脉冲电晕放电等离子体OH自由基发射光谱研究
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摘要
高压脉冲电晕放电等离子体在有毒有害物质脱除、烟气净化等环境领域有着重要的应用前景。在有毒有害物质脱除、烟气净化等反应过程中,起主要作用的是各种自由基和活性物种,特别是OH自由基,由于其氧化性很强,因此在各种物理化学反应中起着极其重要的作用。
本文利用发射光谱技术研究了在正脉冲、双向窄脉冲两种放电情况下各种物理参数对线-板式电晕放电产生的OH自由基的影响。
一、OH(A~2∑→X~2Π 0-0)自由基的发射光谱
利用发射光谱技术在大气压下测量了在氮气、水蒸气混合气体中线-板式正脉冲、双向窄脉冲电晕放电产生的OH(A~2∑→X~2Π 0-0)自由基的发射光谱及在潮湿空气中正脉冲电晕放电OH自由基的发射光谱。
二、OH自由基相对布居的计算
由N_2(C~3Π_u→B~3Π_g)的△v=-3和△v=-4振动带序的发射光谱强度计算得出N_2(C,v′)的相对振动布居及其振动温度,进而采用高斯分布拟合准确地求出了N_2(C~3Π_u→B~3Π_g)的△v=+1(1-0,2-1,3-2,4-3)振动带序的发射光谱强度,由N_2(C~3Π_u→B~3Π_g)的△v=+1振动带序与OH(A~2∑→X~2Π 0-0)相互重叠的发射光谱中减去N_2(C~3Π_u→B~3Π_g)的△v=+1振动带序的发射光谱强度,从而可准确求出OH(A~∑→X~Π 0-0)自由基的发射光谱强度。由OH(A~∑→X~Π 0-0)的发射光谱强度可得到激发态OH(A~2∑)自由基的相对布居。
三、放电电压、频率及添加氧气对OH自由基的影响
在氮气、水蒸气混合气体中分别研究了正脉冲、双向窄脉冲放电峰值电压、放电频率及添加氧气对激发态OH自由基的发射强度和相对布居的影响。并在潮湿空气中测量了正脉冲电晕放电的放电电压及放电频率对激发态OH自由基相对布居的影响。而且分析了放电过程中产生的活性粒子的重要的物理化学反应过程。
实验结果表明:OH自由基发射强度随着放电电压及放电频率的增加而增强,随着添加O_2流量的增加而减弱;相对布居随着放电电压及放电频率的增加呈线性增加趋势,随着添加O_2流量的增加呈e指数递减趋势。
High-voltage pulsed corona discharge plasma has been widely studied in the removal of toxic pollutant, the removal of acid gases from flues gas, and other environment management. The radicals and active spices produced by the pulsed corona discharge play important role in the removal process. Especially, OH radicals with their stronger oxidation play the central role in many physicochemical processes.In this article, the OH radials produced by positive and bi-directional pulse corona discharge in a wire-plate reactor are studied by emission spectra technology I . The emission spectra of OH (A~2∑→X~2П , 0-0) radicalsThe emission spectrum of OH (A~2∑→X~2П , 0-0) emitted from the high-voltage positive and bi-directional pulse corona discharge of N_2 and H_2O mixture gas in a wire-plate reactor is successfully recorded. And in the humid air, the emission spectrum of OH (A~2∑→X~2П, 0-0) emitted from the high-voltage positive pulse corona discharge has also been obtained.II. The calculation of the relative population of the OH radicalsThe relative vibration population and the vibration temperature of N_2(C, v') are obtained by the emission intensity of the Av = -3 and Av = -4 vibration transition band of N_2 (C~3П_u→B~3П_g). The emission spectrum of the Av = +1 (1-0, 2-1, 3-2, 4-3) vibration transition band of N_2 (C~3П_u →B~3П_g) is simulated through gauss distribution. The emission intensity of OH (A~2∑→ X~2П, 0-0) has been exactly gotten by subtracting the emission intensity of the Av = +1 vibration transition band of N_2 (C~3П_u→ B~3П_g) from the overlapping spectra. The relative population of OH (A~2∑) can be obtained by the emission intensity of OH (A~2∑→X~2П, 0-0).III. The influences of the discharge voltage, discharge frequency and the added O_2 on the production of the OH radicalsThe influences of peak voltage, discharge frequency of the positive and the bi-directional pulse discharge and the added O_2 on the emission intensity and the relative population of the OH radicals produced in the N_2 and H_2O mixture gas have been studied. The effects of the positive pulse peak voltage and frequency on the relative population of the OH radicals produced in the humid air have also been investigated. Moreover, the important physicochemical reaction processes of active spices have also been discussed.
The experimental results indicate that: the emission intensity of the OH radicals increase with increasing the peak voltage and the frequency, and decrease with increasing the O2 flow rate; the relative population of the OH radicals increase linearly with increasing the peak voltage and the frequency, and decrease exponentially with increasing the flow rate of added oxygen.
本文利用发射光谱技术研究了在正脉冲、双向窄脉冲两种放电情况下各种物理参数对线-板式电晕放电产生的OH自由基的影响。
一、OH(A~2∑→X~2Π 0-0)自由基的发射光谱
利用发射光谱技术在大气压下测量了在氮气、水蒸气混合气体中线-板式正脉冲、双向窄脉冲电晕放电产生的OH(A~2∑→X~2Π 0-0)自由基的发射光谱及在潮湿空气中正脉冲电晕放电OH自由基的发射光谱。
二、OH自由基相对布居的计算
由N_2(C~3Π_u→B~3Π_g)的△v=-3和△v=-4振动带序的发射光谱强度计算得出N_2(C,v′)的相对振动布居及其振动温度,进而采用高斯分布拟合准确地求出了N_2(C~3Π_u→B~3Π_g)的△v=+1(1-0,2-1,3-2,4-3)振动带序的发射光谱强度,由N_2(C~3Π_u→B~3Π_g)的△v=+1振动带序与OH(A~2∑→X~2Π 0-0)相互重叠的发射光谱中减去N_2(C~3Π_u→B~3Π_g)的△v=+1振动带序的发射光谱强度,从而可准确求出OH(A~∑→X~Π 0-0)自由基的发射光谱强度。由OH(A~∑→X~Π 0-0)的发射光谱强度可得到激发态OH(A~2∑)自由基的相对布居。
三、放电电压、频率及添加氧气对OH自由基的影响
在氮气、水蒸气混合气体中分别研究了正脉冲、双向窄脉冲放电峰值电压、放电频率及添加氧气对激发态OH自由基的发射强度和相对布居的影响。并在潮湿空气中测量了正脉冲电晕放电的放电电压及放电频率对激发态OH自由基相对布居的影响。而且分析了放电过程中产生的活性粒子的重要的物理化学反应过程。
实验结果表明:OH自由基发射强度随着放电电压及放电频率的增加而增强,随着添加O_2流量的增加而减弱;相对布居随着放电电压及放电频率的增加呈线性增加趋势,随着添加O_2流量的增加呈e指数递减趋势。
High-voltage pulsed corona discharge plasma has been widely studied in the removal of toxic pollutant, the removal of acid gases from flues gas, and other environment management. The radicals and active spices produced by the pulsed corona discharge play important role in the removal process. Especially, OH radicals with their stronger oxidation play the central role in many physicochemical processes.In this article, the OH radials produced by positive and bi-directional pulse corona discharge in a wire-plate reactor are studied by emission spectra technology I . The emission spectra of OH (A~2∑→X~2П , 0-0) radicalsThe emission spectrum of OH (A~2∑→X~2П , 0-0) emitted from the high-voltage positive and bi-directional pulse corona discharge of N_2 and H_2O mixture gas in a wire-plate reactor is successfully recorded. And in the humid air, the emission spectrum of OH (A~2∑→X~2П, 0-0) emitted from the high-voltage positive pulse corona discharge has also been obtained.II. The calculation of the relative population of the OH radicalsThe relative vibration population and the vibration temperature of N_2(C, v') are obtained by the emission intensity of the Av = -3 and Av = -4 vibration transition band of N_2 (C~3П_u→B~3П_g). The emission spectrum of the Av = +1 (1-0, 2-1, 3-2, 4-3) vibration transition band of N_2 (C~3П_u →B~3П_g) is simulated through gauss distribution. The emission intensity of OH (A~2∑→ X~2П, 0-0) has been exactly gotten by subtracting the emission intensity of the Av = +1 vibration transition band of N_2 (C~3П_u→ B~3П_g) from the overlapping spectra. The relative population of OH (A~2∑) can be obtained by the emission intensity of OH (A~2∑→X~2П, 0-0).III. The influences of the discharge voltage, discharge frequency and the added O_2 on the production of the OH radicalsThe influences of peak voltage, discharge frequency of the positive and the bi-directional pulse discharge and the added O_2 on the emission intensity and the relative population of the OH radicals produced in the N_2 and H_2O mixture gas have been studied. The effects of the positive pulse peak voltage and frequency on the relative population of the OH radicals produced in the humid air have also been investigated. Moreover, the important physicochemical reaction processes of active spices have also been discussed.
The experimental results indicate that: the emission intensity of the OH radicals increase with increasing the peak voltage and the frequency, and decrease with increasing the O2 flow rate; the relative population of the OH radicals increase linearly with increasing the peak voltage and the frequency, and decrease exponentially with increasing the flow rate of added oxygen.
引文
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[2] 国家环境保护总局.“七省市二氧化硫排放总量控制及排污交易政策”项目.2003年2月
[3] 万客在线.湿法烟气脱硫除尘一体化技术.2005年10月
[4] 国家环境保护总局.“两控区”空气质量状况(2002年).2003年2月
[5] 国家环境保护总局.“两控区”空气质量状况(2003年).2004年4月
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