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ハイエントロピー固溶ナノ合金の創製と新機能探索

Publicly Offered Research

Project AreaHigh Entropy Alloys - Science of New Class of Materials Based on Elemental Multiplicity and Heterogeneity
Project/Area Number 19H05170
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 InstitutionKyoto University

Principal Investigator

北川 宏  京都大学, 理学研究科, 教授 (90234244)

Project Period (FY) 2019-04-01 – 2021-03-31
Project Status Discontinued (Fiscal Year 2020)
Budget Amount *help
¥9,490,000 (Direct Cost: ¥7,300,000、Indirect Cost: ¥2,190,000)
Fiscal Year 2020: ¥5,200,000 (Direct Cost: ¥4,000,000、Indirect Cost: ¥1,200,000)
Fiscal Year 2019: ¥4,290,000 (Direct Cost: ¥3,300,000、Indirect Cost: ¥990,000)
Keywordsハイエントロピー / ナノ合金 / 多元素 / 触媒 / 貴金属 / ナノ固溶合金 / 多元素工エントロピー / ナノ材料 / 多元素高エントロピー
Outline of Research at the Start

本研究では、主にバルク状態では相分離する金属元素の組み合わせを多元素高エントロピー効果により原子レベルで固溶化させることで、多くの新しいナノ物質を創製すると共に、革新的なナノ材料の開発を行う。研究代表者は、2010 年に、元素周期律表上でパラジウムの両隣に位置する銀とロジウムを原子レベルで固溶させることに世界で初めて成功し、Ag-Rh 固溶合金がパラジウムと類似の性質を有することを見出した。謂わば「現代の錬金術」とも言える成果であり、「人工パラジウム」「擬パラジウム」として世界中で広く報道された。

Outline of Annual Research Achievements

令和元年度には、化学還元法を用いて、5元、6元系ハイエントロピー合金の合成に成功しており、本年度は8元系貴金属固溶ナノ合金の合成に取り組んだ。また、昨年度、電極触媒として高い活性を示すことが分かった5元系および6元系ハイエントロピーナノ合金における触媒機構をX線光電子分光を始めとした各種分析を行うことで考察した。
液相還元法により貴金属全8元素から構成されるRuRhPdAgOSIrPtAuナノ合金の合成に成功し、これらを任意の金属組成で合成することが可能となった。また、ソルボサーマル連続フロー合成装置を用いて、昨年度バッチ合成で得られていた5元系RuRhPdIrPtナノ合金の合成にも成功した。また、昨年度電極触媒として物性評価を行ったところ、5元系合金は燃料電池の半反応である水素発生反応(HER)において、酸性およびアルカリ性の両条件において高い活性を示し、それはベンチマークであるPt触媒より高活性を示すことが分かっていた。HERは反応基質である水素原子の吸着エネルギーが触媒金属のdバンドの重心と線形的な相関があるため、dバンド重心によりその活性が予想できることが知られている。そこで、放射光を用いた硬X線光電子分光法により、合成したナノ合金および単金属ナノ粒子の価電子帯の直接観察を行い、そのd-バンド重心と触媒活性の比較を行ったところ、酸性およびアルカリ性溶液共に、RuRhPdIrPtナノ合金触媒は単金属のd-バンド重心理論に従わない極めて高い触媒活性を示すことが分かった。これは、これまでd-バンド重心理論が単純な金属表面をモデルとした水素吸着エネルギーから構成されている点が相違を生んでいる可能性や、開発したHEAがこれまでとは異なる反応機構を示している可能性を示唆した。その他の成果として、排ガス浄化触媒用途や水電解触媒に関する論文などを公表した。

Research Progress Status

令和2年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

令和2年度が最終年度であるため、記入しない。

Report

(2 results)
  • 2020 Annual Research Report
  • 2019 Annual Research Report
  • Research Products

    (35 results)

All 2021 2020 2019

All Journal Article (19 results) (of which Int'l Joint Research: 5 results,  Peer Reviewed: 19 results,  Open Access: 4 results) Presentation (12 results) (of which Int'l Joint Research: 7 results,  Invited: 11 results) Patent(Industrial Property Rights) (4 results)

  • [Journal Article] Highly Stable and Active Solid‐Solution‐Alloy Three‐Way Catalyst by Utilizing Configurational‐Entropy Effect2021

    • Author(s)
      Kusada Kohei, Wu Dongshuang, Nanba Yusuke, Koyama Michihisa, Yamamoto Tomokazu, Tran Xuan Quy, Toriyama Takaaki, Matsumura Syo, Ito Ayano, Sato Katsutoshi, Nagaoka Katsutoshi, Seo Okkyun, Song Chulho, Chen Yanna, Palina Natalia, Kumara Loku Singgappulige Rosantha, Hiroi Satoshi, Sakata Osami, Kitagawa Hiroshi et al.
    • Journal Title

      Advanced Materials

      Volume: in press Issue: 16 Pages: 2005206-2005206

    • DOI

      10.1002/adma.202005206

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Efficient overall water splitting in acid with anisotropic metal nanosheets2021

    • Author(s)
      Wu Dongshuang、Kusada Kohei、Yoshioka Satoru、Yamamoto Tomokazu、Toriyama Takaaki、Matsumura Syo、Chen Yanna、Seo Okkyun、Kim Jaemyung、Song Chulho、Hiroi Satoshi、Sakata Osami、Ina Toshiaki、Kawaguchi Shogo、Kubota Yoshiki、Kobayashi Hirokazu、Kitagawa Hiroshi
    • Journal Title

      Nature Communications

      Volume: 12 Issue: 1 Pages: 1145-1145

    • DOI

      10.1038/s41467-021-20956-4

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] First synthesis of air-stable NiZn homogeneous alloy nanoparticles through chemical reduction2021

    • Author(s)
      Okamoto Shinya、Kusada Kohei、Hashiba Hiroshi、Yotsuhashi Satoshi、Kitagawa Hiroshi
    • Journal Title

      Materials Advances

      Volume: 2 Issue: 2 Pages: 684-687

    • DOI

      10.1039/d0ma00883d

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Nonequilibrium Flow-Synthesis of Solid-Solution Alloy Nanoparticles: From Immiscible Binary to High-Entropy Alloys2020

    • Author(s)
      Kusada Kohei、Yamamoto Tomokazu、Toriyama Takaaki、Matsumura Syo、Sato Katsutoshi、Nagaoka Katsutoshi、Terada Kenji、Ikeda Yasuyuki、Hirai Yoshinari、Kitagawa Hiroshi
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 125 Issue: 1 Pages: 458-463

    • DOI

      10.1021/acs.jpcc.0c08871

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Platinum-Group-Metal High-Entropy-Alloy Nanoparticles2020

    • Author(s)
      Wu Dongshuang、Kusada Kohei、Yamamoto Tomokazu、Toriyama Takaaki、Matsumura Syo、Kawaguchi Shogo、Kubota Yoshiki、Kitagawa Hiroshi
    • Journal Title

      Journal of the American Chemical Society

      Volume: 142 Issue: 32 Pages: 13833-13838

    • DOI

      10.1021/jacs.0c04807

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Significant Enhancement of Hydrogen Evolution Reaction Activity by Negatively Charged Pt through Light Doping of W2020

    • Author(s)
      Kobayashi Daiya、Kobayashi Hirokazu、Wu Dongshuang、Okazoe Shinya、Kusada Kohei、Yamamoto Tomokazu、Toriyama Takaaki、Matsumura Syo、Kawaguchi Shogo、Kubota Yoshiki、Aspera Susan Me?ez、Nakanishi Hiroshi、Arai Shigebumi、Kitagawa Hiroshi
    • Journal Title

      Journal of the American Chemical Society

      Volume: 142 Issue: 41 Pages: 17250-17254

    • DOI

      10.1021/jacs.0c07143

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Coreduction methodology for immiscible alloys of CuRu solid-solution nanoparticles with high thermal stability and versatile exhaust purification ability2020

    • Author(s)
      Huang Bo、Kobayashi Hirokazu、Yamamoto Tomokazu、Matsumura Syo、Nishida Yoshihide、Sato Katsutoshi、Nagaoka Katsutoshi、Haneda Masaaki、Kawaguchi Shogo、Kubota Yoshiki、Kitagawa Hiroshi
    • Journal Title

      Chemical Science

      Volume: 11 Issue: 42 Pages: 11413-11418

    • DOI

      10.1039/d0sc03373a

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] On the electronic structure and hydrogen evolution reaction activity of platinum group metal-based high-entropy-alloy nanoparticles2020

    • Author(s)
      Wu Dongshuang、Kusada Kohei、Yamamoto Tomokazu、Toriyama Takaaki、Matsumura Syo、Gueye Ibrahima、Seo Okkyun、Kim Jaemyung、Hiroi Satoshi、Sakata Osami、Kawaguchi Shogo、Kubota Yoshiki、Kitagawa Hiroshi
    • Journal Title

      Chemical Science

      Volume: 11 Issue: 47 Pages: 12731-12736

    • DOI

      10.1039/d0sc02351e

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] NMR-based gap behavior related to the quantum size effect2020

    • Author(s)
      Okuno Tomonori、Manago Masahiro、Kitagawa Shunsaku、Ishida Kenji、Kusada Kohei、Kitagawa Hiroshi
    • Journal Title

      Physical Review B

      Volume: 101 Issue: 12 Pages: 121406-121406

    • DOI

      10.1103/physrevb.101.121406

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Synthesis of Mo and Ru solid-solution alloy NPs and their hydrogen evolution reaction activity2020

    • Author(s)
      Okazoe Shinya、Kusada Kohei、Wu Dongshuang、Yamamoto Tomokazu、Toriyama Takaaki、Matsumura Syo、Kawaguchi Shogo、Kubota Yoshiki、Kitagawa Hiroshi
    • Journal Title

      Chemical Communications

      Volume: 56 Issue: 92 Pages: 14475-14478

    • DOI

      10.1039/d0cc05958g

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Crystalline to amorphous transformation in solid-solution alloy nanoparticles induced by boron doping2020

    • Author(s)
      Kobayashi Keigo、Kusada Kohei、Wu Dongshuang、Ogiwara Naoki、Kobayashi Hirokazu、Haruta Mitsutaka、Kurata Hiroki、Hiroi Satoshi、Seo Okkyun、Song Chulho、Chen Yanna、Kim Jaemyung、Tayal Akhil、Sakata Osami、Ohara Koji、Honma Tetsuo、Kitagawa Hiroshi
    • Journal Title

      Chemical Communications

      Volume: 56 Issue: 85 Pages: 12941-12944

    • DOI

      10.1039/d0cc05418f

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] New Insights on the Formation Process and Thermodynamics of the α-Phase PdH(D)x through Direct Enthalpy Measurement of H(D) Dissolution2020

    • Author(s)
      Dekura Shun、Akiba Hiroshi、Yamamuro Osamu、Kobayashi Hirokazu、Maesato Mitsuhiko、Kitagawa Hiroshi
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 124 Issue: 16 Pages: 8663-8668

    • DOI

      10.1021/acs.jpcc.0c01817

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Magnetic-Field Dependence of Novel Gap Behavior Related to the Quantum-Size Effect2020

    • Author(s)
      Okuno Tomonori、Kinoshita Yuta、Matsuzaki Satoshi、Kitagawa Shunsaku、Ishida Kenji、Hirata Michihiro、Sasaki Takahiko、Kusada Kohei、Kitagawa Hiroshi
    • Journal Title

      Journal of the Physical Society of Japan

      Volume: 89 Issue: 9 Pages: 095002-095002

    • DOI

      10.7566/jpsj.89.095002

    • NAID

      210000158416

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Statistical Evaluation of the Solid-Solution State in Ternary Nanoalloys2020

    • Author(s)
      Tran Xuan Quy、Kono Yoshiki、Yamamoto Tomokazu、Kusada Kohei、Kitagawa Hiroshi、Matsumura Syo
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 124 Issue: 39 Pages: 21843-21852

    • DOI

      10.1021/acs.jpcc.0c06813

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Chemoselective hydrogenation of heteroarenes and arenes by Pd?Ru?PVP under mild conditions2020

    • Author(s)
      Chaudhari Chandan、Sato Katsutoshi、Nishida Yoshihide、Yamamoto Tomokazu、Toriyama Takaaki、Matsumura Syo、Ikeda Yasuyuki、Terada Kenji、Abe Naoya、Kusuda Kohei、Kitagawa Hiroshi、Nagaoka Katsutoshi
    • Journal Title

      RSC Advances

      Volume: 10 Issue: 72 Pages: 44191-44195

    • DOI

      10.1039/d0ra09981c

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Rational Synthesis for a Noble Metal Carbide2019

    • Author(s)
      W. Takuo, K. Kohei, W. Dongshuang, Y. Tomokazu, T. Takaaki, M. Syo, A. Hiroshi, Y. Osamu, I. Kazutaka, O. Toshiya, P. Natalia, C. Yanna, K. Loku S. R., S. Chulho, S. Osami, X. Wei, K. Michihisa, K. Yoshiki, K. Shogo, A. Ryan L., A. Susan M., A. Elvis F., N. Hiroshi, K. Hiroshi
    • Journal Title

      Journal of the American Chemical Society

      Volume: 142 Issue: 3 Pages: 1247-1253

    • DOI

      10.1021/jacs.9b09219

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Solid-solution alloy nanoparticles of a combination of immiscible Au and Ru with a large gap of reduction potential and their enhanced oxygen evolution reaction performance2019

    • Author(s)
      Quan Zhang, Kohei Kusada, Dongshuang Wu, Naoki Ogiwara, Tomokazu Yamamoto, Takaaki Toriyama, Syo Matsumura, Shogo Kawaguchi, Yoshiki Kubota, Tetsuo Honma, Hiroshi Kitagawa
    • Journal Title

      Chemical Science

      Volume: 印刷中 Issue: 19 Pages: 5133-5137

    • DOI

      10.1039/c9sc00496c

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Observation of the Formation Processes of Hexagonal Close-packed and Face-centered Cubic Ru Nanoparticles2019

    • Author(s)
      Araki Naoki、Kusada Kohei、Yoshioka Satoru、Sugiyama Takeharu、Ina Toshiaki、Kitagawa Hiroshi
    • Journal Title

      Chemistry Letters

      Volume: 48 Issue: 9 Pages: 1062-1064

    • DOI

      10.1246/cl.190338

    • NAID

      130007703009

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] A Novel Platinum(III)?Platinum(III) Neutral Dimer Complex, Pt2(cdtb)4I2 (cdtb: 4-Cyanodithiobenzoate)2019

    • Author(s)
      Moriyama Hayato、Otsubo Kazuya、Aoki Kentaro、Maesato Mitsuhiko、Sugimoto Kunihisa、Kitagawa Hiroshi
    • Journal Title

      Chemistry Letters

      Volume: 48 Issue: 9 Pages: 1035-1037

    • DOI

      10.1246/cl.190355

    • NAID

      130007703014

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Presentation] Conductive Coordination Networks2021

    • Author(s)
      H. Kitagawa
    • Organizer
      International Conference on Advances in Molecular Materials Research
    • Related Report
      2020 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] ナノ合金技術が切り開く未来2021

    • Author(s)
      北川 宏
    • Organizer
      SMBCオンラインセミナー,
    • Related Report
      2020 Annual Research Report
    • Invited
  • [Presentation] Platinum-group-metal high-entropy-alloy nanoparticles for electrocatalysis2020

    • Author(s)
      D. Wu, K. Kusada and H. Kitagawa
    • Organizer
      High Entropy Alloy and Complex Solid Solution Nanoparticles for Electrocatalysis
    • Related Report
      2020 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 非平衡合成による多元素ナノ合金の創製2020

    • Author(s)
      北川 宏
    • Organizer
      革新的触媒と反応制御の今後, JST・触媒学会共催オンライン公開シンポジウム
    • Related Report
      2020 Annual Research Report
    • Invited
  • [Presentation] 非非平衡合成法による多元素ナノ合金粒子の作製と応用2020

    • Author(s)
      北川 宏
    • Organizer
      多様な安定相のエンジニアリングの新展開, 応用物理学会秋季学術講演会シンポジウム
    • Related Report
      2020 Annual Research Report
    • Invited
  • [Presentation] 現代の錬金術:ハイエントロピー効果による革新的ナノ材料の創出2020

    • Author(s)
      北川 宏
    • Organizer
      科学技術展望懇談会
    • Related Report
      2020 Annual Research Report
    • Invited
  • [Presentation] DOS Engineering for New Nano-Materials: Binary to High-Entropy Alloys2020

    • Author(s)
      北川 宏
    • Organizer
      87th CEMS Colloquium
    • Related Report
      2020 Annual Research Report
    • Invited
  • [Presentation] Density-of-States Engineering For New Nano-Materials2020

    • Author(s)
      北川宏
    • Organizer
      IISER TVM Frontier Symposium in Chemistry 2020 (FS-CHM 2020)
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Conductiv Coordination Networkについて2019

    • Author(s)
      北川宏
    • Organizer
      UNIST 2019 Sspring Seminar
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] DOS Engineering for New Green Nano-materials2019

    • Author(s)
      北川宏
    • Organizer
      鄭州大学国際サマースクール
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Conductive Coordination Networks2019

    • Author(s)
      北川宏
    • Organizer
      7TH ASIAN CONFERENCE ON COORDINATION CHEMISTRY ACCC72019
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Solid -state protonic in Coordination Polymers2019

    • Author(s)
      北川宏
    • Organizer
      2019 International Conference on Advanced Fibers and Polymer Materials
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Patent(Industrial Property Rights)] 担持触媒2020

    • Inventor(s)
      草田康平、北川宏、池田泰之、丸子智弘、竹内正史
    • Industrial Property Rights Holder
      草田康平、北川宏、池田泰之、丸子智弘、竹内正史
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      2020-035420
    • Filing Date
      2020
    • Related Report
      2020 Annual Research Report
  • [Patent(Industrial Property Rights)] 合金、合金ナノ粒子の集合体および触媒2020

    • Inventor(s)
      北川宏、草田康平、松村晶、山本知一、Tran Xuan Quy
    • Industrial Property Rights Holder
      北川宏、草田康平、松村晶、山本知一、Tran Xuan Quy
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      2020-116140
    • Filing Date
      2020
    • Related Report
      2020 Annual Research Report
  • [Patent(Industrial Property Rights)] 合金、合金ナノ粒子の集合体および触媒2020

    • Inventor(s)
      北川宏、小林浩和、洞江祐貴、草田康平、松村晶ra
    • Industrial Property Rights Holder
      北川宏、小林浩和、洞江祐貴、草田康平、松村晶ra
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      2020-116142
    • Filing Date
      2020
    • Related Report
      2020 Annual Research Report
  • [Patent(Industrial Property Rights)] 合金ナノ粒子、合金ナノ粒子の集合体、触媒および合金ナノ粒子の製 造方法2020

    • Inventor(s)
      北川宏、草田康平、Wu Dongshuang
    • Industrial Property Rights Holder
      北川宏、草田康平、Wu Dongshuang
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      2020-116149
    • Filing Date
      2020
    • Related Report
      2020 Annual Research Report

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Published: 2019-04-18   Modified: 2021-12-27  

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