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2018 Fiscal Year Research-status Report

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

Research Project

Project/Area Number 18K05202
Research InstitutionKumamoto University

Principal Investigator

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)

Project Period (FY) 2018-04-01 – 2021-03-31
Keywordsmicrowave / carbocatalysis / graphene oxide / sugars / 5-HMF / subcritical water / functionalization / bifunctional catalysts
Outline of Annual Research Achievements

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%.

Current Status of Research Progress
Current Status of Research Progress

1: Research has progressed more than it was originally planned.

Reason

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.

Strategy for Future Research Activity

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.

Causes of Carryover

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.

  • Research Products

    (20 results)

All 2019 2018 Other

All Int'l Joint Research (6 results) Journal Article (6 results) (of which Int'l Joint Research: 6 results,  Peer Reviewed: 6 results) Presentation (7 results) (of which Int'l Joint Research: 6 results,  Invited: 1 results) Book (1 results)

  • [Int'l Joint Research] Chulalongkorn University/King Mongkut U of Technology Thonburi/Silpakorn University(タイ)

    • Country Name
      THAILAND
    • Counterpart Institution
      Chulalongkorn University/King Mongkut U of Technology Thonburi/Silpakorn University
    • # of Other Institutions
      2
  • [Int'l Joint Research] Universiti Teknologi PETRONAS(マレーシア)

    • Country Name
      MALAYSIA
    • Counterpart Institution
      Universiti Teknologi PETRONAS
  • [Int'l Joint Research] De La Salle University(フィリピン)

    • Country Name
      PHILIPPINES
    • Counterpart Institution
      De La Salle University
  • [Int'l Joint Research] Institut Teknologi Sepuluh Nopember(インドネシア)

    • Country Name
      INDONESIA
    • Counterpart Institution
      Institut Teknologi Sepuluh Nopember
  • [Int'l Joint Research] Ho Chi Minh City U of Technology(ベトナム)

    • Country Name
      VIET NAM
    • Counterpart Institution
      Ho Chi Minh City U of Technology
  • [Int'l Joint Research]

    • # of Other Countries
      1
  • [Journal Article] Enhanced Levulinic Acid Production from Cellulose by Combined Bronsted Hydrothermal Carbon and Lewis Acid Catalysts2019

    • Author(s)
      Tat Boonyakarn, Piyaporn Wataniyakul, Panatpong Boonnoun, Armando T Quitain, Tetsuya Kida, Mitsuru Sasaki, Navadol Laosiripojana, Bunjerd Jongsomjit, Artiwan Shotipruk
    • Journal Title

      Industrial & Engineering Chemistry Research

      Volume: 58 Pages: 2697-2703

    • DOI

      10.1021/acs.iecr.8b05332

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Development of high microwave-absorptive bifunctional graphene oxide-based catalyst for biodiesel production2019

    • Author(s)
      Adrian Chun Minh Loy, Armando T Quitain, Man Kee Lam, Suzana Yusup, Mitsuru Sasaki, Tetsuya Kida
    • Journal Title

      Energy Conversion and Management

      Volume: 180 Pages: 1013-1025

    • DOI

      10.1016/j.enconman.2018.11.043

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Integrating reduced graphene oxide with microwave-subcritical water for cellulose depolymerization2018

    • Author(s)
      Elaine G Mission, Armando T Quitain, Yudai Hirano, Mitsuru Sasaki, Maria Jose Cocero, Tetsuya Kida
    • Journal Title

      Catalysis Science & Technology

      Volume: 8 Pages: 5434-5444

    • DOI

      10.1039/C8CY00953H

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Preparation of hydrothermal carbon as catalyst support for conversion of biomass to 5- hydroxymethylfurfural2018

    • Author(s)
      Piyaporn Wataniyakul, Panatpong Boonnoun, Armando T Quitain, Mitsuru Sasaki, Tetsuya Kida, Navadol Laosiripojana, Artiwan Shotipruk
    • Journal Title

      Catalysis Communications

      Volume: 104 Pages: 41-47

    • DOI

      10.1016/j.catcom.2017.10.014

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Preparation of hydrothermal carbon acid catalyst from defatted rice bran2018

    • Author(s)
      Piyaporn Wataniyakul, Panatpong Boonnoun, Armando T Quitain, Tetsuya Kida, Navadol Laosiripojana, Artiwan Shotipruk
    • Journal Title

      Industrial Crops and Products

      Volume: 117 Pages: 286-294

    • DOI

      10.1016/j.indcrop.2018.03.002

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Synthesis of novel graphene oxide/bentonite bi-functional heterogeneous catalyst for one-pot esterification and transesterification reactions2018

    • Author(s)
      Basit Ali, Suzana Yusup, Armando T Quitain, Mohamad Sahban Alnarabiji, Ruzaimah Nik M Kamil, Tetsuya Kida
    • Journal Title

      Energy Conversion and Management

      Volume: 171 Pages: 1801-1812

    • DOI

      10.1016/j.enconman.2018.06.082

    • Peer Reviewed / Int'l Joint Research
  • [Presentation] Microwave Carbocatalysis for Bioenergy and Biochemical Conversion2019

    • Author(s)
      Armando T. Quitain
    • Organizer
      Invited Lecture at Ateneo De Manila University
    • Invited
  • [Presentation] Integrating Graphene-based Catalysis, Microwave Irradiation and Pressurized Water for the Depolymerization of Natural Biopolymers2018

    • Author(s)
      Elaine G. Mission, Armando T. Quitain, Mitsuru Sasaki and Tetsuya Kida.
    • Organizer
      Joint International Symposium on “Multifunctional Reactors and Process Intensification for Chemical, Petrochemical and Biorefinery Industries
    • Int'l Joint Research
  • [Presentation] Synthesis and characterization of reduced graphene oxide for cellulose depolymerization under microwave-subcritical conditions2018

    • Author(s)
      Elaine G. Mission, Armando T. Quitain, Mitsuru Sasaki and Tetsuya Kida.
    • Organizer
      The 6th International Solvothermal and Hydrothermal Association (ISHA) Conference.
    • Int'l Joint Research
  • [Presentation] Fucoidan depolymerization through microwave-graphene oxide synergism2018

    • Author(s)
      Elaine G. Mission, Armando T. Quitain, Mitsuru Sasaki and Tetsuya Kida.
    • Organizer
      The 6th International Solvothermal and Hydrothermal Association (ISHA) Conference.
    • Int'l Joint Research
  • [Presentation] Microwave-Carbocatalysis Method for Conversion of Glucose to 5-HMF2018

    • Author(s)
      Tomomi Hasunuma, Armando T. Quitain, Mitsuru Sasaki, Tetsuya Kida
    • Organizer
      Joint International Symposium "Multifunctional Reactors and Process Intensification for Chemical, Petrochemical and Biorefinery Industries"
    • Int'l Joint Research
  • [Presentation] Insights into the mechanism of the acid-catalyzed hydrolysis of hesperidin using quantum chemical calculations2018

    • Author(s)
      Jonas Karl Agutaya, Armando T. Quitain et al.
    • Organizer
      8th International Symposium on Molecular Thermodynamicss and Molecular Simulation
    • Int'l Joint Research
  • [Presentation] Transition states in the acid-catalyzed hydrolysis of hesperidin2018

    • Author(s)
      Jonas Karl Agutaya, Armando T. Quitain et al.
    • Organizer
      Joint International Symposium "Multifunctional Reactors and Process Intensification for Chemical, Petrochemical and Biorefinery Industries"
    • Int'l Joint Research
  • [Book] Advances in Feedstock Conversion Technologies for Alternative Fuels and Bioproducts2019

    • Author(s)
      Basit Ali, Suzana Yusup, Armando T Quitain, Awais Bokhari, Tetsuya Kida, Lai Fatt Chuah
    • Total Pages
      18
    • Publisher
      Woodhead Publishing
    • ISBN
      978-0-12-817937-6

URL: 

Published: 2019-12-27  

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