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Prepration Of Cerium And Zirconium-based Catalytic Materials Promoted By Acid/basic Sites And Their Performance In The Conversion And Utilization Of Biomass Resources

Posted on:2019-11-17Degree:MasterType:Thesis
Country:ChinaCandidate:C X KeFull Text:PDF
GTID:2371330551961695Subject:Chemistry
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At present,the catalytic cornversion and utilization of biomass derivatives are of great significance for alleviating environmental problems and sustainable development.For example,furfural alcohol derived from renewable biomass has been found to be one of the most prospective biomass platforms for high-valued chemicals and biofuels,and Received extensive attention.Another biomass derivative,5-hydroxymethylfurfural(HMF),which can aerobic oxidation into high value-added 2,5-furandicarboxylic acid(FDCA)is attracting intensive interest due to its prospects for the sustainable and promising production of bio-based aromatic polymers.Therefore,The development of mild conditions reaction is very important.Such as CTH reactions,alkali-free catalytic reactions in the aqueous phase.At the same time,the preparation of highly efficient and stable catalysts also need to be noticed.we focuses on the above reaction,and developed two high-efficiency green catalysts,respectively.The two catalysts has a very high efficiency respectively,for the preparation of FOL by CTH from FA,and the synthesis of FDCA from base-free aerobic selective catalytic oxidation of HMF.(1)As-synthesized ZrO2 exhibited excellent catalytic performance with a high 98.2%FOL selectivity at 97.1%of FA conversion.even comparable with homogeneous Lewis acid catalyst.A series of characterizations and experiments revealed that the superior catalytic performance of as-synthesized ZrO2 was attributed to a synergistic effect between the surface acid-base sites.Moreover,the as-prepared ZrO2 catalyst also presented a potential application for the efficiently catalytic transfer hydrogenation of series biomass-derived carbonyl compounds.(2)We developed a new nitrogen-doped carbon-decorated CeO2(NC-CeO2)supported Pt nanocatalyst for base-free aerobic oxidation of HMF in water.We demonstrated that the activity of supported Pt catalysts strongly depend on surface basicity and defects of supports,and as-fabricated Pt/NC-CeO2 nanoatalyst with abundant defects and favorable basicity enabled an almost 100%yield of FDCA under the optimal reaction conditions.What's more,as-fabricated supported Pt catalyst also presented good stability and reusability,owing to the novel hybrid nanostructure of support.Understanding the role of surface defects and basicity of NC-CeO2 support provides a basis for rationally designing highly efficient and stable supported metal catalysts applied practically in a variety of oxidation of biomass-derived compounds.
Keywords/Search Tags:ZrO2, acid/base sites, furfural, catalytic transfer hydrogenation, Pt/NC-CeO2, base-free aerobic oxidation, positive electric status, 5-hydroxymethylfurfural
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