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高効率水素生成を駆動するナノ構造制御した可視光応答型金属触媒の開発

Research Project

Project/Area Number 17F17381
Research Category

Grant-in-Aid for JSPS Fellows

Allocation TypeSingle-year Grants
Section外国
Research Field Catalyst/Resource chemical process
Research InstitutionOsaka University

Principal Investigator

山下 弘巳  大阪大学, 工学研究科, 教授 (40200688)

Co-Investigator(Kenkyū-buntansha) NAVLANI GARCIA MIRIAM  大阪大学, 工学(系)研究科(研究院), 外国人特別研究員
Project Period (FY) 2017-11-10 – 2020-03-31
Project Status Granted (Fiscal Year 2018)
Budget Amount *help
¥2,200,000 (Direct Cost: ¥2,200,000)
Fiscal Year 2018: ¥1,100,000 (Direct Cost: ¥1,100,000)
Fiscal Year 2017: ¥600,000 (Direct Cost: ¥600,000)
Keywordsギ酸 / 水素キャリア / 合金ナノ粒子 / 窒素ドープカーボン / プラズモン特性 / ナノ粒子 / バイメタル / 金属触媒 / 光触媒
Outline of Annual Research Achievements

水素エネルギー社会を構築するためには、水素を貯蔵・輸送可能な形態に変換して、時間や空間を超えて需要先へ届ける技術を構築する必要がある。安全(非可燃性、非爆発性)かつエネルギー密度が高い水素キャリアとして、ギ酸(HCOOH, 52 gH2/L)やアンモニウムボラン(NH3BH3), 146 gH2/L)が注目されている。
本研究課題では、ギ酸ならびにアンモニウムボランをエネルギーキャリアとした高効率水素貯蔵発生システムの構築をターゲットとし、『水素貯蔵材料からの水素生成触媒』の開発を行った。特に弱塩基性担体のカーボンナイトライド(C3N4)に固定化したPdCo合金が高活性を示すことを報告した。Coのみでは反応しないが、Pdと合金化することで電子的にリッチなPd種が生成し、Pd単独よりも飛躍的に活性が向上する。また、調製した触媒のキャラクタリゼーションを、比表面積測定、XRD、SEMにより解析した。弱塩基性担体は、金属表面へのギ酸の吸着濃縮効果、ならびにギ酸O-H結合の解離促進という役割を果たしていることを実験、理論計算から明らかにし、重要な触媒設計指針を得るに至った。
さらにこの研究を発展させ、細孔径、ドープ量を制御した様々な窒素ドープカーボンを新規に調製し、Ru触媒の担体として用いることでより高活性な触媒の開発に成功した。また、窒素ドープ量によりRuの粒子径が大きく変化し、粒子径とアンモニアボランからの水素生成活性に良い相関関係があることを見出した。

Current Status of Research Progress
Current Status of Research Progress

2: Research has progressed on the whole more than it was originally planned.

Reason

研究開始時期に比べ約2倍以上の触媒活性の向上が達成できた。また、詳細なキャラクタリゼーション並びに理論計算からのアプローチで重要な触媒設計指針を構築できた。

Strategy for Future Research Activity

詳細な構造解析ならびに理論計算からの支援による反応機構の検討により、次世代触媒開発の重要な設計指針も構築できた。しかしながら更なる高活性化、耐久性の向上が課題として残る。具体的にはさらに活性の一桁向上を目指す必要がある。そのためには、第一列遷移金属を加えた、三元系合金合金ナノ粒子の合成、ならびに担体表面修飾などの更なる改良を検討している。

Report

(2 results)
  • 2018 Annual Research Report
  • 2017 Annual Research Report
  • Research Products

    (16 results)

All 2019 2018 2017 Other

All Int'l Joint Research (1 results) Journal Article (10 results) (of which Int'l Joint Research: 10 results,  Peer Reviewed: 10 results,  Open Access: 9 results) Presentation (4 results) (of which Int'l Joint Research: 4 results) Remarks (1 results)

  • [Int'l Joint Research] アリカンテ大学(スペイン)

    • Related Report
      2017 Annual Research Report
  • [Journal Article] Non-noble metal doped perovskite as a promising catalyst for ammonia borane dehydrogenation2019

    • Author(s)
      D. Salinas-Torees, M. Navlani-Garcia, Y. Kuwahara, K. Mori, and H. Yamashita
    • Journal Title

      Catalysis Today

      Volume: 印刷中 Pages: 6-11

    • DOI

      10.1016/j.cattod.2019.03.072

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Tailoring the size and shape of colloidal noble metal nanocrystals as a valuable tool in catalysis2019

    • Author(s)
      M. Navlani-Garcia, D. Salinas-Torees, K. Mori, Y. Kuwahara and H. Yamashita
    • Journal Title

      Catalsis Survey from Asia

      Volume: 印刷中 Issue: 3 Pages: 127-148

    • DOI

      10.1007/s10563-019-09271-7

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Enhanced formic acid dehydrogenation by the synergistic alloying effect of PdCo catalysts supported on graphitic carbon nitride2019

    • Author(s)
      M. Navlani-Garcia, D. Salinas-Torees, K. Mori, Y. Kuwahara and H. Yamashita
    • Journal Title

      International Journal of Hydrogen Energy

      Volume: 印刷中 Issue: 53 Pages: 28483-28493

    • DOI

      10.1016/j.ijhydene.2018.11.057

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Insights on palladium decorated nitrogen-doped carbon xerogels for the hydrogen production from formic acid2019

    • Author(s)
      Navlani-Garcia Miriam、Salinas-Torres David、Mori Kohsuke、Leonard Alexandre F.、Kuwahara Yasutaka、Job Nathalie、Yamashita Hiromi
    • Journal Title

      Catalysis Today

      Volume: 324 Pages: 90-96

    • DOI

      10.1016/j.cattod.2018.06.013

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Nitrogen-doped carbon materials as a promising platform toward the efficient catalysis for hydrogen generation2019

    • Author(s)
      Salinas-Torres David、Navlani-Garcia Miriam、Mori Kohsuke、Kuwahara Yasutaka、Yamashita Hiromi
    • Journal Title

      Applied Catalysis A: General

      Volume: 571 Pages: 25-41

    • DOI

      10.1016/j.apcata.2018.11.034

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Recent Strategies Targeting the Efficient Hydrogen Production from Chemical Hydrogen Storage Materials over Carbon-supported Catalysts2018

    • Author(s)
      Miriam Navlani-Garcia, Kohsuke Mori, Yasutaka Kuwahara, Hiromi Yamashita
    • Journal Title

      NPG Asia Materials

      Volume: in press Issue: 4 Pages: 277-292

    • DOI

      10.1038/s41427-018-0025-6

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Visible-Light-Enhanced Catalytic Activity of Ru Nanoparticles over Carbon Modified g-C3N42018

    • Author(s)
      Miriam Navlani-Garcia, Priyanka Verma, Yasutaka Kuwahara, Takashi Kamegawa, Kohsuke Mori, Hiromi Yamashita
    • Journal Title

      Photochemical & Photobiology A:Chemistry

      Volume: 358 Pages: 327-333

    • DOI

      10.1016/j.jphotochem.2017.09.007

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Production of H2 from Ammonia Borane Solution Utilizing Surface Plasmon Resonance Enhancement of Photocatalytic Activity with Pd Nanoparticle Decorated-Cu2-xS Nanowires2017

    • Author(s)
      P.-H. Liu, M. Wen, C.-S. Tan, M. Navlani-García, Y. Kuwahara, K. Mori, H. Yamashita, L.-J, Chen
    • Journal Title

      Nano Energy

      Volume: 31 Pages: 57-63

    • DOI

      10.1016/j.nanoen.2016.10.064

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Palladium Nanoparticles Supported on Titanium Doped Graphitic Carbon Nitride for Formic Acid Dehydrogenation2017

    • Author(s)
      Yongmei Wu, Meicheng Wen, Miriam Navlani-Garcia, Yasutaka Kuwahara, Kohsuke Mori, Hiromi Yamashita
    • Journal Title

      Chemistry-An Asian Journal

      Volume: 12 Issue: 8 Pages: 860-867

    • DOI

      10.1002/asia.201700041

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Morphology Controlled Pd Nanocrystals as Catalysts in Tandem Dehydrogenation-hydrogenation Reactions2017

    • Author(s)
      M. Navlani-Garcia, P. Verma, K. Mori, Y. Kuwahara,H. Yamashita
    • Journal Title

      Journal of Chemical Science

      Volume: 129 Issue: 11 Pages: 1695-1703

    • DOI

      10.1007/s12039-017-1370-7

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Presentation] The 8th Tokyo Conference on Advanced Catalytic Science and Technology2018

    • Author(s)
      ○Miriam NAVLANI-GARCIA, Kohsuke MORI, Yasutaka KUWAHARA, Hiromi YAMASHITA
    • Organizer
      TOCAT8, The 8th Tokyo Conference on Advanced Catalytic Science and Technology
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Insights on Palladium Decorated Nitrogen-Containing Carbon Xerogels for the H2 Production2018

    • Author(s)
      ○David Salinas-Torres, Miriam Navlani-Garcia, Kohsuke Mori, Yasutaka Kuwahara, Nathalie Job, Hiromi Yamashita
    • Organizer
      ZMPC2018, International Symposium on Zeolites and Microporous Crystals 2018
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Formic Acid Dehydrogenation over Pd-based Catalysts2018

    • Author(s)
      ○Miriam Navlani-Garcia, Kohsuke Mori, Yasutaka Kuwahara, Hiromi Yamashita
    • Organizer
      NPC2018, International Symposium on Nanostructured Photocatalysts and Catalysts
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Hydrogen production from formic acid over carbon-supported Pd nanoparticles: effect of the nanoparticle size2017

    • Author(s)
      〇Miriam Navlani-Garcia, Kohsuke Mori, Yasutaka Kuwahara, Hiromi Yamashita
    • Organizer
      Europacat2017, 13th European Congress on Catalysis
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Remarks] 山下研究室ホームページ

    • URL

      http://www.mat.eng.osaka-u.ac.jp/msp1/MSP1-HomeJ.htm

    • Related Report
      2017 Annual Research Report

URL: 

Published: 2017-11-13   Modified: 2024-03-26  

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