非热放电与催化耦合降解室内苯和甲苯研究
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摘要
在实验室前期研究基础上,本文系统研究了不同条件下多针对板电晕放电中O、N自由基的产生特点及其产率优化；利用针阵列电晕放电催化耦合技术对室内空气中常见有机污染物(VOCs)苯和甲苯进行去除实验研究,总结出适用于室内空气净化的以针阵列对板直流电晕放电为核心净化单元的空气净化器运行参数；利用气相色谱—质谱联用仪(GC-MS)等多种气体分析仪研究了针阵列电晕放电—催化耦合技术去除苯和甲苯的作用机理,为以该技术为核心构建实用室内空气净化装置提供理论支撑。
首先,以激发态O、N原子为研究对象,利用发射光谱技术研究电晕放电中的放电功率、放电极性、电极间距、相对湿度等因素对激发态O和N自由基产量的影响。在稳定放电条件下,获知两种活性自由基的产生规律以及宏观参数与其微观特性之间的相互关系。从而可更加全面地了解多针对板电晕放电产生活性物种的相关规律,为利用这些活性基团净化室内污染气体提供相应的设备优化参数。
其次,以苯和甲苯为研究对象,在封闭小室内利用针阵列电晕放电技术对两种VOCs去除规律进行研究。在正、负直流电晕放电中,分别考察了初始浓度、放电功率、电极间距以及相对湿度等参数对两种污染物去除率的影响。获知了该放电方式降解苯和甲苯的相关规律,确定了以针阵列对板电晕放电为核心净化单元的净化装置的相关运行参数。在此基础上,构建了等离子体光催化、等离子体协同MnO2和等离子体光催化协同MnO2三种耦合净化体系。在不同放电功率和相对湿度条件下,分别研究三种净化体系中苯和甲苯去除率变化,总结出以针阵列直流电晕放电技术为核心,不同耦合净化体系降解苯和甲苯的相关规律。为针阵列电晕放电催化耦合室内空气净化装置提供设计依据。
最后,采用GC-MS和CO、等多种气体检测仪,对不同净化体系中苯和甲苯降解产物及放电产生的有害副产物进行了定性和定量分析,探讨了针阵列电晕放电催化耦合技术去除苯和甲苯作用机理,为以针阵列电晕放电为核心的室内空气净化装置的设计提供理论支持。
Based on the former research in our laboratory, the production characteristic of O and N radical produced in needle matrix to plate corona discharge and their yield optimization under different experimental conditions were systematically investigated in this paper. Benzene and toluene are the common Volatile Organic Compounds (VOCs) in indoor air, the removal experiments of these two VOCs by needle matrix corona discharge coupled with catalysis was conducted. The operating parameters of indoor air purifier with needle matrix DC corona discharge as core purification unit were obtained. The removal mechanisms of benzene and toluene by needle matrix to plate corona discharge coupled with catalysis were analyzed using Gas Chromatography-Mass Spectrometer (GC-MS) and other gas analyzers, providing the theoretical support to the application of air purifier with needle matrix DC corona discharge as core technology.
Firstly, the effects of discharge power, discharge polarity, electrode gap and relative humidity on the production of excited state O and N atom were investigated by optical emission spectroscopy. The production pattern and the relationship between macro parameters and micro characteristics of O and N atom were obtained under stable discharge condition. These results could provide comprehensive understanding to the law of radicals generated in needle matrix to plate corona discharge, and then also provide corresponding optimization parameters for indoor air purifier.
Secondly, the technique of needle matrix to plate corona discharge was adopted to investigate the removal of benzene and toluene in a closed chamber. The effects of initial concentration, discharge power, electrode gap and relative humidity on the removal efficiencies of benzene and toluene were studied in positive and negative DC corona discharge. The removal patterns of benzene and toluene in this discharge mode were observed, and the operating parameters of purification device with needle matrix DC corona discharge as core purification unit were suggested. On this basis, plasma-photocatalysis, plasma-MnO2and plasma-photocatalysis-MnO2coupled purification systems were constructed. The variation trends of benzene and toluene removal efficiencies under different power and relative humidity were studied, and corresponding removal patterns of the two VOCs in different purification system were observed, providing the basis for air purifier of needle matrix DC corona discharge coupled with catalysis.
Finally, the qualitative and/or quantitative analysis for benzene and toluene degradation products and harmful byproducts in different purification systems were conducted by GC-MS and other gas analyzers. Then, the removal mechanisms of benzene and toluene by needle matrix DC corona discharge coupled with catalysis were analyzed in detail, providing the theoretical support to air purifier design with needle matrix DC corona discharge as core technology.
首先,以激发态O、N原子为研究对象,利用发射光谱技术研究电晕放电中的放电功率、放电极性、电极间距、相对湿度等因素对激发态O和N自由基产量的影响。在稳定放电条件下,获知两种活性自由基的产生规律以及宏观参数与其微观特性之间的相互关系。从而可更加全面地了解多针对板电晕放电产生活性物种的相关规律,为利用这些活性基团净化室内污染气体提供相应的设备优化参数。
其次,以苯和甲苯为研究对象,在封闭小室内利用针阵列电晕放电技术对两种VOCs去除规律进行研究。在正、负直流电晕放电中,分别考察了初始浓度、放电功率、电极间距以及相对湿度等参数对两种污染物去除率的影响。获知了该放电方式降解苯和甲苯的相关规律,确定了以针阵列对板电晕放电为核心净化单元的净化装置的相关运行参数。在此基础上,构建了等离子体光催化、等离子体协同MnO2和等离子体光催化协同MnO2三种耦合净化体系。在不同放电功率和相对湿度条件下,分别研究三种净化体系中苯和甲苯去除率变化,总结出以针阵列直流电晕放电技术为核心,不同耦合净化体系降解苯和甲苯的相关规律。为针阵列电晕放电催化耦合室内空气净化装置提供设计依据。
最后,采用GC-MS和CO、等多种气体检测仪,对不同净化体系中苯和甲苯降解产物及放电产生的有害副产物进行了定性和定量分析,探讨了针阵列电晕放电催化耦合技术去除苯和甲苯作用机理,为以针阵列电晕放电为核心的室内空气净化装置的设计提供理论支持。
Based on the former research in our laboratory, the production characteristic of O and N radical produced in needle matrix to plate corona discharge and their yield optimization under different experimental conditions were systematically investigated in this paper. Benzene and toluene are the common Volatile Organic Compounds (VOCs) in indoor air, the removal experiments of these two VOCs by needle matrix corona discharge coupled with catalysis was conducted. The operating parameters of indoor air purifier with needle matrix DC corona discharge as core purification unit were obtained. The removal mechanisms of benzene and toluene by needle matrix to plate corona discharge coupled with catalysis were analyzed using Gas Chromatography-Mass Spectrometer (GC-MS) and other gas analyzers, providing the theoretical support to the application of air purifier with needle matrix DC corona discharge as core technology.
Firstly, the effects of discharge power, discharge polarity, electrode gap and relative humidity on the production of excited state O and N atom were investigated by optical emission spectroscopy. The production pattern and the relationship between macro parameters and micro characteristics of O and N atom were obtained under stable discharge condition. These results could provide comprehensive understanding to the law of radicals generated in needle matrix to plate corona discharge, and then also provide corresponding optimization parameters for indoor air purifier.
Secondly, the technique of needle matrix to plate corona discharge was adopted to investigate the removal of benzene and toluene in a closed chamber. The effects of initial concentration, discharge power, electrode gap and relative humidity on the removal efficiencies of benzene and toluene were studied in positive and negative DC corona discharge. The removal patterns of benzene and toluene in this discharge mode were observed, and the operating parameters of purification device with needle matrix DC corona discharge as core purification unit were suggested. On this basis, plasma-photocatalysis, plasma-MnO2and plasma-photocatalysis-MnO2coupled purification systems were constructed. The variation trends of benzene and toluene removal efficiencies under different power and relative humidity were studied, and corresponding removal patterns of the two VOCs in different purification system were observed, providing the basis for air purifier of needle matrix DC corona discharge coupled with catalysis.
Finally, the qualitative and/or quantitative analysis for benzene and toluene degradation products and harmful byproducts in different purification systems were conducted by GC-MS and other gas analyzers. Then, the removal mechanisms of benzene and toluene by needle matrix DC corona discharge coupled with catalysis were analyzed in detail, providing the theoretical support to air purifier design with needle matrix DC corona discharge as core technology.
引文
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