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Preparation Of Palladium Or Copper Supported On Porous Nitrogen-doped Carbon Material Catalyst And Its Catalystic Reaction To Aromatic Alkynes

Posted on:2022-07-29Degree:MasterType:Thesis
Country:ChinaCandidate:L MaFull Text:PDF
GTID:2491306491984739Subject:Environment Science and Resources Utilization
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Heterogeneous catalysis has been studied by many scientific researchers because of its characteristics of easy separation,easy amplification,and multiple utilization.In recent years,carbon-based materials doped with nitrogen have been widely used in the field of heterogeneous catalysis due to their special surface structure.In this paper,the preparation of the transition metal-supported carbon-nitrogen material catalyst and its catalytic performance for aromatic alkynes were studied.The main contents are as follows:1.Phosphorus and nitrogen-doped palladium nanomaterials support on coral-like carbon materials as the catalyst for semi-hydrogenation of phenylacetylene and mechanism studyIn this work,Pd nanoparticles were supported on a nitrogen-phosphorus-doped carbon material catalyst CN-P-Pd-1.4 were prepared by calcination with sodium glutamate as raw material and applied to the selective hydrogenation of phenylacetylene to styrene.The effects of temperature,solvent,heteroatom doping and other conditions on the reaction activity of the catalyst were discussed.The results showed that the conversion rate of phenylacetylene was 99.9%after reaction with methanol(15 m L),H2(1 atm),25℃for 0.5h.In addition,the best catalyst also had high reactivity to other alkynes,and the conversion rate can reach more than 95%.And the optimal catalyst can be reused for four times without significantly reducing its reactivity.2.High-efficiency catalyst for copper nanoparticles attached to porous nitrogen-doped carbon materials:applied to the coupling reaction of alkyne groups under mild conditionsIn this work,we designed a high-efficiency catalyst that uses acetone and urea as materials to synthesize copper nanoparticles supported on carbon and nitrogen materials with two calcinations and realized the reaction of acetylene derivatives to form 1,3-diyne through self-coupling.The effects of alkali,solvent,temperature,etc.on the reaction activity of the catalyst were investigated.The results showed that Cu/Cu O@CN(8)exhibited excellent reactivity to the self-coupling reaction and reached a high conversion frequency(TOF=96.8).The conversion rate of phenylacetylene can reach 99.9%under the conditions of Na OH(2 mmol),tert-butanol(2 m L),O2(1 atm)and reaction temperature of 60℃for 1h.Besides,the optimum catalyst can be reused five times under optimal conditions without a significant decrease in reactivity.
Keywords/Search Tags:heterogeneous catalysis, phenylacetylene, selective reduction, coupling reaction, mechanistic study
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