过渡金属电极对挥发性有机氯化物的电催化还原研究

发布时间：2023-12-04 18:25

　　挥发性有机氯化物（Cl-VOCs）包括氯代甲烷类（PCMs）、氯代乙烷类（PCAs）、氯代乙烯类(PCEs)三类物质，是环境中最常见的一类污染物。然而，由于其自身的毒性，部分物质甚至被推测为环境致癌物，致使它们中的一些物质被包括中国，美国环保署以及欧盟在内的国家和政府机构列为优先控制污染物，在饮用水中严加控制。因此，开展对此类物质的削减技术研究，寻求高效的污染控制技术，具有重要的科学技术意义。本研究在N,N-二甲基甲酰胺溶液中，考察了不同电极材料对挥发性有机氯化物的电催化脱氯活性，探讨了Cl-VOCs的电催化还原脱氯机理，并验证了电催化脱氯技术用于控制该类污染物的技术可行性。乙炔是电催化去除氯代乙烷类物质的主要中间产物，且去除乙烯气体中的乙炔杂质，是聚合物合成工业中一个非常重要的技术环节。在本研究的最后，首次提出并开发了一种新型的催化乙炔加氢技术——电催化乙炔加氢技术。 在N,N-二甲基甲酰胺溶液中，系统考察了Ag，Au，Pd，Pt，Cu，Fe，Ni，Pb，Zn和GC（玻碳电极）对氯代乙烷类物质的电化学还原脱氯活性，其中，GC电极由于其极弱的电催化特性，被选为衡量各金属电极催化效果的基...

【文章页数】：212 页

【学位级别】：博士

【文章目录】：
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
攻读博士学位期间取得的研究成果
Acknowledgements
附件



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