2019 Fiscal Year Research-status Report
Development of heterogeneous catalysts for oxidant-free conversion of biomass to fine chemicals
| Project/Area Number |
19K05556
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| Research Institution | Hokkaido University |
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Principal Investigator |
Siddiki Hakim 北海道大学, 触媒科学研究所, 特任助教 (60722650)
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| Project Period (FY) |
2019-04-01 – 2022-03-31
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| Keywords | Heterogeneous catalysis / Biomass conversion |
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| Outline of Annual Research Achievements |
To develop the heterogeneous catalytic methods for the proposed plan, the reactions including (1) Acetalization of glycerol with aldehydes and ketones,(2) Methanolysis of triglycerides/fats to form fatty acid methyl esters(FAMEs), (3) Selective alkenylation of oxindole with aldehydes, and (4)Challenging phenolysis of amides to form esters are being demonstrated employing sustainable and environmentally benign green synthesis methods through the selective conversion of biomass-derived feedstock to fine chemicals and these findings have been published in papers. In addition to these the effective the catalyst for the dehydrogenative hetero-cyclization of glycerol in reaction with ammonia to produce pyrazine is being assigned and further kinetic and mechanistic studies are underway.
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| Current Status of Research Progress |
Current Status of Research Progress
2: Research has progressed on the whole more than it was originally planned.
Reason
Dehydrogenative selective conversion of glycerol to N-heterocycles in reaction with gaseous ammonia to produce pyrazines using supported Pt nanoparticles catalysts resulted in >80% yield with >90% selectivity to the desired pyrazine. The developed catalytic system proceeds under solvent free, oxidant free conditions with the generation of environmentally benign gaseous hydrogen and water as the only byproducts. A series of metal oxides including acidic, basic, amphoteric supports and different metals nanoparticles have been tested for this dehydrogenative heterocyclization reaction. Carbon supported Pt nanoparticles showed the best performance for this reaction.
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| Strategy for Future Research Activity |
Heterogeneous property of the most effective catalysts in the synthesis of pyrazines from glycerol and ammonia will be demonstrated and to this extent catalyst reusability, metal leaching and related experiment and analyses are being designed to perform. Reaction kinetics and mechanistic studies will be revealed to obtain further catalysts design guidelines. DFT calculations and in situ spectroscopic methods are being planned so that I can use them also for this study. Novel and efficient catalytic systems would be realized on the basis of the established guidelines. Proposed N- and C-methylation reactions using glycerol as a methylating agent, will be executed as a greener methylation method using heterogeneous catalysts.
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