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Synthesis Of Porous Metal Materials In Air-stabilized Ionic Liquid Systems And Their Applications

Posted on:2022-04-24Degree:DoctorType:Dissertation
Country:ChinaCandidate:Z R SongFull Text:PDF
GTID:1481306728983739Subject:Physical chemistry
Abstract/Summary:PDF Full Text Request
The design and preparation of porous metal materials are of great significance.Ionic liquids exhibit many properties.There are special structures and interactions in the air-stable ionic liquid mixed systems.In this paper,a variety of methods were proposed to synthesize porous metal materials based on the characteristics of ionic liquid mixed systems,and a series of new and efficiency porous metal materials were prepared.The main research contents are as follows:1.The microstructures of the partially miscible ionic liquid/ethanol mixed system were studied.The composition of the mixed system was very sensitive to the microzone size.Especially near the phase interface,the microzone size increased sharply.The porous PBAs,Ma[Co(CN)6]b(M=Cu,Fe,Mn,Zn)were synthesized in the partially miscible system of 1-butyl-3-methylimidazolium hexafluorophosphate([C4mim][PF6])/ethanol.And the microstructure of the solution was used as a template.The porous PBAs catalysts were applied to the epoxidation of styrene,and it showed high activity and good stability.The PBAs prepared in ionic liquid system had higher catalytic activity than that synthesized in conventional solution.The reason was that the PBAs prepared in ionic liquid system had porpsity and high specific surface area,which was conducive to the diffusion and transport of substrates and products,and its numerous active site can be promoted the reaction more effectively.2.A new strategy for the synthesis of graded porous MOF using nanostructure domain as soft template in ionic liquid/ethanol system was proposed.The morphology and porosity of MOF can be easily adjusted by controlling the amount of ligands.The porous MOF materials were synthesized in 1-hexyl-3-methylimidazolium hexafluorophosphate([C6mim][PF6])/ethanol solution.The reaction temperature of MOF in ionic liquid mixture was lower than that in organic solvent,and the synthesis temperature was reduced from 70-180 oC to 25 oC.The activity of the self-synthesized porous HKUST-1 catalyst was significantly higher than the commercial HKUST-1catalyst in the aerobic oxidation of different alcohols,and the stability was good.These graded porous MOF had the advantages of large specific surface area,adjustable pore size and designed pore environment,which shown very high catalytic activity in the aerobic oxidation of alcohols.3.The microstructures of 1-butyl-3-methylimidazolium tetrafluoroborate([C4mim][BF4])/water mixed system at different temperatures were studied.At the same temperature,the microzone in the solution near the phase interface suddenly increased.Based on this phenomenon,the changes of the microzone in the solution near the phase interface at different temperatures were studied.It was found that the ligand2-methylimidazole could aggregate and form aggregates in the solution of 70 wt%[C4mim][BF4]+30 wt%H2O.With the increased of temperature,that is,the amount of2-methylimidazole increased,the aggregate size also increased.On this basis,a new method for the synthesis of porous ZIF-8 using the microstructure of solution as template was proposed.The ZIF-8 synthesized by this method had large specific surface area and multi-stage pore properties.And the ZIF-8 had a good potential for the adsorption of heavy metal ions.The porous structure of ZIF-8 can be greatly improved the adsorption performance.In this part,not only the adsorption properties of porous material ZIF-8were studied,but also the kinetics of the whole adsorption process were studied.4.The effect of CaCl2 on the microstructure was studied in ionic liquid1-butyl-3-methylimidazoliumtetrafluoroborate([C4mim][BF4])/1-hexyl-3-methylimidazolium hexafluorophosphate([C6mim][PF6])aqueous solution.The nanotechnology areat was founded in the system,and the size increased with the increased the amount of CaCl2.Based on these findings,a new strategy for controlling the synthesis of porous material TiO2 was proposed.And the porous material TiO2was applied to the photodegradation of methylene blue.The self-synthesized porous material TiO2 showed high catalytic activity and good stability.The kinetics of the whole photodegradation process was studied.
Keywords/Search Tags:Ionic liquids, Mixed systems, Porous materials, Material synthesis, Catalytic activity
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