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Preparation Of ZIFs-derived Nanometerials And Their Catalytic Performance For Hydrogenation Of Biomass-based Furfural

Posted on:2022-01-15Degree:MasterType:Thesis
Country:ChinaCandidate:Y F FanFull Text:PDF
GTID:2481306617498264Subject:Material Science
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With the increasing consumption of fossil energy and the sharply prominent environmental problems,the development and utilization of biomass energy has received more and more attention.In the utilization of biomass resources,the catalytic conversion of the biomass platform molecule furfural(FF)is of great significance in the synthesis of high value-added chemicals and liquid fuels.Furfuryl alcohol(FAL),as an important hydrogenation product of furfural,is widely used in the synthesis of adhesives,resins,and synthetic fibers.Therefore,the development of high-efficiency and stable catalysts plays an important role in realizing the highly selective conversion of furfural to furfuryl alcohol.First,through the ZIFs precursor,the multi-metal Cu,Co,Zn supported on the nitrogen-doped porous carbon catalyst(Cu Co/Zn@NPC)was designed and synthesized using the multi-metal control strategy.The conversion rate of FF of Cu Co/Zn@NPC-600 catalyst after heat treatment at 600 oC is close to 100%at 140 oC,while the selectivity of FAL is 100%.At the same time,in the catalytic hydrogen transfer reaction(CTH)with isopropanol as the hydrogen donor,the conversion rate of FF reached 95.8%,and the selectivity of FAL reached99.1%.The yield of Zn doped on Cu Co/Zn@NPC-600 catalyst is 37.3 times that of Cu Co@NPC-600 catalyst,and the yield of catalytic reaction is increased by 2.3 times when Cu is added.In addition,the Cu Co/Zn@NPC-600 catalyst showed good FF hydrogenation cycle performance in the 4 cycles test.The high activity of the Cu Co/Zn@NPC-600 catalyst is mainly due to the high dispersion of metallic Co nanoparticles,the advanced porous structure formed by the volatilization of Zn from the precursor template,and the synergy between Cu and Co.In addition,we used ZIFs precursors and host-guest strategies to successfully prepare a catalyst(Ni-SAs/NC)with a single Ni atom supported on nitrogen-doped carbon,which was used for the first time in the hydrogen transfer reaction of furfural to furfuryl alcohol.The atom-dispersed Ni-N4 sites change the electron density of the metal center,showing specific adsorption and desorption for FF and FAL.Ni-SAs/NC exhibits excellent catalytic performance.Under 130 oC reaction conditions,the FAL selectivity is as high as 97.1%,and the conversion frequency(TOF)is 832 h-1.It is the supported Ni nano-catalyst(Ni-NPs/NC)9 times.The Ni-SAs/NC catalyst has good stability,and the catalytic activity does not decrease significantly after four reaction cycles.Ni-SAs/NC also has good catalytic activity for the conversion of many?,?-unsaturated aldehydes to?,?-unsaturated alcohols.
Keywords/Search Tags:Furfural, Hydrogenation reaction, Nanoparticles, Single-atom, Catalytic transfer hydrogenation reaction
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