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未利用な太陽光エネルギーを利用する多元量子ドット光触媒の開発

Research Project

Project/Area Number 22H00341
Research Category

Grant-in-Aid for Scientific Research (A)

Allocation TypeSingle-year Grants
Section一般
Review Section Medium-sized Section 36:Inorganic materials chemistry, energy-related chemistry, and related fields
Research InstitutionNagoya University

Principal Investigator

鳥本 司  名古屋大学, 未来社会創造機構(工), 教授 (60271029)

Project Period (FY) 2022-04-01 – 2026-03-31
Project Status Granted (Fiscal Year 2025)
Budget Amount *help
¥42,770,000 (Direct Cost: ¥32,900,000、Indirect Cost: ¥9,870,000)
Fiscal Year 2025: ¥8,190,000 (Direct Cost: ¥6,300,000、Indirect Cost: ¥1,890,000)
Fiscal Year 2024: ¥8,190,000 (Direct Cost: ¥6,300,000、Indirect Cost: ¥1,890,000)
Fiscal Year 2023: ¥8,190,000 (Direct Cost: ¥6,300,000、Indirect Cost: ¥1,890,000)
Fiscal Year 2022: ¥18,200,000 (Direct Cost: ¥14,000,000、Indirect Cost: ¥4,200,000)
Keywords量子ドット / 組成制御 / 多元半導体 / 発光特性 / 光エネルギー変換 / 光触媒 / 近赤外光応答 / 近赤外光 / 水素製造 / 発光 / I-III-VI族半導体 / 異方性結晶成長
Outline of Research at the Start

低次元材料である量子ドットは、極めて大きな比表面積をもつ非平衡材料であり、他の物質との相溶性や非化学量論組成が大幅に拡大するので、材料設計の自由度が大きい。これを利用して本研究課題では、多元半導体(3元素以上)の化学組成・非化学量論性と異種元素のドープ量を精密に制御し、量子ドットの電子構造を自在に制御する。さらに、結晶成長の異方性を発現させて量子ドットの粒子形状・ナノ構造の精密制御法を確立する。これらにより、太陽光を高効率に利用する新規光触媒反応系の構築を目指す。

Outline of Annual Research Achievements

低次元材料である量子ドットは、極めて大きな比表面積をもつ非平衡材料であり、他の物質との相溶性や非化学量論組成が大幅に拡大するので、材料設計の自由度が大きい。現在、高毒性元素を含むCdSe,CdTe,PbSなどの二元半導体量子ドットが主な研究対象となっているが、その利用範囲は厳しく制限されており実用化が困難な材料といえる。そこで本研究課題では、低毒性元素からなる多元半導体(3元素以上)の化学組成・非化学量論性と異種元素のドープ量を精密に制御し、量子ドットの電子構造を自在に制御することを目指す。本年度は、近赤外光領域にバンドギャップ(Eg)をもつ新規多元量子ドットの合成を継続して行うと共に、光電変換特性に及ぼす粒子組成・サイズの影響を評価した。
近赤外領域にバンドギャップを持つ半導体としてAgBiS2を選び、、液相化学合成により粒子サイズと組成の制御を行った。反応温度を100oCから200oCへ上昇させると、量子ドットのサイズが2.6 nmから8.1 nmに増大した。粒子組成は、反応温度の上昇に伴ってAg割合が増大し、150℃以上で合成した量子ドットでは、AgBiS2の化学量論組成に近い値を示した。化学量論組成のAg-Bi-S量子ドットをITO電極上に担持して光電気化学特性を評価したところp型半導体の光応答が得られ、その光電流の立ち上がり電位は価電子帯準位によく一致した。光電流の作用スペクトルを測定から、近赤外光照射によって光電流が生成したことがわかった。一方で、Ag含有率の少ない量子ドットは、バンドギャップ内に光電流の立ち上がり電位を示し、再結合中心となる欠陥サイトがバンドギャップ内に存在することが示唆された。以上のように、粒子内の欠陥準位を精度良く制御することで、効率よく光エネルギー変換できるAg-Bi-S量子ドットが作製できることを明らかにした。

Current Status of Research Progress
Current Status of Research Progress

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

Reason

近赤外光領域にエネルギーギャップを有する金属カルコゲナイド化合物半導体の1つであるAgBiS2を対象として、Ag-B-S量子ドットの液相化学合成に成功し、粒子サイズと組成を高精度に制御することに成功した。さらにAg-B-S量子ドットの電子エネルギー構造が化学組成により大きく変化することを解明し、量子ドットの光エネルギー変換特性に大きな影響を及ぼす欠陥準位の存在とそのエネルギーレベルを見積もることに成功した。
これらの成果は、当初の計画に予定していたものであり、「おおむね順調に進展している」と評価した。

Strategy for Future Research Activity

前年度までに行った低毒性多元量子ドットの精密液相合成法の開発と、サイズ・形状制御による電子エネルギー構造の制御を引き続き行うとともに、その光触媒活性を評価し、量子ドット光触媒の作製と高活性化のための設計指針を得る。

Report

(3 results)
  • 2023 Annual Research Report
  • 2022 Comments on the Screening Results   Annual Research Report
  • Research Products

    (25 results)

All 2024 2023 2022

All Journal Article (15 results) (of which Int'l Joint Research: 1 results,  Peer Reviewed: 15 results,  Open Access: 6 results) Presentation (10 results) (of which Int'l Joint Research: 6 results,  Invited: 4 results)

  • [Journal Article] Photosensitization of TiO2 electrodes immobilized with chiral plasmonic Au nanocolloids by circularly polarized light irradiation2024

    • Author(s)
      Kameyama Tatsuya、Isogawa Shuji、Akiyoshi Kazutaka、Kashida Hiromu、Asanuma Hiroyuki、Torimoto Tsukasa
    • Journal Title

      The Journal of Chemical Physics

      Volume: 160 Issue: 9 Pages: 094709-094709

    • DOI

      10.1063/5.0192366

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Spectrally Narrow Band-edge Photoluminescence from AgInS2-based Core/shell Quantum Dots for Electroluminescence Applications2024

    • Author(s)
      Uematsu Taro, Izumi Ryunosuke, Sugano Shoki, Sugano Riku, Hirano Tatsuya, Motomura Genichi, Torimoto Tsukasa, Kuwabata Susumu
    • Journal Title

      Faraday Discussions

      Volume: 250 Pages: 281-297

    • DOI

      10.1039/d3fd00142c

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Photoluminescence Redshift of AgInS<sub>2</sub> Quantum Dots by Employing Shells with Graded Composition2023

    • Author(s)
      Navapat Krobkrong, Taro Uematsu, Tsukasa Torimoto, Susumu Kuwabata
    • Journal Title

      Electrochemistry

      Volume: 91 Issue: 10 Pages: 107001-107001

    • DOI

      10.5796/electrochemistry.23-00084

    • ISSN
      1344-3542, 2186-2451
    • Year and Date
      2023-10-31
    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Size- and Shape-Dependent Separation of Multinary Quantum Dots with Plasmonic Thin-Layer Chromatography2023

    • Author(s)
      Akiyoshi Kazutaka、Maeda Yui、Yamaguchi Naoko、Kameyama Tatsuya、Tsuboi Yasuyuki、Yamane Hidemasa、Ishihara Hajime、Torimoto Tsukasa
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 128 Issue: 2 Pages: 908-918

    • DOI

      10.1021/acs.jpcc.3c06531

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Bright Red Luminescence from Ag-In-Ga-S-Based Quantum Dots with the Introduction of Copper2023

    • Author(s)
      Uematsu Taro, Krobkrong Navapat, Asai Kenichiro, Motomura Genichi, Fujisaki Yoshihide, Torimoto Tsukasa, Kuwabata Susumu
    • Journal Title

      Bulletin of the Chemical Society of Japan

      Volume: 96 Issue: 11 Pages: 1274-1282

    • DOI

      10.1246/bcsj.20230216

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] One-pot synthesis of Ag-In-Ga-S nanocrystals embedded in a Ga2O3 matrix and enhancement of band-edge emission by Na+ doping2023

    • Author(s)
      Tozawa Makoto、Miyamae Chie、Akiyoshi Kazutaka、Kameyama Tatsuya、Yamamoto Takahisa、Motomura Genichi、Fujisaki Yoshihide、Uematsu Taro、Kuwabata Susumu、Torimoto Tsukasa
    • Journal Title

      Nanoscale Advances

      Volume: 5 Issue: 24 Pages: 7057-7066

    • DOI

      10.1039/d3na00755c

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Promoting Oxygen Reduction Reaction by Excitation of Localized Surface Plasmon of Shape- and Facet-Controlled Octahedral Au@Pt Core-Shell Nanocrystals2023

    • Author(s)
      Tatsuya Kameyama, Kentaro Sato, Takahisa Yamamoto, Mamoru Tamura, Takuya Iida, Tatsuya Shoji, Yasuyuki Tsuboi, Tsukasa Torimoto
    • Journal Title

      ChemElectroChem

      Volume: 10 Issue: 17

    • DOI

      10.1002/celc.202300182

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Development of Cu-In-Ga-S quantum dots with a narrow emission peak for red electroluminescence2023

    • Author(s)
      Jiang Chang、Tozawa Makoto、Akiyoshi Kazutaka、Kameyama Tatsuya、Yamamoto Takahisa、Motomura Genichi、Fujisaki Yoshihide、Uematsu Taro、Kuwabata Susumu、Torimoto Tsukasa
    • Journal Title

      The Journal of Chemical Physics

      Volume: 158 Issue: 16 Pages: 164708-164708

    • DOI

      10.1063/5.0144271

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Facile High-Yield Synthesis of Ag-In-Ga-S Quaternary Quantum Dots and Coating with Gallium Sulfide Shells for Narrow Band-Edge Emission2023

    • Author(s)
      Taro Uematsu, Manunya Tepakidareekul, Tatsuya Hirano, Tsukasa Torimoto, and Susumu Kuwabata
    • Journal Title

      Chemistry of Materials

      Volume: 35 Issue: 3 Pages: 1094-1106

    • DOI

      10.1021/acs.chemmater.2c03023

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Controlling optical properties and electronic energy structure of I-III-VI semiconductor quantum dots for improving their photofunctions2023

    • Author(s)
      Tsukasa Torimoto, Tatsuya Kameyama, Taro Uematsu, and Ssusumu Kuwabata
    • Journal Title

      Journal of Photochemistry and Photobiology C: Photochemistry Reviews

      Volume: 54 Pages: 100569-100569

    • DOI

      10.1016/j.jphotochemrev.2022.100569

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Electrocatalyst Fabrication Using Metal Nanoparticles Prepared in Ionic Liquids2023

    • Author(s)
      Yu Yao, Tetsuya Tsuda, Tsukasa Torimoto, and Susumu Kuwabata
    • Journal Title

      The Chemical Record

      Volume: 23 Issue: 8

    • DOI

      10.1002/tcr.202200274

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Encapsulation of AgInS2/GaSx core/shell quantum dots in In-fumarate metal-organic frameworks for stability enhancement2022

    • Author(s)
      Tepakidareekul Manunya、Uematsu Taro、Torimoto Tsukasa、Kuwabata Susumu
    • Journal Title

      CrystEngComm

      Volume: - Issue: 20 Pages: 3715-3723

    • DOI

      10.1039/d2ce00343k

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Development of plasmonic thin-layer chromatography for size-selective and optical-property-dependent separation of quantum dots2022

    • Author(s)
      Torimoto Tsukasa、Yamaguchi Naoko、Maeda Yui、Akiyoshi Kazutaka、Kameyama Tatsuya、Nagai Tatsuya、Shoji Tatsuya、Yamane Hidemasa、Ishihara Hajime、Tsuboi Yasuyuki
    • Journal Title

      NPG Asia Materials

      Volume: 14 Issue: 1 Pages: 64-76

    • DOI

      10.1038/s41427-022-00414-3

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Direct Detection of Long-Range Interdomain Auger Recombination in Dumbbell-Shaped Quasi-Type-II Nanoparticle2022

    • Author(s)
      Masafumi Koga, Ko Masuoka, Shuhei Tsuneizumi, Tatsuya Kameyama, Syoji Ito, Tsukasa Torimoto, and Hiroshi Miyasaka
    • Journal Title

      J Phys. Chem. Lett.

      Volume: 13 Issue: 29 Pages: 6845-6851

    • DOI

      10.1021/acs.jpclett.2c01077

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Composition control of alloy nanoparticles consisting of bulk-immiscible Au and Rh metals via an ionic liquid/metal sputtering technique for improving their electrocatalytic activity2022

    • Author(s)
      Kazutaka Akiyoshi, Yumezo Watanabe, Tatsuya Kameyama, Tokuhisa Kawawaki, Yuichi Negishi, Susumu Kuwabata and Tsukasa Torimoto
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 24 Issue: 39 Pages: 24335-24344

    • DOI

      10.1039/d2cp01461k

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Presentation] 多元半導体量子ドットの液相合成と光機能開発2023

    • Author(s)
      鳥本 司
    • Organizer
      アトムハイブリッドシンポジウム
    • Related Report
      2023 Annual Research Report
    • Invited
  • [Presentation] Tunable Optical Properties of Less-toxic Multinary Quantum Dots Composed of Ag-In-Ga-S Alloys and Related Compounds2023

    • Author(s)
      Tsukasa Torimoto, Tatsuya Kameyama, Taro Uematsu, Susumu Kuwabata
    • Organizer
      The 31th International Conference on Photochemistry 2023 (ICP2023)
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Photoluminescence Property of Cu(In,Ga)S2 Quantum Dots Depending on Their Composition and -Nanostucture2023

    • Author(s)
      T. Torimoto, C. Jiang, T. Kameyama, T. Uematsu, S. Kuwabata
    • Organizer
      243rd ECS Meeting
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Colloidal Synthesis and Photoluminescence Property of Near-IR-Responsive Ag8GeS6 Quantum Dots2023

    • Author(s)
      N. Rismaningsih, J. Kubo, N. Fujihira, T. Kameyama, T. Torimoto
    • Organizer
      243rd ECS Meeting
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Dependence of Photoelectrochemical Properties of AgBiS2 Quantum Dots on Their Size and Composition2023

    • Author(s)
      Wentao Zhang, Kazutaka Akiyoshi, Tatsuya Kameyama, Tsukasa Torimoto
    • Organizer
      The 31th International Conference on Photochemistry 2023 (ICP2023)
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 光エネルギー変換材料への応用を目指したBi系カルコハライド半導体ナノ結晶の合成とその光化学特性制御2023

    • Author(s)
      春日 夢乃, 秋吉 一孝, 亀山 達矢, 鳥本 司
    • Organizer
      2023年電気化学秋季大会
    • Related Report
      2023 Annual Research Report
  • [Presentation] 異方形状をもつI-III-VI族半導体ナノ結晶の合成と水素生成光触媒活性2023

    • Author(s)
      住友 竜司, 秋吉 一孝, 亀山 達矢, 鳥本 司
    • Organizer
      2023年電気化学秋季大会
    • Related Report
      2023 Annual Research Report
  • [Presentation] 近赤外光応答するAg-Cu-In-Teナノロッドのサイズ制御とその光化学特性2023

    • Author(s)
      久保田 翔, 武藤 千聖, 亀山 達矢, 桑畑 進, 鳥本 司
    • Organizer
      2023年光化学討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Preparation of Group I-III-VI-based Quantum Dots with Less Toxicity and Their Photofunctions2022

    • Author(s)
      Tsukasa Torimoto
    • Organizer
      INSPINSA2022 (The 12th International Seminar on New Paradigm and Innovation on Natural Sciences and its Application)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Controlling the Energy Structure of Ag(In,Ga)S Quantum Dots for Photocatalytic H2 Evolution2022

    • Author(s)
      T. Torimoto, T. Mori, T. Kameyama, T. Uematsu and S. Kuwabata
    • Organizer
      241st ECS Meeting
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited

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Published: 2022-04-19   Modified: 2025-06-20  

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