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Synergy in magnetic Ni_(x)co_(1)o_(y) oxides enables base-free selective oxidation of 5-hydroxymethylfurfural on loaded Au nanoparticles

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Journal of Energy chemistry 2023年第3期78卷 526-536,I0014页

作者： Hao Zhang Yinghao Wang Qizhao Zhang Bang Gu Qinghu Tang Qiue cao Kun Wei Wenhao Fang School of chemical Science and Technology National Demonstration Center for Experimental Chemistry and Chemical Engineering EducationYunnan UniversityKunming 650091YunnanChina School of chemistry and chemical Engineering Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine ChemicalsKey Laboratory of Green Chemical Media and ReactionsMinistry of EducationHenan Normal UniversityXinxiang 453007HenanChina

The base-free aerobic oxidation of 5-hydroxymethylfurfural(HMF) to 2,5-furandicarboxylic acid(FDcA)in water is recognized as an important and sustainable upgrading process for cellulosic ***,selectivity control still remains a ***,we disclose that the unique synergy in magnetic Ni_(x)co_(1)o_(y)(x=1,3 and 5) bimetallic oxides can induce reactive oxygen defects and simultaneously stabilize small-sized metallic Au nanoparticles in the Au/Ni_(x)co_(1)o_(y)*** catalytic features render effective adsorption and activation of o_(2),oH and c=o groups,realizing selective oxidation of HMF to *** a series of magnetic Au/Ni_(x)co_(1)o_(y)catalysts with almost identical Au loadings(ca.0.5 wt%) and particle sizes(ca.2.7 nm),the variable Ni/co molar ratios give rise to the tunable electron density of Au sites and synergistic effect between Nio and coo_(y).The initial conversion rates of HMF and its derived intermediates(i.e., DFF,HMFcA and FFcA) show a volcano-like dependence on the number of oxygen defects(i.e.,o_(2)^(-)and o^(-)) and electron-rich *** optimum Au/Ni3co1oycatalyst exhibits a highest productivity of FDcA(12.5 mmol_(FDcA)mol_(Au)^(-1)h^(-1)) among all the Au catalysts in the literature and achieves> 99% yield of FDcA at 120℃ and 10 bar of o_(2).In addition,this catalyst can be easily recovered by a magnet and show superior stability and reusability during six consecutive cycling *** work may shed a light on Au catalysis for the base-free oxidation of biomass compounds by smartly using the synergy in bimetallic oxide carriers.

关键词： Aerobic oxidation 2,5-Furandicarboxylic acid c=o group conversion Magnetic catalyst oxygen defects Synergistic effect

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