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過渡金屬電極對(duì)揮發(fā)性有機(jī)氯化物的電催化還原研究

發(fā)布時(shí)間:2023-12-04 18:25
  揮發(fā)性有機(jī)氯化物(Cl-VOCs)包括氯代甲烷類(PCMs)、氯代乙烷類(PCAs)、氯代乙烯類(PCEs)三類物質(zhì),是環(huán)境中最常見的一類污染物。然而,由于其自身的毒性,部分物質(zhì)甚至被推測為環(huán)境致癌物,致使它們中的一些物質(zhì)被包括中國,美國環(huán)保署以及歐盟在內(nèi)的國家和政府機(jī)構(gòu)列為優(yōu)先控制污染物,在飲用水中嚴(yán)加控制。因此,開展對(duì)此類物質(zhì)的削減技術(shù)研究,尋求高效的污染控制技術(shù),具有重要的科學(xué)技術(shù)意義。本研究在N,N-二甲基甲酰胺溶液中,考察了不同電極材料對(duì)揮發(fā)性有機(jī)氯化物的電催化脫氯活性,探討了Cl-VOCs的電催化還原脫氯機(jī)理,并驗(yàn)證了電催化脫氯技術(shù)用于控制該類污染物的技術(shù)可行性。乙炔是電催化去除氯代乙烷類物質(zhì)的主要中間產(chǎn)物,且去除乙烯氣體中的乙炔雜質(zhì),是聚合物合成工業(yè)中一個(gè)非常重要的技術(shù)環(huán)節(jié)。在本研究的最后,首次提出并開發(fā)了一種新型的催化乙炔加氫技術(shù)——電催化乙炔加氫技術(shù)。 在N,N-二甲基甲酰胺溶液中,系統(tǒng)考察了Ag,Au,Pd,Pt,Cu,F(xiàn)e,Ni,Pb,Zn和GC(玻碳電極)對(duì)氯代乙烷類物質(zhì)的電化學(xué)還原脫氯活性,其中,GC電極由于其極弱的電催化特性,被選為衡量各金屬電極催化效果的基...

【文章頁數(shù)】:212 頁

【學(xué)位級(jí)別】:博士

【文章目錄】:
摘要
Abstract
Table of contents
Chapter 1 Introduction
    1.1 The properties, sources of Cl-VOCs and their harms to human
        1.1.1 Chlorinated methanes
        1.1.2 Chlorinated ethanes
        1.1.3 Chlorinated ethylenes
    1.2 Remediation technologies for Cl-VOCs
    1.3 Research motivations
    1.4 Research scope
    Reference
Chapter 2 Literature review
    2.1 Electron transfer mechanism to chlorinated aliphatic compounds
    2.2 Electrochemical kinetics towards dechlorination of Cl-VOCs
    2.3 Electrochemical reduction of chlorinated volatile organic compounds (Cl-VOCs)
        2.3.1 Cathode materials
        2.3.2 Cathodic potentials
        2.3.3 Solvent chemistry
        2.3.4 Fabrication of electrochemical reactor
        2.3.5 Molecular structure of chlorinated compounds
    Reference
Chapter 3 Electrocatalytic properties of transition metals towards reductive dechlorination of polychloroethanes
    Abstract
    3.1 Introduction
    3.2 Experimental and methods
        3.2.1 Materials and chemicals
        3.2.2 Experiment instrumentation
        3.2.3 Cyclic voltammetry experiments
        3.2.4 Analysis
    3.3 Results and discussion
        3.3.1 Cyclic voltammetries of polychloroethanes
        3.3.2 Electron transfer to PCAs
        3.3.3 Electrocatalytic activities of transition metals towards PCAs reduction
        3.3.4 Thermodynamics of ET to PCAs
    3.4 Conclusions
    Reference
Chapter 4 Electrolytic dechlorination of polychloroethanes (PCAs) on catalytic and non-catalytic electrodes
    Abstract
    4.1 Introduction
    4.2 Experimental and methods
        4.2.1 Materials and chemicals
        4.2.2 Experimental instrumentations
        4.2.3 Cyclic voltammetry and electrolysis
        4.2.4 Analysis
    4.3 Results and discussion
        4.3.1 Electrolysis of 1,1,1-TCA
        4.3.2. Electrolysis of 1,1,1,2-tetrachloroethane
        4.3.3 Electrocatalytic dechlorination of geminal PCAs on Cu electrode
    4.4 Conclusions
    Reference
Chapter 5 Electrocatalytic dechlorination of polychloromethanes (PCMs) on Cu electrode
    Abstract
    5.1 Introduction
    5.2 Experimental and methods
        5.2.1 Materials and chemicals
        5.2.2 Experiment instrumentation
        5.2.3 Cyclic voltammetry and electrolysis experiments
        5.2.4 Analysis
    5.3 Results and discussion
        5.3.1 Cyclic voltammetry of polychloromethanes
        5.3.2 Electrolysis of carbon tetrachloride
        5.3.3 Electrolysis of chloroform
        5.3.4 Reduction of PCMs and geminal PCAs at Cu
    5.4 Conclusions
    Reference
Chapter 6 Eletrochemical partial hydrogenation of acetylene at precious and non-precious metal electrodes
    Abstract
    6.1. Introduction
    6.2. Experimental and Methods
        6.2.1. Materials and chemicals
        6.2.2. Experimental instrumentation
        6.2.3. Cyclic voltammetry experiments and electrolysis
        6.2.4. Analysis
    6.3. Results and discussion
        6.3.1. Cyclic voltammetry of acetylene at different electrodes
        6.3.2 Electrochemical hydrogenation of acetylene
    6.4. Conclusion
    References
Chapter 7 Conclusions and suggestions
    7.1 Conclusions
    7.2 Suggestions
攻讀博士學(xué)位期間取得的研究成果
Acknowledgements
附件



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