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Photoreduction mechanism undelying laser-induced particle formation of metal ion complexes

Research Project

Project/Area Number 20K05426
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Review Section Basic Section 32010:Fundamental physical chemistry-related
Research InstitutionNational Institutes for Quantum Science and Technology

Principal Investigator

Nakanishi Ryuzo  国立研究開発法人量子科学技術研究開発機構, 高崎量子応用研究所 東海量子ビーム応用研究センター, 主幹研究員 (70447324)

Project Period (FY) 2020-04-01 – 2023-03-31
Project Status Completed (Fiscal Year 2022)
Budget Amount *help
¥4,290,000 (Direct Cost: ¥3,300,000、Indirect Cost: ¥990,000)
Fiscal Year 2022: ¥1,040,000 (Direct Cost: ¥800,000、Indirect Cost: ¥240,000)
Fiscal Year 2021: ¥1,040,000 (Direct Cost: ¥800,000、Indirect Cost: ¥240,000)
Fiscal Year 2020: ¥2,210,000 (Direct Cost: ¥1,700,000、Indirect Cost: ¥510,000)
Keywordsレーザー光還元 / 微粒子化反応 / エネルギー分散型XAFS / 量子化学計算 / 還元微粒子化 / レーザー還元微粒子化 / MRCI計算 / レーザー光還元微粒子化 / Ab initio MRCI / 時間分解分光 / 金属ナノ粒子
Outline of Research at the Start

金属錯イオンを前駆体とするレーザー誘起微粒子化反応では,光照射初期や粒子成長期のイオン還元過程において従来モデルでは説明できない新規な還元反応が進行していることが示唆されている。本研究では,金やパラジウムなどの貴金属イオンを対象に時間分解分光を用いてこの新規な光還元反応を励起状態ダイナミクスの観点から詳細に検討し,レーザー光誘起過程の特徴を素過程レベルで解明するとともに,その発現機構・反応機構を明らかにする。

Outline of Final Research Achievements

Laser-induced particle formation has opened up a unique approach for synthesizing various types of metal particles; pulsed laser irradiation effectively reduces metal ions to neutral atoms and induces the growth of embryonic particles. However, the photochemical reaction mechanism underlying these processes remains unclear. To address this gap, we investigated the kinetics and dynamics of the laser-induced processes involving noble metal ions such as Rh, Pd, and Au by employing time-resolved energy-dispersive XAFS(DXAFS) and quantum chemical calculations. In situ measurements of DXAFS allowed us to trace the electronic and structural changes of metal precursors during the photoreduction. Our results revealed that the new reaction pathways and the reaction intermediates are involved in each reaction system, providing insights into the intricate details of the reaction processes.

Academic Significance and Societal Importance of the Research Achievements

レーザー光誘起微粒子化における金属錯イオンの光還元について実験・理論の両面からその反応機構の解明に取り組み、ロジウム・パラジウム・金が関与する光還元反応について、提唱されていた反応機構を検証するとともに、新たな反応経路を提唱した。金属錯イオンの液相光還元は微粒子合成、金属回収、触媒表面修飾に使われている手法であり、詳細な反応機構研究は新規な微粒子生成法や金属分離・回収法の開発に繋がると期待される。

Report

(4 results)
  • 2022 Annual Research Report   Final Research Report ( PDF )
  • 2021 Research-status Report
  • 2020 Research-status Report
  • Research Products

    (11 results)

All 2023 2022 2021

All Journal Article (4 results) (of which Peer Reviewed: 4 results) Presentation (7 results) (of which Int'l Joint Research: 1 results)

  • [Journal Article] Reaction pathways for palladium(I) reduction in laser-induced particle formation of Pd: An ab initio molecular orbital study2023

    • Author(s)
      Kurosaki Yuzuru、Nakanishi Ryuzo、Saeki Morihisa、Ohba Hironori
    • Journal Title

      Chemical Physics

      Volume: 569 Pages: 111857-111857

    • DOI

      10.1016/j.chemphys.2023.111857

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Dispersive XAFS Study on the Laser-Induced Reduction of a Rh3+ Ion Complex: Presence of a Rh+ Intermediate in Direct Photoreduction2022

    • Author(s)
      Saeki Morihisa、Matsumura Daiju、Nakanishi Ryuzo、Yomogida Takumi、Tsuji Takuya、Saitoh Hiroyuki、Ohba Hironori
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 126 Issue: 12 Pages: 5607-5616

    • DOI

      10.1021/acs.jpcc.1c10160

    • Related Report
      2021 Research-status Report
    • Peer Reviewed
  • [Journal Article] Ab initio study of palladium dichloride PdCl2 and its anion PdCl2-2021

    • Author(s)
      Kurosaki Yuzuru、Nakanishi Ryuzo、Saeki Morihisa、Ohba Hironori
    • Journal Title

      Chemical Physics

      Volume: 551 Pages: 111349-111349

    • DOI

      10.1016/j.chemphys.2021.111349

    • Related Report
      2021 Research-status Report
    • Peer Reviewed
  • [Journal Article] Ab initio MRCI study on potential energy surfaces for double Cl loss from the palladium tetrachloride anion PdCl42-2021

    • Author(s)
      Kurosaki Yuzuru、Nakanishi Ryuzo、Saeki Morihisa、Ohba Hironori
    • Journal Title

      Chemical Physics Letters

      Volume: 764 Pages: 138247-138247

    • DOI

      10.1016/j.cplett.2020.138247

    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Presentation] Sensitive Detection of Alkali and Precious Metals in Aqueous Solutions Using LIBS with Liquid Sheet Jets2022

    • Author(s)
      Nakanishi Ryuzo、Saeki Morihisa、Ohba Hironori
    • Organizer
      SAAMT2022
    • Related Report
      2022 Annual Research Report
  • [Presentation] 水/エタノール混合溶液中Rh3+イオン錯体のレーザー誘起還元反応に関する時間分解XAFS研究2022

    • Author(s)
      佐伯盛久、松村大樹、中西隆造、蓬田匠、辻卓也、齋藤寛之、大場弘則
    • Organizer
      第16回分子科学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] レーザー誘起Pd微粒子生成に関する理論的研究2022

    • Author(s)
      黒崎譲、中西隆造、佐伯盛久、大場弘則
    • Organizer
      第16回分子科学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] DXAFSによるRhIIIイオン錯体のレーザー誘起光還元機構の研究2021

    • Author(s)
      佐伯盛久,松村大樹,中西隆造,蓬田匠,辻卓也,齋藤寛之,大場弘則
    • Organizer
      第24回XAFS討論会
    • Related Report
      2021 Research-status Report
  • [Presentation] In Situ Time-Resolved XAFS Study on Laser-Induced Particle Formation of Pd(II) Ion in a Solution2021

    • Author(s)
      Morihisa Saeki, Daiju Matsumura, Takumi Yomogida, Tomitsugu Taguchi, Takuya Tsuji, Hiroyuki Saito, Ryuzo Nakanishi, Hironori Oba
    • Organizer
      6th International Conference on Advanced Nanoparticle Generation & Excitation by Lasers in Liquids
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research
  • [Presentation] 密度汎関数法による塩化パラジウム錯イオン[PdCl4]2-のCl光解離過程の理論的研究2021

    • Author(s)
      安齋愛子,黒崎譲,中西隆造,佐伯盛久,大場弘則,村岡梓
    • Organizer
      第15回分子科学討論会
    • Related Report
      2021 Research-status Report
  • [Presentation] 第一原理計算を用いた[PdCl4]2-のCl 光解離過程における溶媒効果2021

    • Author(s)
      安齋愛子,黒崎譲,中西隆造,佐伯盛久,大場弘則,村岡梓
    • Organizer
      日本コンピュータ化学会2021年秋季年会
    • Related Report
      2021 Research-status Report

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Published: 2020-04-28   Modified: 2024-01-30  

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