presentation
      北海道大学(札幌市)
    • Year and Date
      2012-01-31
    • Related Report
      2011 Annual Research Report
  • [Presentation] Preparation and Catalysis of Monolayer of Rh-diisocyanide on Gold Surface2012

    • Author(s)
      Kenji Hara, Sachin Jagtap, Yoshinori Kaji, Atsushi Fukuoka
    • Organizer
      CRC International Symposium on Green & Sustainable Catalysis : from Theoretical and Fundamental Aspects to Catalyst Design
    • Place of Presentation
      北海道大学(札幌市)
    • Year and Date
      2012-01-26
    • Related Report
      2011 Annual Research Report
  • [Presentation] Oxidation of Ethylene over Pt Nanoparticles Supported on Mesoporous Silica2012

    • Author(s)
      Chuanxia Jiang, Kenji Hara, Atsushi Fukuoka
    • Organizer
      CRC International Symposium on Green & Sustainable Catalysis : from Theoretical and Fundamental Aspects to Catalyst Design
    • Place of Presentation
      北海道大学(札幌市)
    • Year and Date
      2012-01-26
    • Related Report
      2011 Annual Research Report
  • [Presentation] 規整表面上における金属錯体の精密集積による反応場設計2012

    • Author(s)
      原賢二
    • Organizer
      触媒学会横浜地区講演会
    • Place of Presentation
      東京工業大学(横浜市)(招待講演)
    • Year and Date
      2012-01-24
    • Related Report
      2011 Annual Research Report
  • [Presentation] 規整表面上に金属錯体を集積した触媒反応場の構築と応用2012

    • Author(s)
      原賢二
    • Organizer
      文部科学省科学研究費補助金「新学術領域研究」直截的物質変換をめざした分子活性化法の開発第2回公開シンポジウム
    • Place of Presentation
      京都大学(宇治市)
    • Year and Date
      2012-01-20
    • Related Report
      2011 Annual Research Report
  • [Presentation] 規整表面上での触媒反応場の構築と応用2011

    • Author(s)
      原賢二
    • Organizer
      長崎大学第2期中期目標・中期計画重点研究課題「次世代エネルギー物質科学の基盤構築」平成23年度第1回講演会
    • Place of Presentation
      長崎大学(長崎市)(招待講演)
    • Year and Date
      2011-12-08
    • Related Report
      2011 Annual Research Report
  • [Presentation] Densely Packed Monolayer of Rh-Diisocyanide on Gold Surface as Recyclable Catalyst for Hydrogenation of Enones2011

    • Author(s)
      Hara, K
    • Organizer
      International Symposium and the Third Iwasawa Conference on Catalysis and Surface Science for Efficient Utilization of Carbon Resources and Related Topics
    • Place of Presentation
      Xiamen University (China)(招待講演)
    • Year and Date
      2011-12-04
    • Related Report
      2011 Annual Research Report
  • [Presentation] Densely Packed Monolayer of Metal Complex on Gold Surface : Application in Selective Catalysis2011

    • Author(s)
      Hara, K
    • Organizer
      9th Asian Conference on Chemical Sensors
    • Place of Presentation
      Chientan Youth Activity Center (Taiwan)(招待講演)
    • Year and Date
      2011-11-15
    • Related Report
      2011 Annual Research Report
  • [Presentation] Densely Packed Monolayer of Rh-Diisocyanide on Gold Surface as Recyclable Catalyst for Hydrogenation of Alkynes and Enones2011

    • Author(s)
      Kenji Hara, Sachin Jagtap, Yoshinori Kaji, Atsushi Fukuoka
    • Organizer
      1st International Symposium on Molecular Activation
    • Place of Presentation
      淡路夢舞台国際会議場(淡路市)
    • Year and Date
      2011-11-10
    • Related Report
      2011 Annual Research Report
  • [Presentation] 規整表面上における金属錯体の精密集積による反応場設計2011

    • Author(s)
      原賢二
    • Organizer
      統合物質創製化学推進事業第2回統合物質シンポジウム「化学合成力と機能創出」
    • Place of Presentation
      名古屋大学(名古屋市)
    • Year and Date
      2011-11-07
    • Related Report
      2011 Annual Research Report
  • [Presentation] 金表面上におけるロジウム-ジイソシアニド錯体単分子層の形成と触媒機能2011

    • Author(s)
      原賢二, Sachin Jagtap, 梶義規, 福岡淳
    • Organizer
      統合物質創製化学推進事業第2回統合物質シンポジウム「化学合成力と機能創出」
    • Place of Presentation
      名古屋大学(名古屋市)
    • Year and Date
      2011-11-06
    • Related Report
      2011 Annual Research Report
  • [Presentation] Preparation and Catalysis of Densely Packed Monolayer of Rhodium-Diisocyanide Monolayer on Gold Suface2011

    • Author(s)
      Hara, K
    • Organizer
      The 14th Asian Chemical Congress 2011
    • Place of Presentation
      クイーンシリキットコンベンションセンター(Thailand)(招待講演)
    • Year and Date
      2011-09-08
    • Related Report
      2011 Annual Research Report
  • [Presentation] 金表面上に高密度に集積化した単分子層を利用する触媒反応2011

    • Author(s)
      原賢二
    • Organizer
      ワークショップ「ナノ粒子触媒の構造制御と表面化学」
    • Place of Presentation
      北海道大学(札幌市)
    • Year and Date
      2011-06-28
    • Related Report
      2011 Annual Research Report
  • [Book] 触媒調製ハンドブック、岩本正和監修「Pt/メソポーラスシリカ」2011

    • Author(s)
      原賢二、福岡淳
    • Total Pages
      2
    • Publisher
      エヌ・ティー・エス出版
    • Related Report
      2011 Annual Research Report

URL: 

Published: 2011-04-06   Modified: 2018-03-28  

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