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Metal Porphyrin Electrocatalysis Inert Carbon Halogen Bond Activation And Carboloy Reaction

Posted on:2019-01-09Degree:MasterType:Thesis
Country:ChinaCandidate:J X WenFull Text:PDF
GTID:2371330566968766Subject:Chemical Engineering
Abstract/Summary:PDF Full Text Request
Organo-halogen contaminants,due to the long-term accumulation and persistence,are plaguing human production and life,especially the threat to the environment and human health.The search for efficient methods for the degradation and conversion of organohalogen compounds has been a hot topic for chemists.Investigations and studies have shown that electro-catalytic reduction of organic halogens is highly efficient,easy to operate,and less polluting,making it the best choice for solving this problem.In addition,the electro-catalytic reduction method can also be applied to electrocatalytic reduction of hydrogen evolution reactions to generate clean new energy hydrogen,solve the energy crisis,and fundamentally alleviate the shortage of fossil fuels and air pollution.In this paper,we have selected environmental pollutants such as hexachlorocyclohexane??-HCH?,hexafluorobenzene,and pentafluoropyridine,and selected metal porphyrins that are inexpensive,easy to synthesize,and have high catalytic activity.The catalysts,using electro-catalytic reduction techniques,were subjected to degradation tests and mechanisms.In the paper,a variety of metal porphyrin catalysts were synthesized,including iron porphyrin,cobalt porphyrin,nickel porphyrin,manganese porphyrin,copper porphyrin and zinc porphyrin.A2B metal cobalt with Push-Pull electronic structure was also synthesized.The electronic structures of the compounds were studied by spectroscopic,electrochemical,spectroelectrochemical and other methods.Using metal porphyrins as catalysts to act on fluorine-containing pollutants hexafluorobenzene and pentafluoropyridine,the results show that different metalloporphyrins have different catalytic efficiencies under weak alkaline conditions,among which cobalt porphyrins have the most effective effect.Strong;The solvent effect was also studied.Dimethyl sulfoxide?DMSO?and N,N'-dimethylformamide?DMF?were selected and found in a weakly basic solvent N,N'-dimethylformamide?DMF?.The effect of defluorination is better;under the conditions of energization and natural agitation,it is found that access to controllable potentials can effectively promote defluorination,and many studies have yielded results that are worthy of consideration,and also for follow-up studies.Provide more ideas.Finally,we synthesized six kinds of A2B metal cobalt pyrrole complexes with Push-Pull electronic structure and three kinds of copper pyrrole complexes.The spectroscopic,electrochemical,spectroelectrochemical and TD-DFT theoretical calculation methods The electronic structures of compounds have been studied,and the catalytic efficiencies of various compounds in the hydrogen evolution reaction in non-aqueous solutions have been studied.The catalytic mechanism and structure-activity relationship have been proposed to generate new energy hydrogen,which can effectively solve the energy crisis.
Keywords/Search Tags:mental porphyrin, mental pyrrole, electrochemical catalysis, carbon-chlorine bond cleavage, hydrogen evolution reaction
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