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Chemical design and DFT approach of heterojunction photocatalysts for CO2 reduction

Research Project

Project/Area Number 22KF0285
Project/Area Number (Other) 21F21342 (2021-2022)
Research Category

Grant-in-Aid for JSPS Fellows

Allocation TypeMulti-year Fund (2023)
Single-year Grants (2021-2022)
Section外国
Review Section Basic Section 26030:Composite materials and interfaces-related
Research InstitutionKyushu University

Principal Investigator

笹木 圭子  九州大学, 工学研究院, 教授 (30311525)

Co-Investigator(Kenkyū-buntansha) SHENOY SULAKSHANA  九州大学, 工学研究院, 外国人特別研究員
Project Period (FY) 2023-03-08 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥2,300,000 (Direct Cost: ¥2,300,000)
Fiscal Year 2023: ¥900,000 (Direct Cost: ¥900,000)
Fiscal Year 2022: ¥1,100,000 (Direct Cost: ¥1,100,000)
Fiscal Year 2021: ¥300,000 (Direct Cost: ¥300,000)
Keywords光触媒 / photocatalysis / graphitic carbon nitride / mixed metal oxides / heterojunction / hydrogen generation / pollutant degradation / Photocatalysis / multi-metal oxide / CO2 reduction / solar fuels
Outline of Research at the Start

While treating g-C3N4 by nitrogen plasma, power of plasma treatment will be optimized in the beginning. The optimized plasma treated g-C3N4 shall be used to form the composites with NiMnO3. The ratio of the g-C3N4-NiMnO3 composites will be varied and the best performing photocatalyst will be determined by its performance towards the photocatalytic hydrogen evolution reaction. The stability of the photocatalyst will be determined by repeatedly recycling it after the use. Active radicals involved in the reaction will be analysed and reaction pathway for the heterojunction will be proposed.

Outline of Annual Research Achievements

CO2排出量の高い鉄鋼プロセスから生ずるスラグから合成可能なCaFe2O4とメタルフリー光触媒として注目を集めているg-C3N4の複合体により光触媒を合成し、複合化の方法や助触媒Ptの担持方法を工夫して可視光照射のもとで起こる有害有機物の分解や水素生成に応用し、窒化炭素単独の数倍の効率に向上させたことである。CaFe2O4とg-C3N4との複合体ではTEM像から両結晶の接合を直接観察し、スピン電子共鳴により・O2-が光触媒反応の主要ラジカルであること、2種の物質の接合界面を介してZスキーム機構により電子励起が起こっていることを明らかにした。ciprofloxacin および phenol光触媒反応において、二金属酸化物単独ではほとんど分解が起きないにもかかわらず、g-C3N4を複合化させると、g-C3N4単独よりも分解効率を促進した。
類似試料として、CuCo2O4とg-C3N4との複合体も検討し、Pt担持方法として化学還元法、光化学還元法を比較した。後者ではg-C3N4単独より20%増のH2生成効率を示した。この裏付けとして、光化学還元法の方がEXAFS法に依るPt-Pt原子間距離が小さく、TEM観察によるPtナノ粒子サイズが小さいことを挙げている。TEMによる局所的な裏付けだけでなく、より広域情報としてのEXAFSによる裏付けを得たのは初めてである。光化学還元では、光触媒表面に吸着したPt (OH)2Cl42-が光触媒の電子励起が起きている表面で電子授受が行われるため、より強い結合で担持され、より細かいPt粒子が形成されて、高い光触媒効果を生んだものと考えられる。一方、NaBH4による化学還元では、バルク溶液でもPt (OH)2Cl42-の還元が起き、主触媒との接合しないPt(0)ができ、溶液内でクラスターも形成されやすく結果的に光触媒反応の高効率化にはつながらなかった。

Report

(3 results)
  • 2023 Annual Research Report
  • 2022 Annual Research Report
  • 2021 Annual Research Report
  • Research Products

    (15 results)

All 2023 2022 Other

All Int'l Joint Research (2 results) Journal Article (11 results) (of which Int'l Joint Research: 11 results,  Peer Reviewed: 11 results,  Open Access: 4 results) Presentation (2 results) (of which Int'l Joint Research: 2 results)

  • [Int'l Joint Research] SRM Institute of Science and Technology(インド)

    • Related Report
      2023 Annual Research Report
  • [Int'l Joint Research] SRM Institute of Science and Technology(インド)

    • Related Report
      2022 Annual Research Report
  • [Journal Article] Atomic‐level investigation on significance of photoreduced Pt nanoparticles over g‐C<sub>3</sub>N<sub>4</sub>/bimetallic oxide composites2023

    • Author(s)
      Shenoy Sulakshana、Chuaicham Chitiphon、Sekar Karthikeyan、Sasaki Keiko
    • Journal Title

      ChemSusChem

      Volume: 16 Issue: 20 Pages: 478-491

    • DOI

      10.1002/cssc.202300478

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Mixed-Phase Fe2O3 Derived from Natural Hematite Ores/C3N4 Z-Scheme Photocatalyst for Ofloxacin Removal2023

    • Author(s)
      Shenoy Sulakshana、Farahat Mohsen M.、Chuaicham Chitiphon、Sekar Karthikeyan、Ramasamy Boopathy、Sasaki Keiko
    • Journal Title

      Catalysts

      Volume: 13 Issue: 5 Pages: 792-792

    • DOI

      10.3390/catal13050792

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Tailoring Interfacial Physicochemical Properties in Cu<sub>2</sub>O-TiO<sub>2</sub>@rGO Heterojunction: Insights from EXAFS and Electron Trap Distribution Analysis2023

    • Author(s)
      Shenoy Sulakshana、Chuaicham Chitiphon、Shanmugam Mariyappan、Okumura Takamasa、Balijapalli Umamahesh、Li Wei、Balakumar Vellaichamy、Sasaki Keiko、Sekar Karthikeyan
    • Journal Title

      ACS Applied Materials &amp; Interfaces

      Volume: 15 Issue: 46 Pages: 54105-54118

    • DOI

      10.1021/acsami.3c12130

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Simple tactic polycondensation synthesis of Z-scheme quasi-polymeric g-C3N4/CaFe2O4 composite for enhanced photocatalytic water depollution via p-n heterojunction2023

    • Author(s)
      Shenoy Sulakshana、Chuaicham Chitiphon、Okumura Takamasa、Sekar Karthikeyan、Sasaki Keiko
    • Journal Title

      Chemical Engineering Journal

      Volume: 453 Pages: 139758-139758

    • DOI

      10.1016/j.cej.2022.139758

    • Related Report
      2023 Annual Research Report 2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Simultaneous Photocatalytic Sugar Conversion and Hydrogen Production Using Pd Nanoparticles Decorated on Iron-Doped Hydroxyapatite2023

    • Author(s)
      Chuaicham Chitiphon、Noguchi Yuto、Shenoy Sulakshana、Shu Kaiqian、Trakulmututa Jirawat、Srikhaow Assadawoot、Sekar Karthikeyan、Sasaki Keiko
    • Journal Title

      Catalysts

      Volume: 13 Issue: 4 Pages: 675-675

    • DOI

      10.3390/catal13040675

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Unveiling the influence of Fe2O3 nanoparticles on CuxO-TiO2(B) nanofibers for dual Z-scheme electron transfer visible light photocatalysts: investigation on local atomic structures and electronic properties2023

    • Author(s)
      Preeyanghaa Mani、Chuaicham Chitiphon、Shenoy Sulakshana、Vellaichamy Balakumar、Li Wei、Manokaran Kamaraj、Varathan Elumalai、Neppolian Bernaurdshaw、Ohtani Bunsho、Sasaki Keiko、Sekar Karthikeyan
    • Journal Title

      Environmental Science: Nano

      Volume: XXXX Issue: 5 Pages: 1268-1283

    • DOI

      10.1039/d3en00038a

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Recent Clay-Based Photocatalysts for Wastewater Treatment2023

    • Author(s)
      Chuaicham Chitiphon、Trakulmututa Jirawat、Shu Kaiqian、Shenoy Sulakshana、Srikhaow Assadawoot、Zhang Li、Mohan Sathya、Sekar Karthikeyan、Sasaki Keiko
    • Journal Title

      Separations

      Volume: 10 Issue: 2 Pages: 77-77

    • DOI

      10.3390/separations10020077

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Bio-reduced Ag nanoparticle decorated on ZnO for enhancement of photocatalytic reduction of hexavalent chromium and photocatalytic degradation of rhodamine B2023

    • Author(s)
      Chuaicham Chitiphon、Rizki Intan Nurul、Sekar Karthikeyan、Shenoy Sulakshana、Srikhaow Assadawoot、Trakulmututa Jirawat、Sasaki Keiko
    • Journal Title

      Journal of Alloys and Compounds

      Volume: 939 Pages: 168797-168797

    • DOI

      10.1016/j.jallcom.2023.168797

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Fabrication of Reduced Ag Nanoparticle Using Crude Extract of Cinnamon Decorated on ZnO as a Photocatalyst for Hexavalent Chromium Reduction2023

    • Author(s)
      Rizki Intan Nurul、Inoue Takumi、Chuaicham Chitiphon、Shenoy Sulakshana、Srikhaow Assadawoot、Sekar Karthikeyan、Sasaki Keiko
    • Journal Title

      Catalysts

      Volume: 13 Issue: 2 Pages: 265-265

    • DOI

      10.3390/catal13020265

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Effect of transformation temperature toward optical properties of derived CuO/ZnO composite from Cu?Zn hydroxide nitrate for photocatalytic ciprofloxacin degradation2022

    • Author(s)
      Trakulmututa Jirawat、Chuaicham Chitiphon、Shenoy Sulakshana、Srikhaow Assadawoot、Sasaki Keiko、Smith Siwaporn Meejoo
    • Journal Title

      Optical Materials

      Volume: 133 Pages: 112941-112941

    • DOI

      10.1016/j.optmat.2022.112941

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Cu2O/Reduced Graphene Oxide Nanocomposites for Electrocatalytic Overall Water Splitting2022

    • Author(s)
      Nallal Muthuchamy、Park Kang Hyun、Park Sungkyun、Kim Jaeyong、Shenoy Sulakshana、Chuaicham Chitiphon、Sasaki Keiko、Sekar Karthikeyan
    • Journal Title

      ACS Applied Nano Materials

      Volume: 5 Issue: 11 Pages: 17271-17280

    • DOI

      10.1021/acsanm.2c04491

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Presentation] Simple tactic polycondensation synthesis of Z-scheme Quasi-Polymeric g-C3N4/CaFe2O4 composite for enhanced photocatalytic water depollution via p-n heterojunction2023

    • Author(s)
      Sulakshana Shenoy, Keiko Sasaki
    • Organizer
      ACS 2023 spring
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Simple tactic polycondensation synthesis of Z-scheme Quasi-Polymeric g-C3N4/CaFe2O4 composite for enhanced photocatalytic water depollution via p-n heterojunction,2023

    • Author(s)
      Sulakshana Shenoy, Keiko Sasaki,
    • Organizer
      ACS 2023 spring
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research

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Published: 2022-02-08   Modified: 2024-12-25  

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