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Development of metal-modified covalent organic frameworks as selective photocatalysts

Research Project

Project/Area Number 17H04798
Research Category

Grant-in-Aid for Young Scientists (A)

Allocation TypeSingle-year Grants
Research Field Nanomaterials chemistry
Research InstitutionOsaka University

Principal Investigator

Kamiya Kazuhide  大阪大学, 太陽エネルギー化学研究センター, 准教授 (50716016)

Project Period (FY) 2017-04-01 – 2020-03-31
Project Status Completed (Fiscal Year 2019)
Budget Amount *help
¥25,480,000 (Direct Cost: ¥19,600,000、Indirect Cost: ¥5,880,000)
Fiscal Year 2019: ¥4,810,000 (Direct Cost: ¥3,700,000、Indirect Cost: ¥1,110,000)
Fiscal Year 2018: ¥7,150,000 (Direct Cost: ¥5,500,000、Indirect Cost: ¥1,650,000)
Fiscal Year 2017: ¥13,520,000 (Direct Cost: ¥10,400,000、Indirect Cost: ¥3,120,000)
Keywords電子移動触媒 / 光触媒 / 共有結合性有機構造体 / ナノ材料 / 単一原子触媒 / 半導体 / 電極触媒 / 光-化学エネルギー変換 / 電気化学 / 部分酸化 / 光電気化学
Outline of Final Research Achievements

In the present work, we attempted to develop (photo)electrocatalysts for selective oxidative upgrading of organics, which are composed of metal-modified covalent triazine frameworks (M-CTF). The specific achievements are as follows.
(1) A single Ru atom-modified covalent triazine framework (Ru-CTF) has selectivity for the electrooxidation of benzyl alcohol in water over the oxygen evolution reaction.
(2) The Cu-CTF/TiO2 hybrid photocatalytically reduced HNO2 without an external bias under artificial and natural sunlight. The dominant reaction product changes from N2O to NH4+ with an increase in the light intensity due to the shift of operating potentials.

Academic Significance and Societal Importance of the Research Achievements

本研究では水溶液系での有機物電気化学酸化反応において、競合反応である水および触媒自身の酸化をほぼ完全に抑えることに成功した。これはM-CTF触媒がガス状炭化水素の電気化学酸化アップグレーディングなどのより有用性の高い反応へ展開できることに一定の目途がついたことを意味する。
さらに、本研究で実証した光強度およびそれに伴う作動電位の変調が光反応の選択性に及ぼす影響は、高効率な人工光合成系の構築において、必要不可欠な設計指針の一つになると考えられる。

Report

(4 results)
  • 2019 Annual Research Report   Final Research Report ( PDF )
  • 2018 Annual Research Report
  • 2017 Annual Research Report
  • Research Products

    (52 results)

All 2020 2019 2018 2017 Other

All Journal Article (13 results) (of which Peer Reviewed: 11 results,  Open Access: 3 results) Presentation (35 results) (of which Int'l Joint Research: 10 results,  Invited: 11 results) Remarks (4 results)

  • [Journal Article] Rational Molecular Design of Electrocatalysts Based on Single-Atom Modified Covalent Organic Frameworks for Efficient Oxygen Reduction Reaction2020

    • Author(s)
      Iwase Kazuyuki、Nakanishi Shuji、Miyayama Masaru、Kamiya Kazuhide
    • Journal Title

      ACS Applied Energy Materials

      Volume: 3 Issue: 2 Pages: 1644-1652

    • DOI

      10.1021/acsaem.9b02141

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Glycerol Oxidation Catalyzed by High-valency Ruthenium Species at Electrochemical Interfaces2020

    • Author(s)
      Tabata Hiro、Kato Shintaro、Yamaguchi Shingi、Harada Takashi、Iwase Kazuyuki、Kamiya Kazuhide、Nakanishi Shuji
    • Journal Title

      Chemistry Letters

      Volume: 49 Issue: 5 Pages: 513-516

    • DOI

      10.1246/cl.200056

    • NAID

      130007840190

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Electrochemical CO2 reduction using gas diffusion electrode loading Ni-doped covalent triazine frameworks in acidic electrolytes2020

    • Author(s)
      Yuxin Wu、 Kazuhide Kamiya、 Takuya Hashimoto、 Rino Sugimoto、Takashi Harada、Katsushi Fujii、Shuji Nakanishi
    • Journal Title

      Electrochemistry

      Volume: -

    • NAID

      130007896986

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Light intensity responsive changes of products in photocatalytic reduction of nitrous acid on a Cu‐doped covalent triazine framework/TiO2 hybrid2020

    • Author(s)
      Kamiya Kazuhide、Sugimoto Rino、Tatebe Tomomi、Harada Takashi、Nakanishi Shuji
    • Journal Title

      ChemSusChem

      Volume: - Issue: 13 Pages: 3462-3468

    • DOI

      10.1002/cssc.202000687

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 共有結合性有機構造体の細孔内への単一金属原子ドープとその電極触媒能2020

    • Author(s)
      神谷和秀
    • Journal Title

      化学工業

      Volume: 71 Pages: 160-166

    • Related Report
      2019 Annual Research Report
  • [Journal Article] Electrochemical Formation of Fe(IV)=O Derived from H 2 O 2 on a Hematite Electrode as an Active Catalytic Site for Selective Hydrocarbon Oxidation Reactions2019

    • Author(s)
      Kamiya Kazuhide、Kuwabara Akito、Harada Takashi、Nakanishi Shuji
    • Journal Title

      ChemPhysChem

      Volume: 20 Issue: 5 Pages: 648-650

    • DOI

      10.1002/cphc.201801207

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Photo-induced direct interfacial charge transfer at TiO2 modified with hexacyanoferrate(iii)2018

    • Author(s)
      Tatebe Tomomi、Harada Takashi、Kamiya Kazuhide、Nakanishi Shuji
    • Journal Title

      Photochemical & Photobiological Sciences

      Volume: 17 Issue: 9 Pages: 1153-1156

    • DOI

      10.1039/c8pp00237a

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Covalent triazine framework modified with coordinatively-unsaturated Co or Ni atoms for CO2 electrochemical reduction2018

    • Author(s)
      Su Panan、Iwase Kazuyuki、Harada Takashi、Kamiya Kazuhide、Nakanishi Shuji
    • Journal Title

      Chemical Science

      Volume: - Issue: 16 Pages: 3941-3947

    • DOI

      10.1039/c8sc00604k

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Covalent organic frameworks (COFs) to create new catalytic materials2018

    • Author(s)
      Kamiya Kazuhide
    • Journal Title

      Impact

      Volume: 2018 Issue: 11 Pages: 57-59

    • DOI

      10.21820/23987073.2018.11.57

    • Related Report
      2018 Annual Research Report
    • Open Access
  • [Journal Article] Sulfur-Linked Covalent Triazine Frameworks Doped with Coordinatively Unsaturated Cu(I) as Electrocatalysts for Oxygen Reduction2018

    • Author(s)
      Iwase Kazuyuki、Kamiya Kazuhide、Miyayama Masaru、Hashimoto Kazuhito、Nakanishi Shuji
    • Journal Title

      ChemElectroChem

      Volume: 5 Issue: 5 Pages: 805-810

    • DOI

      10.1002/celc.201701361

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Cooperative Electrocatalytic Reduction of Nitrobenzene to Aniline in Aqueous Solution by Copper-modified Covalent Triazine Framework2018

    • Author(s)
      Iwase Kazuyuki、Fujinami Nobuhiro、Hashimoto Kazuhito、Kamiya Kazuhide、Nakanishi Shuji
    • Journal Title

      Chemistry Letters

      Volume: 47 Issue: 3 Pages: 304-307

    • DOI

      10.1246/cl.171117

    • NAID

      130006434176

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Selective Reduction of Nitrate by a Local Cell Catalyst Composed of Metal-Doped Covalent Triazine Frameworks2018

    • Author(s)
      Kamiya Kazuhide、Tatebe Tomomi、Yamamura Shuhei、Iwase Kazuyuki、Harada Takashi、Nakanishi Shuji
    • Journal Title

      ACS Catalysis

      Volume: 8 Issue: 4 Pages: 2693-2698

    • DOI

      10.1021/acscatal.7b04465

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Ru atom-modified covalent triazine framework as a robust electrocatalyst for selective alcohol oxidation in aqueous electrolytes2017

    • Author(s)
      Yamaguchi Shingi、Kamiya Kazuhide、Hashimoto Kazuhito、Nakanishi Shuji
    • Journal Title

      Chemical Communications

      Volume: 53 Issue: 75 Pages: 10437-10440

    • DOI

      10.1039/c7cc05841a

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Presentation] 共有結合性有機構造体の光電気化学反応への応用2020

    • Author(s)
      細川智哉, 都司柾貴,神谷和秀,原田隆史,中西周次
    • Organizer
      電気化学会第87回大会
    • Related Report
      2019 Annual Research Report
  • [Presentation] 配位構造が精密制御された単一原子電子移動触媒の開発2020

    • Author(s)
      神谷和秀
    • Organizer
      電気化学会第87回大会
    • Related Report
      2019 Annual Research Report
    • Invited
  • [Presentation] Rational design of single-atom electrocatalysts for efficient oxygen reduction reaction; : A first-principles study2020

    • Author(s)
      岩瀬和至, 中西周次, 神谷和秀
    • Organizer
      日本化学会第100春季年会
    • Related Report
      2019 Annual Research Report
  • [Presentation] 太陽エネルギー化学研究センターにおけるCO2電解に関する取り組み2020

    • Author(s)
      神谷和秀,中西周次
    • Organizer
      太陽エネルギー化学研究センター・シンポジウム「CO2の電解還元による有用化合物生成技術の動向」
    • Related Report
      2019 Annual Research Report
    • Invited
  • [Presentation] Selective CO2 reduction in acidic electrolytes by gas diffusion electrodes carrying 3d-metal modified COFs2019

    • Author(s)
      Wu Yuxin, Kazuhide amiya, Takashi Harada, Katuji Fujii, Shuji Nakanishi
    • Organizer
      2019年 電気化学秋季大会
    • Related Report
      2019 Annual Research Report
  • [Presentation] 配位不飽和金属中心が示す電極触媒能の第一原理計算を用いた理論的解析2019

    • Author(s)
      神谷和秀、岩瀬和至、中西周次
    • Organizer
      2019年 電気化学秋季大会
    • Related Report
      2019 Annual Research Report
  • [Presentation] 銅イオン担持共有結合性有機構造体薄膜の合成とその光電気化学特性2019

    • Author(s)
      細川智哉,都司柾貴,神谷和秀,原田隆史,中西周次
    • Organizer
      2019年電気化学会秋季大会
    • Related Report
      2019 Annual Research Report
  • [Presentation] 単一ルテニウム原子触媒を搭載したガス拡散電極による炭化水素部分酸化反応2019

    • Author(s)
      加藤慎太郎,原田隆史,神谷和秀,中西周次
    • Organizer
      第57回炭素材料夏季セミナー
    • Related Report
      2019 Annual Research Report
  • [Presentation] Photocatalytic reaction systems in which light-intensity functions as a control parameter for reaction selectivity2019

    • Author(s)
      Rino Sugimoto, Takashi Hard, Kazuhude Kamiya, Shuji Nakanishi原田隆史神谷和秀中西周次
    • Organizer
      Taiwan-Japan Bilateral Workshop 2019
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] リチウム空気電池の充放電サイクル特性の劣化過程 -電位制御試験による検討-2019

    • Author(s)
      森本 航太,西岡季穂,楠元崇孔,原田隆史,神谷和秀,中西周次
    • Organizer
      日本化学会秋季事業第9回CSJ化学フェスタ2019
    • Related Report
      2019 Annual Research Report
  • [Presentation] イミン架橋型共有結合性有機構造体のプロトン伝導特性の光制御2019

    • Author(s)
      都司柾貴,原田隆史,神谷和秀,中西周次
    • Organizer
      第9回 CSJ化学フェスタ2019
    • Related Report
      2019 Annual Research Report
  • [Presentation] 銅イオン担持共有結合性有機構造体薄膜の合成とその細孔内での光誘起電子移動2019

    • Author(s)
      細川智哉, 神谷和秀,原田隆史,中西周次
    • Organizer
      第9回CSJ化学フェスタ2019
    • Related Report
      2019 Annual Research Report
  • [Presentation] Single-Atom Doped Covalent Organic Frameworks as Electron-Transfer Catalysts for Applications in Energy Conversion2019

    • Author(s)
      Kazuhide Kamiya
    • Organizer
      International Workshop on Frontier of Science and Technology for Solar Energy Conversion
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Metal-doped bipyridine linked covalent organic framework fillms for photoelectrochemical applications2019

    • Author(s)
      Tomoya Hosokawa, Masaki Tsuji,Kkazuhude Kamiya,Takashi Harada,Shuji. Nakanishi
    • Organizer
      International symposium for Nano Science
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Selective hydrocarbon oxidation reactions by the gas diffusion electrode carrying Ru-modified covalent triazine frameworks2019

    • Author(s)
      Shintaro . Kato, Takashi Harada, Kazuhide Kamiya,Shuji Nakanishi
    • Organizer
      International symposium for Nano Science
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 単核金属原子ドープ共有結合性有機構造体の電子移動触媒への展開2019

    • Author(s)
      神谷和秀
    • Organizer
      機能性材料セミナー
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] 銅イオン担持ビピリジン架橋型共有結合性有機構造体から成る薄膜材料の光電気化学特性2019

    • Author(s)
      細川智哉,都司柾貴,神谷和秀,原田隆史,中西周次
    • Organizer
      日本化学会第99春季年会
    • Related Report
      2018 Annual Research Report
  • [Presentation] イミン架橋型共有結合性有機構造体のプロトン伝導特性2019

    • Author(s)
      都司柾貴,原田隆史,神谷和秀,中西周次
    • Organizer
      日本化学会第99春季年会
    • Related Report
      2018 Annual Research Report
  • [Presentation] 導電性基板上での触媒ネットワークによる亜硝酸の光誘起選択還元反応2019

    • Author(s)
      杉本梨乃,原田隆史,神谷和秀,中西周次
    • Organizer
      2019年電気化学会第86回大会
    • Related Report
      2018 Annual Research Report
  • [Presentation] 金属ドープ共有結合性有機構造体から成る電子移動触媒のガス拡散電極反応への応用2019

    • Author(s)
      加藤慎太郎, WU YUXIN,原田隆史,神谷和秀,中西周次
    • Organizer
      2019年電気化学会第86回大会
    • Related Report
      2018 Annual Research Report
  • [Presentation] 電子移動触媒としての金属担持共有結合性有機構造体とその局部電池反応への展開2018

    • Author(s)
      神谷和秀
    • Organizer
      PHyM主催講演会
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] Oxygen-Tolerant Electrodes with Single-Atom Platinum Modified Covalent Triazine Frameworks for the Hydrogen Oxidation Reaction2018

    • Author(s)
      Kazuhide Kamiya, Ryo Kamai,Kazuhito Hashimoto,Shuji Nakanishi
    • Organizer
      223rd ECS meeting
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Covalent triazine framework modified with coordinatively-unsaturated Ni atoms for CO2 electrochemical reduction2018

    • Author(s)
      Kazuhide Kamiya, Shuji Nakanishi
    • Organizer
      43rd International Conference on Coordination Chemistry(ICCC2018)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 酸化鉄半導体電極による炭化水素の光酸化反応2018

    • Author(s)
      桑原彬任,神谷和秀,原田隆史,中西周次
    • Organizer
      2018年電気化学会秋季大会
    • Related Report
      2018 Annual Research Report
  • [Presentation] 金属担持共有結合性有機構造体の二酸化炭素還元能とその反応メカニズム解析2018

    • Author(s)
      岩瀬 和至 ,神谷和秀,中西周次,橋本和仁
    • Organizer
      2018年電気化学会秋季大会
    • Related Report
      2018 Annual Research Report
  • [Presentation] 共有結合性有機構造体からなる局部電池触媒による窒素酸化物の選択的還元反応2018

    • Author(s)
      建部友実,原田隆史,岩瀬 和至 ,神谷和秀,中西周次
    • Organizer
      2018年電気化学秋季大会
    • Related Report
      2018 Annual Research Report
  • [Presentation] 有機構造体/酸化チタン複合材料から成る光局部電池触媒による亜硝酸の選択還元反応2018

    • Author(s)
      杉本梨乃,原田隆史,神谷和秀,中西周次
    • Organizer
      日本化学会秋季事業第8回CSJ化学フェスタ2018
    • Related Report
      2018 Annual Research Report
  • [Presentation] 単一金属担持共有結合性トリアジン構造体による選択的硝酸還元反応2018

    • Author(s)
      建部友実,原田隆史,神谷和秀,中西周次
    • Organizer
      日本化学会秋季事業第8回CSJ化学フェスタ2018
    • Related Report
      2018 Annual Research Report
  • [Presentation] Covalent triazine framework modified with coordinatively-unsaturated Co or Ni atoms for electrochemical CO2 reduction reaction2018

    • Author(s)
      Kazuhide Kamiya,Kazuyuki Iwase,Takashi Harada,Shuji Nakanishi
    • Organizer
      International Conference on Emerging Advanced Nanomaterials (ICEAN)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Carbon-based electron transfer catalysts for artificial photosynthesis2018

    • Author(s)
      Shuji Nakanishi, Kazuhide Kamiya
    • Organizer
      The 2018 International Conference on Green Electrochemical Technologies
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 単一白金原子担持有機構造体による水素酸化触媒能とその酸素耐性2017

    • Author(s)
      神谷和秀釜井亮橋本和仁中西周次
    • Organizer
      2017年電気化学秋季大会
    • Related Report
      2017 Annual Research Report
  • [Presentation] Selective reduction of nitrate by the local-cell catalyst composed of metal modified covalent triazine frameworks2017

    • Author(s)
      神谷和秀山村修平建部友美原田 隆史中西周次
    • Organizer
      2017 International Workshop on Electrified Interfaces for Energy Conversions
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 金属原子ドープ共有結合性有機構造体の電極触媒への応用2017

    • Author(s)
      神谷和秀
    • Organizer
      2017年度第2回関西電気化学研究会
    • Related Report
      2017 Annual Research Report
    • Invited
  • [Presentation] Highly active and selective electrocatalysts based on covalent organic frameworks modified with single metal atoms2017

    • Author(s)
      神谷和秀
    • Organizer
      International Congress on Pure & Applied Chemistry (ICPAC2018)
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 共有結合性有機構造体の固体 NMR による解析と新規機能開拓2017

    • Author(s)
      神谷和秀
    • Organizer
      地域セミナー「固体NMRを用いた材料の分析(IV)」
    • Related Report
      2017 Annual Research Report
    • Invited
  • [Remarks] 所属研究室

    • URL

      https://rcsec.osaka-u.ac.jp/nakanishilab

    • Related Report
      2019 Annual Research Report 2018 Annual Research Report
  • [Remarks] 研究者総覧

    • URL

      http://www.dma.jim.osaka-u.ac.jp/view?u=10006292

    • Related Report
      2019 Annual Research Report 2018 Annual Research Report
  • [Remarks] researchmap

    • URL

      https://researchmap.jp/kamiya0908

    • Related Report
      2019 Annual Research Report 2018 Annual Research Report
  • [Remarks] http://www.rcsec.osaka-u.ac.jp/ec/index.html

    • Related Report
      2017 Annual Research Report

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Published: 2017-04-28   Modified: 2021-02-19  

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