• 研究課題をさがす
  • 研究者をさがす
  • KAKENの使い方
  1. 課題ページに戻る

2018 年度 実施状況報告書

Synergy of Microwave and Graphene-Based Catalysis for Conversion of Sugars Into Useful Chemicals

研究課題

研究課題/領域番号 18K05202
研究機関熊本大学

研究代表者

キタイン アルマンド  熊本大学, グローバル教育カレッジ, 教授 (50504693)

研究期間 (年度) 2018-04-01 – 2021-03-31
キーワードmicrowave / carbocatalysis / graphene oxide / sugars / 5-HMF / subcritical water / functionalization / bifunctional catalysts
研究実績の概要

GO synthesized by Hummers’ method was successfully reduced using microwave irradiation. The reduced graphene oxide (rGO) was used as a catalyst.Water as a solvent, glucose and catalysts were placed in the reactor, and microwave irradiation was applied to heat the mixture to temperatures up to 240 oC at high temperature and reaction time of up to 60 min. The products were then analyzed by high performance liquid chromatography (HPLC). The highest yield of 5-HMF obtained at this condition was about 20%. By increasing the water-glucose ratio, two-fold increase in the yield up to 38.1% was observed, confirming the role of subcritical water as catalyst for the reaction.

Results had also confirmed rGO to be an efficient catalyst for the conversion of glucose, and synergism of carbocatalysis and microwave was found to be effective.
Future direction will include tailoring the catalyst having the optimum balance of acidity to further enhance glucose conversion to 5-HMF including doping it with phosphorus or boron. One student has been sent to Prof. Anke Krueger of Wuerzburg University (Germany) to study the methods of functionalization of P and B on carbon materials in order to increase Lewis acidity that will help in increasing the rate of isomerization of glucose to fructose. The next approach is to balance the Lewis and Bronsted acidities on the surface to increase the yield of 5-HMF above 50%.

現在までの達成度 (区分)
現在までの達成度 (区分)

1: 当初の計画以上に進展している

理由

In addition to the main topic going rather smoothly as planned, a new multilateral, multidisciplinary international research collaborative project on the application of the method (i. e. microwave carbocatalysis) for the conversion of algae into bioenergy has been approved for funding by the e-ASIA joint research program (JST funding of Japan side).This collaborative research project combined the expertise of top researchers in Southeast Asian region in solving the issues and challenges regarding the use of biomass for bioenergy and biochemical production in the region.
The method has also been applied to hydrolysis of marine polysaccharide (fucoidan) for fucose production.

今後の研究の推進方策

The rGO-based catalysts will be tailored or functionalized based on the target compounds. A balance of Lewis and Bronsted acidities on the catalyst surface is important for the synthesis of 5-HMF. This can be adjusted by GO reduction by MW. This method detaches oxygen functionalities, thus increasing the Lewis acid sites on the GO surface. When necessary, GO will also be functionalized by nitrogen-doping with our simple, safe and novel approach using aqueous NH3.
A combination with Cu-based metal oxide catalysts to increase dehydration rate will also be explored. The catalysts will be characterized using XRD, FT-IR, SEM/TEM, XPS, TPD-NH3/CO2, etc.

次年度使用額が生じた理由

An RI detector and a column oven were not purchased last fiscal year.The column oven was already available in the laboratory, and an ELSD detector will be purchased in the next fiscal year using other research funds. The allocated funds for these two equipments were diverted instead for consumables, thus incurring an excess amount to be used in the next fiscal year.

The incurred amount (40,176 yen) will be used next fiscal year for consumables since it is expected that more reagents and solvents will be used due to the promising results obtained in the previous year that will require further experimental investigation and verification.

  • 研究成果

    (20件)

すべて 2019 2018 その他

すべて 国際共同研究 (6件) 雑誌論文 (6件) (うち国際共著 6件、 査読あり 6件) 学会発表 (7件) (うち国際学会 6件、 招待講演 1件) 図書 (1件)

  • [国際共同研究] Chulalongkorn University/King Mongkut U of Technology Thonburi/Silpakorn University(タイ)

    • 国名
      タイ
    • 外国機関名
      Chulalongkorn University/King Mongkut U of Technology Thonburi/Silpakorn University
    • 他の機関数
      2
  • [国際共同研究] Universiti Teknologi PETRONAS(マレーシア)

    • 国名
      マレーシア
    • 外国機関名
      Universiti Teknologi PETRONAS
  • [国際共同研究] De La Salle University(フィリピン)

    • 国名
      フィリピン
    • 外国機関名
      De La Salle University
  • [国際共同研究] Institut Teknologi Sepuluh Nopember(インドネシア)

    • 国名
      インドネシア
    • 外国機関名
      Institut Teknologi Sepuluh Nopember
  • [国際共同研究] Ho Chi Minh City U of Technology(ベトナム)

    • 国名
      ベトナム
    • 外国機関名
      Ho Chi Minh City U of Technology
  • [国際共同研究]

    • 他の国数
      1
  • [雑誌論文] Enhanced Levulinic Acid Production from Cellulose by Combined Bronsted Hydrothermal Carbon and Lewis Acid Catalysts2019

    • 著者名/発表者名
      Tat Boonyakarn, Piyaporn Wataniyakul, Panatpong Boonnoun, Armando T Quitain, Tetsuya Kida, Mitsuru Sasaki, Navadol Laosiripojana, Bunjerd Jongsomjit, Artiwan Shotipruk
    • 雑誌名

      Industrial & Engineering Chemistry Research

      巻: 58 ページ: 2697-2703

    • DOI

      10.1021/acs.iecr.8b05332

    • 査読あり / 国際共著
  • [雑誌論文] Development of high microwave-absorptive bifunctional graphene oxide-based catalyst for biodiesel production2019

    • 著者名/発表者名
      Adrian Chun Minh Loy, Armando T Quitain, Man Kee Lam, Suzana Yusup, Mitsuru Sasaki, Tetsuya Kida
    • 雑誌名

      Energy Conversion and Management

      巻: 180 ページ: 1013-1025

    • DOI

      10.1016/j.enconman.2018.11.043

    • 査読あり / 国際共著
  • [雑誌論文] Integrating reduced graphene oxide with microwave-subcritical water for cellulose depolymerization2018

    • 著者名/発表者名
      Elaine G Mission, Armando T Quitain, Yudai Hirano, Mitsuru Sasaki, Maria Jose Cocero, Tetsuya Kida
    • 雑誌名

      Catalysis Science & Technology

      巻: 8 ページ: 5434-5444

    • DOI

      10.1039/C8CY00953H

    • 査読あり / 国際共著
  • [雑誌論文] Preparation of hydrothermal carbon as catalyst support for conversion of biomass to 5- hydroxymethylfurfural2018

    • 著者名/発表者名
      Piyaporn Wataniyakul, Panatpong Boonnoun, Armando T Quitain, Mitsuru Sasaki, Tetsuya Kida, Navadol Laosiripojana, Artiwan Shotipruk
    • 雑誌名

      Catalysis Communications

      巻: 104 ページ: 41-47

    • DOI

      10.1016/j.catcom.2017.10.014

    • 査読あり / 国際共著
  • [雑誌論文] Preparation of hydrothermal carbon acid catalyst from defatted rice bran2018

    • 著者名/発表者名
      Piyaporn Wataniyakul, Panatpong Boonnoun, Armando T Quitain, Tetsuya Kida, Navadol Laosiripojana, Artiwan Shotipruk
    • 雑誌名

      Industrial Crops and Products

      巻: 117 ページ: 286-294

    • DOI

      10.1016/j.indcrop.2018.03.002

    • 査読あり / 国際共著
  • [雑誌論文] Synthesis of novel graphene oxide/bentonite bi-functional heterogeneous catalyst for one-pot esterification and transesterification reactions2018

    • 著者名/発表者名
      Basit Ali, Suzana Yusup, Armando T Quitain, Mohamad Sahban Alnarabiji, Ruzaimah Nik M Kamil, Tetsuya Kida
    • 雑誌名

      Energy Conversion and Management

      巻: 171 ページ: 1801-1812

    • DOI

      10.1016/j.enconman.2018.06.082

    • 査読あり / 国際共著
  • [学会発表] Microwave Carbocatalysis for Bioenergy and Biochemical Conversion2019

    • 著者名/発表者名
      Armando T. Quitain
    • 学会等名
      Invited Lecture at Ateneo De Manila University
    • 招待講演
  • [学会発表] Integrating Graphene-based Catalysis, Microwave Irradiation and Pressurized Water for the Depolymerization of Natural Biopolymers2018

    • 著者名/発表者名
      Elaine G. Mission, Armando T. Quitain, Mitsuru Sasaki and Tetsuya Kida.
    • 学会等名
      Joint International Symposium on “Multifunctional Reactors and Process Intensification for Chemical, Petrochemical and Biorefinery Industries
    • 国際学会
  • [学会発表] Synthesis and characterization of reduced graphene oxide for cellulose depolymerization under microwave-subcritical conditions2018

    • 著者名/発表者名
      Elaine G. Mission, Armando T. Quitain, Mitsuru Sasaki and Tetsuya Kida.
    • 学会等名
      The 6th International Solvothermal and Hydrothermal Association (ISHA) Conference.
    • 国際学会
  • [学会発表] Fucoidan depolymerization through microwave-graphene oxide synergism2018

    • 著者名/発表者名
      Elaine G. Mission, Armando T. Quitain, Mitsuru Sasaki and Tetsuya Kida.
    • 学会等名
      The 6th International Solvothermal and Hydrothermal Association (ISHA) Conference.
    • 国際学会
  • [学会発表] Microwave-Carbocatalysis Method for Conversion of Glucose to 5-HMF2018

    • 著者名/発表者名
      Tomomi Hasunuma, Armando T. Quitain, Mitsuru Sasaki, Tetsuya Kida
    • 学会等名
      Joint International Symposium "Multifunctional Reactors and Process Intensification for Chemical, Petrochemical and Biorefinery Industries"
    • 国際学会
  • [学会発表] Insights into the mechanism of the acid-catalyzed hydrolysis of hesperidin using quantum chemical calculations2018

    • 著者名/発表者名
      Jonas Karl Agutaya, Armando T. Quitain et al.
    • 学会等名
      8th International Symposium on Molecular Thermodynamicss and Molecular Simulation
    • 国際学会
  • [学会発表] Transition states in the acid-catalyzed hydrolysis of hesperidin2018

    • 著者名/発表者名
      Jonas Karl Agutaya, Armando T. Quitain et al.
    • 学会等名
      Joint International Symposium "Multifunctional Reactors and Process Intensification for Chemical, Petrochemical and Biorefinery Industries"
    • 国際学会
  • [図書] Advances in Feedstock Conversion Technologies for Alternative Fuels and Bioproducts2019

    • 著者名/発表者名
      Basit Ali, Suzana Yusup, Armando T Quitain, Awais Bokhari, Tetsuya Kida, Lai Fatt Chuah
    • 総ページ数
      18
    • 出版者
      Woodhead Publishing
    • ISBN
      978-0-12-817937-6

URL: 

公開日: 2019-12-27  

サービス概要 検索マニュアル よくある質問 お知らせ 利用規程 科研費による研究の帰属

Powered by NII kakenhi