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Base-free selective oxidation of monosaccharide into sugar acid by surface-functionalized carbon nanotube composites

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Chinese Chemical Letters 2023年第11期34卷 116-123页

作者： Zengyong Li Di Li Linxin Zhong Xuehui Li Chuanfu Liu Xinwen Peng State Key Laboratory of Pulp and Paper Engineering South China University of TechnologyGuangzhou 510641China School of Chemistry and Chemical Engineering South China University of TechnologyGuangzhou 510641China

Selective oxidation of biomass-derived monosaccharide into high value-added chemicals is highly desirable from sustainability perspectives.Herein,we demonstrate a surface-functionalized carbon nanotubesupported gold(Au/CNT-O and Au/CNT-N)catalyst for base-free oxidation of monosaccharide into sugar acid.Au/CNT-O and Au/CNT-N surfaces successfully introduced oxygen-and nitrogen-containing functional groups,respectively.The highest yields of gluconic acid and xylonic acid were 93.3%and 94.3%,respectively,using Au/CNT-N at 90℃ for 240 min,which is higher than that of using Au/CNT-O.The rate constants for monosaccharide decomposition and sugar acid formation in Au/CNT-N system were higher,while the corresponding activation energy was lower than in Au/CNT-O system.DFT calculation revealed that the mechanism of glucose oxidation to gluconic acid involves the adsorption and activation of O_(2),adsorption of glucose,dissociation of the formyl C-H bond and formation of O-H bond,and formation and desorption of gluconic acid.The activation energy barrier for the glucose oxidation over Au/CNT-N is lower than that of Au/CNT-O.The nitrogen-containing functional groups are more beneficial for accelerating monosaccharide oxidation and enhancing sugar acid selectivity than oxygen-containing functional groups.This work presents a useful guidance for designing and developing highly active catalysts for producing high-value-added chemicals from biomass.

关键词： Surface functionalization Base-free oxidation sugar acid Kinetic study DFT calculation

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Biomass-based N doped carbon as metal-free catalyst for selective oxidation of D-xylose into D-xylonic acid

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Green Energy & Environment 2022年第6期7卷 1310-1317页

作者： Zengyong Li Yiming Huang Xiao Chi Di Li Linxin Zhong Xuehui Li Chuanfu Liu Xinwen Peng State Key Laboratory of Pulp and Paper Engineering South China University of TechnologyGuangzhou510640China School of Chemistry and Chemical Engineering South China University of TechnologyGuangzhou510640China

Rational design and facile preparation of low-cost and efficient catalysts for the selective converting of biomass-derived monosaccharides into high value-added chemicals is highly demanded,yet challenging.Herein,we first demonstrate a N doped defect-rich carbon(NC-800-5)as metal-free catalyst for the selective oxidation of D-xylose into D-xylonic acid in alkaline aqueous solution at 100℃ for 30 min,with 57.4%yield.The doped graphitic N is found to be the active site and hydroxyl ion participating in the oxidation of D-xylose.Hydroxyl ion and D-xylose first adsorb on NC-800-5 surface,and the aldehyde group of D-xylose is catalyzed to form germinal diols ion.Then,C–H bond break to yield carboxylic group.Furthermore,NC-800-5 catalyst shows high stability in recycled test.

关键词： Biomass carbon Metal-free catalysts D-xylose sugar acid Selective oxidation

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