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2022 年度 実績報告書

CO2削減のための光触媒複合体の化学設計およびDFT解析

研究課題

研究課題/領域番号 21F21342
配分区分補助金
研究機関九州大学

研究代表者

笹木 圭子  九州大学, 工学研究院, 教授 (30311525)

研究分担者 SHENOY SULAKSHANA  九州大学, 工学(系)研究科(研究院), 外国人特別研究員
研究期間 (年度) 2021-11-18 – 2024-03-31
キーワードphotocatalysis / graphitic carbon nitride / mixed metal oxides / heterojunction / hydrogen generation / pollutant degradation
研究実績の概要

A simple chemical synthesis was used to prepare mixed metal oxide namely calcium ferrite (CaFe2O4). Different amounts of CaFe2O4 were mixed with right amount of urea and calcined in a muffle furnace to make graphitic carbon nitride(g-C3N4)-CaFe2O4 heterojunction. The photodegradation of ciprofloxacin and phenol was evaluated using as-synthesized composites. Improved photocatalytic performance of composite was confirmed by electrochemical and X-ray photoelectron spectroscopy analyses. Scavenging studies and electron spin resonance spectra were used to determine active species responsible for the photodegradation process. Depending on these results, the Z-scheme charge transfer pathway is proposed and confirmed. In October 2022, this work was published in Chemical Engineering Journal. In next work, hydrothermal method was used to prepare copper cobaltite (CuCo2O4) and formed a heterojunction with g-C3N4 nanotubes. Using platinum (Pt) as a co-catalyst in as-synthesized heterojunction we evaluated its performance towards photocatalytic hydrogen evolution reaction using aqueous triethanolamine solution. Two different techniques namely photo-reduction and chemical reduction were used for reducing the Pt nanoparticles over CuCo2O4/g-C3N4 composites. The photocatalytic performance was evaluated towards H2 evolution. Mechanism for the enhanced performance in the photo-reduced Pt over the composite is evaluated based on various analytical techniques such as TEM and EXAFS. Mechanism for charge transfer is proposed. The work will soon be submitted for evaluation to reputed journal.

現在までの達成度 (区分)
現在までの達成度 (区分)

2: おおむね順調に進展している

理由

Due to a lack of resources, we shifted our focus from CO2 reduction to hydrogen production. For analyzing the byproducts of CO2 reduction, gas chromatography (GC) is essential. Although GC is available in our lab, carrier gas used is argon, which is more suited for hydrogen detection. We need to utilize a different carrier gas (helium) to measure the byproducts like CO, CH4 from CO2 reduction. Argon is low sensitive to these gases. However, only one carrier gas can be utilized at any given time. If you try to use two different carrier gases with a single GC, you will seriously damage the column. Since most of the other researchers in the lab are focusing on hydrogen generation, I shifted my research in that direction to facilitate parallel efforts. The next fiscal year 2023, have an exciting new collaboration with an AI company whose employees are well-versed in DFT. For our hydrogen generation experiments, we hope to acquire theoretical models from them at the very least.

今後の研究の推進方策

In upcoming research scheme, g-C3N4 nanosheets shall be treated with nitrogen plasma at different plasma power (20, 40, 60, 80 and 100 W) to modify surface properties. Activity of plasma modified g-C3N4 nanosheets shall be evaluated for simultaneous photo-reforming of glucose into hydrogen and valuable bio-chemicals. The transformed products after photo-reforming process are determined by high-performance liquid chromatography techniques. The evolved hydrogen in the simultaneous reaction process is quantified by gas chromatography. The experimental parameters shall be optimized depending on the primary lignocellulose source, its concentration, temperature of the reaction, catalyst loading amount and so on. We have already obtained some preliminary results for these plasma-treated samples and found that the ones treated at 80 W work better than the ones that were not treated. To understand the reason behind the enhanced performance of these plasma treated samples, X-ray photoelectron spectroscopy analysis must be conducted to determine surface changes happening after the plasma treatment. Also, it is required to conduct electron spin resonance analysis to know if any vacancies are being generated due to plasma treatment. Depending on characterization techniques reason for the enhanced photocatalytic performance will be explained. In addition, after optimization of parameter conditions g-C3N4 will be combined with various other mixed metal oxides to form composites for this simultaneous photocatalytic hydrogen evolution reaction and glucose conversion reaction.

  • 研究成果

    (10件)

すべて 2023 2022 その他

すべて 国際共同研究 (1件) 雑誌論文 (8件) (うち国際共著 8件、 査読あり 8件、 オープンアクセス 3件) 学会発表 (1件) (うち国際学会 1件)

  • [国際共同研究] SRM Institute of Science and Technology(インド)

    • 国名
      インド
    • 外国機関名
      SRM Institute of Science and Technology
  • [雑誌論文] Simple tactic polycondensation synthesis of Z-scheme quasi-polymeric g-C3N4/CaFe2O4 composite for enhanced photocatalytic water depollution via p-n heterojunction2023

    • 著者名/発表者名
      Shenoy Sulakshana、Chuaicham Chitiphon、Okumura Takamasa、Sekar Karthikeyan、Sasaki Keiko
    • 雑誌名

      Chemical Engineering Journal

      巻: 453 ページ: 139758~139758

    • DOI

      10.1016/j.cej.2022.139758

    • 査読あり / 国際共著
  • [雑誌論文] Simultaneous Photocatalytic Sugar Conversion and Hydrogen Production Using Pd Nanoparticles Decorated on Iron-Doped Hydroxyapatite2023

    • 著者名/発表者名
      Chuaicham Chitiphon、Noguchi Yuto、Shenoy Sulakshana、Shu Kaiqian、Trakulmututa Jirawat、Srikhaow Assadawoot、Sekar Karthikeyan、Sasaki Keiko
    • 雑誌名

      Catalysts

      巻: 13 ページ: 675~675

    • DOI

      10.3390/catal13040675

    • 査読あり / オープンアクセス / 国際共著
  • [雑誌論文] 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

    • 著者名/発表者名
      Preeyanghaa Mani、Chuaicham Chitiphon、Shenoy Sulakshana、Vellaichamy Balakumar、Li Wei、Manokaran Kamaraj、Varathan Elumalai、Neppolian Bernaurdshaw、Ohtani Bunsho、Sasaki Keiko、Sekar Karthikeyan
    • 雑誌名

      Environmental Science: Nano

      巻: XXXX ページ: XXXX

    • DOI

      10.1039/D3EN00038A

    • 査読あり / 国際共著
  • [雑誌論文] Recent Clay-Based Photocatalysts for Wastewater Treatment2023

    • 著者名/発表者名
      Chuaicham Chitiphon、Trakulmututa Jirawat、Shu Kaiqian、Shenoy Sulakshana、Srikhaow Assadawoot、Zhang Li、Mohan Sathya、Sekar Karthikeyan、Sasaki Keiko
    • 雑誌名

      Separations

      巻: 10 ページ: 77~77

    • DOI

      10.3390/separations10020077

    • 査読あり / オープンアクセス / 国際共著
  • [雑誌論文] Bio-reduced Ag nanoparticle decorated on ZnO for enhancement of photocatalytic reduction of hexavalent chromium and photocatalytic degradation of rhodamine B2023

    • 著者名/発表者名
      Chuaicham Chitiphon、Rizki Intan Nurul、Sekar Karthikeyan、Shenoy Sulakshana、Srikhaow Assadawoot、Trakulmututa Jirawat、Sasaki Keiko
    • 雑誌名

      Journal of Alloys and Compounds

      巻: 939 ページ: 168797~168797

    • DOI

      10.1016/j.jallcom.2023.168797

    • 査読あり / 国際共著
  • [雑誌論文] Fabrication of Reduced Ag Nanoparticle Using Crude Extract of Cinnamon Decorated on ZnO as a Photocatalyst for Hexavalent Chromium Reduction2023

    • 著者名/発表者名
      Rizki Intan Nurul、Inoue Takumi、Chuaicham Chitiphon、Shenoy Sulakshana、Srikhaow Assadawoot、Sekar Karthikeyan、Sasaki Keiko
    • 雑誌名

      Catalysts

      巻: 13 ページ: 265~265

    • DOI

      10.3390/catal13020265

    • 査読あり / オープンアクセス / 国際共著
  • [雑誌論文] Effect of transformation temperature toward optical properties of derived CuO/ZnO composite from Cu/Zn hydroxide nitrate for photocatalytic ciprofloxacin degradation2022

    • 著者名/発表者名
      Trakulmututa Jirawat、Chuaicham Chitiphon、Shenoy Sulakshana、Srikhaow Assadawoot、Sasaki Keiko、Smith Siwaporn Meejoo
    • 雑誌名

      Optical Materials

      巻: 133 ページ: 112941~112941

    • DOI

      10.1016/j.optmat.2022.112941

    • 査読あり / 国際共著
  • [雑誌論文] Cu2O/Reduced Graphene Oxide Nanocomposites for Electrocatalytic Overall Water Splitting2022

    • 著者名/発表者名
      Nallal Muthuchamy、Park Kang Hyun、Park Sungkyun、Kim Jaeyong、Shenoy Sulakshana、Chuaicham Chitiphon、Sasaki Keiko、Sekar Karthikeyan
    • 雑誌名

      ACS Applied Nano Materials

      巻: 5 ページ: 17271~17280

    • DOI

      10.1021/acsanm.2c04491

    • 査読あり / 国際共著
  • [学会発表] Simple tactic polycondensation synthesis of Z-scheme Quasi-Polymeric g-C3N4/CaFe2O4 composite for enhanced photocatalytic water depollution via p-n heterojunction,2023

    • 著者名/発表者名
      Sulakshana Shenoy, Keiko Sasaki,
    • 学会等名
      ACS 2023 spring
    • 国際学会

URL: 

公開日: 2023-12-25  

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