基于光学检测方法的脉冲电晕放电过程中氮氧化物转化实验与机理研究
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摘要
随着社会经济的发展和人类生活水平的提高,污染物的排放也随之增加,这些污染物会对环境以及人类的身体健康产生很大的危害。燃煤电厂排放的污染物主要有SO2、NOX、Hg、VOCs和PAHs,随着排放标准的日渐严格,对污染物排放的控制要求也越来越高。NOx是其中一种非常重要且急需得到控制的污染物,所以研究NOx的脱除具有十分重要的意义。
脉冲电晕放电是一种典型的低温等离子体技术,能够产生OH、O、N、H、 HO2等大量活性自由基,这些自由基物质能够与污染物反应,将其降解成为无害的物质,从而实现多种污染物的协同脱除。在脱除过程中这些自由基和污染物的反应过程十分复杂,研究自由基与污染物的反应机理对于更有效地控制污染物具有指导性的作用。但由于自由基的存在时间非常短,检测也较为困难,而光学测量手段是一种非接触式的测量手段,它不会对整个放电过程产生干扰,且具有较高的精度,是研究污染物与自由基作用过程的理想测量方法。本文以光学测量为主要手段,以NOx为目标污染物,对NOx与自由基的反应机理进行了探讨。
本文首先对脉冲电晕放电的物理特性进行了研究。研究表明少量惰性气体(Ar)的加入可以有效减小起晕电压,气体成分中O2含量的增加减小了放电电流,提高了击穿电压。在放电区域的气体温度接近于常温,但是在尖端电极附近的温度较高,最高超过600K,且温度梯度很大。同时,进一步研究了脉冲电晕放电过程中OH自由基的演化规律,结果表明放电后OH自由基的淬灭过程可以分为两个阶段：快速淬灭阶段和慢速淬灭阶段。OH自由基的浓度随着O2浓度和湿度的增加而增加,在快速淬灭阶段OH自由基的淬灭速率随着O2浓度的增加而减小,随着湿度的增加而变大。在加入NO后,OH自由基浓度减小,但OH的淬灭速率与NO初始浓度的关系不大。
反应器结构会对NOx的转化起到较大的影响。本文以NO为目标污染物,研究了反应器结构对NO转化过程的影响。研究表明在针板放电中,针尖电极曲率半径越小,放电时流光强度越强,NO转化效率越高,针尖电极尖端数目越多,流光分布范围越广,NO转化效率也越高；在喷嘴-平板的放电形式下,由于电极气的加入,增加了自由基的产率,提高了NO的转化效率。基于上述研究,提出了一种新型的电极形式——喷气分离式放电电极,它可以有效地改善反应区域电极气和背景气的混合,增加自由基与NO的碰撞几率,提高了NO的转化效率。
电极气在脉冲电晕放电污染物脱除中关系到自由基产率和污染物脱除效果。电极气成分方面,随着Ar浓度的增加,NO的转化效率提高,OH的产率提高;随着O2浓度的增加,虽然OH的产率降低,但由于O和O3的作用NO的转化效率提高。电极气的雷诺数方面,电极气和背景气存在相互卷吸效应,雷诺数较大时(Re=4138),NO的氧化效率要高于雷诺数较低(Re=1379)的工况；同时我们对不同雷诺数下OH自由基的产率和分布进行了测量,结果也表明OH自由基在雷诺数较大时(Re=4138)的产率要比雷诺数较小时(Re=1379)高,且分布范围也更大。
在以上实验研究和理论分析基础上,进一步对NOx间的相互转化机理进行了实验和数值模拟研究。结果表明在NO2向NO的转化过程中,N2主要产生N和N2的激发态,从而起到对NO和NO2的还原作用；O2在放电过程中产生的多为氧化性自由基(O、OH、O3), NO主要被氧化成NO2,并且O2含量的提高可以有效地抑制NO2向NO的转化过程；此外NO2的初始浓度越高,在烟气条件下NO2向NO转化的效率越低。另外,我们还通过数值模拟对相应工况下的NOx转化反应进行了反应动力学计算,得到了脉冲电晕放电过程中NOx和各种自由基的演化规律。
The emission of pollutants to the environment is inevitable with the development of economy and society, which results in threats to the environment and health of human being. The pollutants emitted from coal-combustion plants mainly include SO2NOX, Hg, VOCs and PAHs. It is urgent to control the pollutants emission from combustion device as regulation to limit the pollutants emission becoming strict. NOX is an important pollutant and it is urgent to be controlled, so the investigation of NOx conversion process is significant.
Pulsed corona discharge is a typical non-thermal plasma form. The radicals such as OH, O, N, H, HO2etc. generated by pulsed corona discharge can react with pollutants so as to decompose them. The multi-pollutants simultaneous removal can be achieved by pulsed corona discharge. The reactions between pollutants and radicals are complicated in the discharge process, so investigation of the mechanism between pollutants and radicals are significant to control the pollutants effectively. However, the lifetimea of radicals are very short, and it is difficult to detect them. The optical diagnostics will not disturb the discharge process since they are non-contant measurements. They are suitable for investigation of pollutants removal mechanism because of the high resolution. NOX was chosen as a typical pollutant, and its conversion mechanism was studied by optical mehods in this thesis.
The physical characteristics in the pulsed corona discharge were studied in the thesis firstly. The results show that a little Ar could obviously reduce the threshold voltage; the increase of O? component decreased the discharge current and increased the break-down voltage. The gas temperature in the discharge zone almost equaled the room temperature, but the temperature near the tip electrode was high (more than600K), and the temperature gradient was large. The OH evolution was investigated. The OH decay after discharge can be divided into two periods:fast decay period and slow decay period. The OH density increased with increase of O2conentration and humidity. The OH decay rate in the fast decay period decreasd with increase of O2concentration, and increased with increase of humidty. The OH density decreased as NO was introduced into the reactor. The OH decay velocity was independent with the initial NO concentration.
The structure of reactor affect the NOx conversion process in corona discharge. The results show that the intensity of streamer and the NO conversion rate increased with the decrease of curve radius in needle-to-plate discharge; the streamer distribution zone and NO conversion rate increased with the increase of needle tip numbers; in the nozzle-to-plate discharge form, the OH yield and NO conversion increased because of the addition gas. In order to improve the NO conversion further, we represent a new discharge form:separated radical injection discharge, which can increase the collision probability between radicals and NO, and improve the NO conversion rate.
The addition gas is an important parameter that affects the NO conversion in pulsed corona discharge. The NO conversion was investigated under different addition gas conditions. First, the effects gas components on NO conversion were studied. The increase of Ar component improved the NO conversion rate and OH yield; the increase of O2component also improved the NO conversion, but decreased the OH yield. Then, the effects of Reynolds numbers on NO conversion were discussed. The NO conversion rate for Re=4138was larger than that for Re=1379. The OH yield and distribution zone also increased with increase of Re number.
NOX conversion mechanism in the pulsed corona discharge process was investigated based on the results above. In the process of NO2to NO. the effect of N2is reduction. N and the excited N2were produced in the discharge through the reactions between electron and N2, and then reacted with NO2to generate NO or N2; the effect of O2was oxidation. O, O3and OH radical were produced through the reactions between electron and O2, and then reacted with NO2to generate other nitric oxides. In the process of NO to NO2, the effect of N2and O2were also reduction and oxidization, repectively, which led NO convert to N2or NO2. In the process of NOX formation, there was only NO2produced under the condition of N2/O2/Ar, and the NO2concentration increased with the increase of No or O2concentration. The simulation of NOX conversion mechanism has been done under the same conditions of the experiments.
脉冲电晕放电是一种典型的低温等离子体技术,能够产生OH、O、N、H、 HO2等大量活性自由基,这些自由基物质能够与污染物反应,将其降解成为无害的物质,从而实现多种污染物的协同脱除。在脱除过程中这些自由基和污染物的反应过程十分复杂,研究自由基与污染物的反应机理对于更有效地控制污染物具有指导性的作用。但由于自由基的存在时间非常短,检测也较为困难,而光学测量手段是一种非接触式的测量手段,它不会对整个放电过程产生干扰,且具有较高的精度,是研究污染物与自由基作用过程的理想测量方法。本文以光学测量为主要手段,以NOx为目标污染物,对NOx与自由基的反应机理进行了探讨。
本文首先对脉冲电晕放电的物理特性进行了研究。研究表明少量惰性气体(Ar)的加入可以有效减小起晕电压,气体成分中O2含量的增加减小了放电电流,提高了击穿电压。在放电区域的气体温度接近于常温,但是在尖端电极附近的温度较高,最高超过600K,且温度梯度很大。同时,进一步研究了脉冲电晕放电过程中OH自由基的演化规律,结果表明放电后OH自由基的淬灭过程可以分为两个阶段：快速淬灭阶段和慢速淬灭阶段。OH自由基的浓度随着O2浓度和湿度的增加而增加,在快速淬灭阶段OH自由基的淬灭速率随着O2浓度的增加而减小,随着湿度的增加而变大。在加入NO后,OH自由基浓度减小,但OH的淬灭速率与NO初始浓度的关系不大。
反应器结构会对NOx的转化起到较大的影响。本文以NO为目标污染物,研究了反应器结构对NO转化过程的影响。研究表明在针板放电中,针尖电极曲率半径越小,放电时流光强度越强,NO转化效率越高,针尖电极尖端数目越多,流光分布范围越广,NO转化效率也越高；在喷嘴-平板的放电形式下,由于电极气的加入,增加了自由基的产率,提高了NO的转化效率。基于上述研究,提出了一种新型的电极形式——喷气分离式放电电极,它可以有效地改善反应区域电极气和背景气的混合,增加自由基与NO的碰撞几率,提高了NO的转化效率。
电极气在脉冲电晕放电污染物脱除中关系到自由基产率和污染物脱除效果。电极气成分方面,随着Ar浓度的增加,NO的转化效率提高,OH的产率提高;随着O2浓度的增加,虽然OH的产率降低,但由于O和O3的作用NO的转化效率提高。电极气的雷诺数方面,电极气和背景气存在相互卷吸效应,雷诺数较大时(Re=4138),NO的氧化效率要高于雷诺数较低(Re=1379)的工况；同时我们对不同雷诺数下OH自由基的产率和分布进行了测量,结果也表明OH自由基在雷诺数较大时(Re=4138)的产率要比雷诺数较小时(Re=1379)高,且分布范围也更大。
在以上实验研究和理论分析基础上,进一步对NOx间的相互转化机理进行了实验和数值模拟研究。结果表明在NO2向NO的转化过程中,N2主要产生N和N2的激发态,从而起到对NO和NO2的还原作用；O2在放电过程中产生的多为氧化性自由基(O、OH、O3), NO主要被氧化成NO2,并且O2含量的提高可以有效地抑制NO2向NO的转化过程；此外NO2的初始浓度越高,在烟气条件下NO2向NO转化的效率越低。另外,我们还通过数值模拟对相应工况下的NOx转化反应进行了反应动力学计算,得到了脉冲电晕放电过程中NOx和各种自由基的演化规律。
The emission of pollutants to the environment is inevitable with the development of economy and society, which results in threats to the environment and health of human being. The pollutants emitted from coal-combustion plants mainly include SO2NOX, Hg, VOCs and PAHs. It is urgent to control the pollutants emission from combustion device as regulation to limit the pollutants emission becoming strict. NOX is an important pollutant and it is urgent to be controlled, so the investigation of NOx conversion process is significant.
Pulsed corona discharge is a typical non-thermal plasma form. The radicals such as OH, O, N, H, HO2etc. generated by pulsed corona discharge can react with pollutants so as to decompose them. The multi-pollutants simultaneous removal can be achieved by pulsed corona discharge. The reactions between pollutants and radicals are complicated in the discharge process, so investigation of the mechanism between pollutants and radicals are significant to control the pollutants effectively. However, the lifetimea of radicals are very short, and it is difficult to detect them. The optical diagnostics will not disturb the discharge process since they are non-contant measurements. They are suitable for investigation of pollutants removal mechanism because of the high resolution. NOX was chosen as a typical pollutant, and its conversion mechanism was studied by optical mehods in this thesis.
The physical characteristics in the pulsed corona discharge were studied in the thesis firstly. The results show that a little Ar could obviously reduce the threshold voltage; the increase of O? component decreased the discharge current and increased the break-down voltage. The gas temperature in the discharge zone almost equaled the room temperature, but the temperature near the tip electrode was high (more than600K), and the temperature gradient was large. The OH evolution was investigated. The OH decay after discharge can be divided into two periods:fast decay period and slow decay period. The OH density increased with increase of O2conentration and humidity. The OH decay rate in the fast decay period decreasd with increase of O2concentration, and increased with increase of humidty. The OH density decreased as NO was introduced into the reactor. The OH decay velocity was independent with the initial NO concentration.
The structure of reactor affect the NOx conversion process in corona discharge. The results show that the intensity of streamer and the NO conversion rate increased with the decrease of curve radius in needle-to-plate discharge; the streamer distribution zone and NO conversion rate increased with the increase of needle tip numbers; in the nozzle-to-plate discharge form, the OH yield and NO conversion increased because of the addition gas. In order to improve the NO conversion further, we represent a new discharge form:separated radical injection discharge, which can increase the collision probability between radicals and NO, and improve the NO conversion rate.
The addition gas is an important parameter that affects the NO conversion in pulsed corona discharge. The NO conversion was investigated under different addition gas conditions. First, the effects gas components on NO conversion were studied. The increase of Ar component improved the NO conversion rate and OH yield; the increase of O2component also improved the NO conversion, but decreased the OH yield. Then, the effects of Reynolds numbers on NO conversion were discussed. The NO conversion rate for Re=4138was larger than that for Re=1379. The OH yield and distribution zone also increased with increase of Re number.
NOX conversion mechanism in the pulsed corona discharge process was investigated based on the results above. In the process of NO2to NO. the effect of N2is reduction. N and the excited N2were produced in the discharge through the reactions between electron and N2, and then reacted with NO2to generate NO or N2; the effect of O2was oxidation. O, O3and OH radical were produced through the reactions between electron and O2, and then reacted with NO2to generate other nitric oxides. In the process of NO to NO2, the effect of N2and O2were also reduction and oxidization, repectively, which led NO convert to N2or NO2. In the process of NOX formation, there was only NO2produced under the condition of N2/O2/Ar, and the NO2concentration increased with the increase of No or O2concentration. The simulation of NOX conversion mechanism has been done under the same conditions of the experiments.
引文
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