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Electrochemical-driven Nanoparticulate Catalysis For Highly Efficient Dechlorination Of Chlorinated Environmental Pollutant

Posted on:2022-05-27Degree:MasterType:Thesis
Country:ChinaCandidate:J Y ZhangFull Text:PDF
GTID:2491306731485964Subject:Environmental Science and Engineering
Abstract/Summary:PDF Full Text Request
Electrocatalytic reduction hydrodechlorination technology is an effective method to solve the increasingly serious water pollution at this stage.At present,the three-dimensional system constructed by adding nanoparticles to the traditional two-dimensional electrode system can solve its inherent low mass transfer rate.The defects of low free radical utilization,low current efficiency and high energy consumption also can be solved,so as to significantly improve the catalytic performance of the electrochemical system.Chlorinated pollutants are widespread in the environment,as a highly toxic and difficult-to-degrade pollutant,a new multifunctional catalytic system is designed to effectively remove chlorinated environmental pollutants in water,which has a significant impact on the environment and human health.According to the characteristic of pollutants,choosing a suitable nano-catalyst can effectively improve the removal effect of target pollutants.Palladium catalysts are widely used in the field of dechlorination and hydrogenation due to their excellent dechlorination performance.For the methodology that combines the advantages of electrochemical reduction and nanocatalysis,this method can successfully overcome their respective shortcomings,and ultimately help improve the dechlorination activity and efficiency.However,related studies are rarely reported,and the underlying mechanism of dehalogenation has not been fully resolved.Therefore,this work aims to resolve this knowledge gap.By combining the advantages of electrochemistry and nanotechnology,we have built a conceptually novel and universal electrochemically driven nanoparticle catalysis method in this article for the efficient dehalogenation of organic chlorides.By implementing this strategy,a continuous flow of 4-chlorophenol can be quickly removed with a dechlorination efficiency of 100%within 120 minutes.Importantly,we have observed that the dechlorination product phenol can be further hydrogenated to completely convert it a mixture of hexanone and cyclohexanol,the production of this mixture is significantly better than any reported catalytic method.The essence of the activation mechanism is attributed to the electric field-driven nanoparticles,which are used to activate the hydrogen generated by the electrolysis of water to produce many reactive species(such as atomic hydrogen),promote direct electron transfer on the particle surface,and effectively make it react quickly with neighboring pollutants.By carrying out research on cyclic voltammetry and atomic hydrogen quenching experiments,we first demonstrated the direct and indirect ways to reduce chlorinated environmental pollutants in the voltammogram,and provided a new evidence for the existence of these two mechanisms in the dehalogenation process.What’s more,the development of the cycle experiment shows that the pollutants can still be completely removed after five dechlorination cycles,that is,the removal rate is 100%,and the dechlorination efficiency is as high as 90%.This result confirms that all the selected materials have excellent performance and excellent stability which can greatly improve catalyst utilization.The research carried out in this paper is a study on the efficient dehalogenation of organic chlorides driven by continuous flow.The progress of this research provides a reference for the application of electrochemically driven nanoparticle catalysis for the removal of organic chlorides.At the same time,we can confirm that this method has many advantages,such as quasi-homogeneous catalytic performance with multiple reaction sites and active species,reliable and stable hydrogen source,strong safety and convenience,wide application range of p H,and fast removal rate of chlorinated environmental pollutants,strong dechlorination performance of chlorinated environmental pollutants,etc.This work also provides the first insights for electrochemically driven nanoparticle catalysis to promote the dehalogenation of chlorinated environmental pollutants,reveals in detail the removal mechanism of palladium nanocatalysts in the dechlorination and hydrogenation reaction of4-chlorophenol,and demonstrates the catalyst excellent dechlorination performance and stability.The sequence batch operation of the entire device is closer to the actual application of water pollution treatment engineering,which provides a new type of reaction device and removal idea for water pollution treatment,and also shows the electrochemical catalytic reduction technology has a wide range of application prospects.
Keywords/Search Tags:Electrocatalytic hydrodechlorination, nanoparticulate catalysis, Electrochemical, Pd/Fe3O4, chlorinated environmental pollutants
PDF Full Text Request
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