O2介质阻挡放电微等离子体制备O3

doi:10.11949/0438-1157.20191068

摘要/Abstract

摘要：

介质阻挡放电(DBD)是工业生产臭氧(O₃)最有效的方法。研究以O₂为原料气采用DBD微等离子体放电制备O₃，研究了放电间距、放电长度、放电功率以及停留时间对产生O₃的影响。此外，通过向正弦AC等离子体电源中叠加调制脉冲，探讨了脉冲占空比与调制频率对O₃生成的影响。结果表明：O₃浓度与DBD反应器的放电间距呈负相关，与O₂的停留时间呈正相关，放电功率及有效放电长度对O₃浓度的影响呈现火山形变化趋势。综合考虑O₃浓度及能量产率确定了适宜的参数。与普通正弦交流电源相比，在其基础上叠加脉冲调制电源有利于O₃的产生，而能量产率与占空比呈正相关，与调制频率呈负相关，据此确定了合适的占空比与调制频率。

关键词: 氧化, 反应器, 制备, 介质阻挡放电, 臭氧, 微等离子体

Abstract:

Dielectric barrier discharge (DBD) is considered to be the most efficient method for industrial production of ozone (O₃). O₃ was prepared by using DBD microplasma discharge with O₂ as the raw material gas. The effects of the discharge interval, discharge length, discharge power and residence time on the production of O₃ were studied. In addition, the modulated pulse was added to the sinusoidal AC power supply, and studied the effect of pulse duty cycle and modulation frequency. The results showed that the concentration of O₃ decreased with the increase of discharge length, while the energy efficiency increased first and then decreased. At the discharge length of 0.75 mm, both were in a higher range. Excessive or too small discharge length was not conducive to the formation of O₃. The suitable discharge length was 80－90 mm. With the increase of discharge power, the concentration of O₃ rose first and then decreased, and the energy efficiency decreased almost linearly.The residence time of O₂ was positively correlated with the concentration of O₃, and negatively correlated with energy efficiency. The optimal discharge power was (6.7 ± 0.2) W, and the appropriate residence time was 1.0—1.4 s. It was found that the superposition of pulse modulation power supply on the basis of common sinusoidal alternating current is beneficial to the generation of O₃, and the energy efficiency decreased with the increase of the duty cycle, increased with the enhancement of the modulation frequency. The appropriate duty cycle and modulation frequency was 60%, 800 Hz, respectively.

Key words: oxidation, reactor, preparation, dielectric barrier discharge, ozone, microplasma

中图分类号:

TQ 123.2

王保伟, 苏会娟, 姚淑美. O₂介质阻挡放电微等离子体制备O₃[J]. 化工学报, 2020, 71(2): 746-754.

Baowei WANG, Huijuan SU, Shumei YAO. Preparation of O₃ by O₂ DBD microplasma[J]. CIESC Journal, 2020, 71(2): 746-754.

图/表 12

图1 DBD微等离子体制备臭氧实验装置

Fig.1 Experimental device for O3 preparation by DBD microplasma

图2 实测DBD放电波形图

Fig.2 Measured oscillograms of DBD

图3 实测DBD放电Lissajous图

Fig.3 Measured Lissajous figure of DBD

图4 放电间距对臭氧产生性能及电子能量分布的影响

Fig.4 Effect of discharge gap on O3 production performance and electron energy distribution(discharge length: 80 mm; supply frequency: 18 kHz; Pdis: (6.7 ± 0.2) W; residence time: 1.4 s)

表1 放电间距对应的折合电场强度及平均电子能量

Table 1 E/N and mean electron energy at different discharge gap

Discharge gap/mm	(E/N)/Td	Mean electron energy/eV
0.25	760.3	16.2
0.5	488.8	11.7
0.75	360.2	9.38
1	285.2	7.93
1.25	236	6.96

图5 放电长度对臭氧产生性能的影响

Fig.5 Effect of discharge length on O3 production performance(discharge gap: 0.75 mm； supply frequency: 18 kHz； Pdis: (6.7 ± 0.2) W; residence time: 1.4 s)

图6 放电功率对臭氧浓度及能量产率的影响

Fig.6 Effect of discharge power on O3 concentration and energy yield (discharge length: 80 mm; discharge gap: 0.75 mm; supply frequency: 18 kHz; residence time: 1.4 s)

表2 放电功率对应的折合电场强度及平均电子能量

Table 2 E/N and mean electron energy at different discharge power

Discharge power/W	(E/N)/Td	Mean electron energy/eV
5	328.9	8.78
6.7	360.2	9.38
7.9	383.7	9.83
9.3	415	10.4
10.7	430.7	10.7
12.9	446.3	11

图7 放电功率对电子能量分布及反应器温度、能量密度的影响

Fig.7 Effect of discharge power on reactor temperature, SEI and EEDF(discharge length: 80 mm; discharge gap: 0.75 mm; supply frequency: 18 kHz; residence time: 1.4 s)

图8 停留时间对臭氧产生性能的影响

Fig.8 Effect of residence time on O3 production performance concentration and energy yield(discharge gap: 0.75 mm; discharge length: 80 mm; Pdis: (6.7 ± 0.2) W; supply frequency: 18 kHz)

图9 调制脉冲占空比对臭氧产生及SEI的影响

Fig.9 Effect of duty cycle of modulated pulse on O3 generation and SEI (discharge gap: 0.75 mm; discharge length: 80 mm; Pdis: (6.7 ± 0.2) W, residence time: 1.4 s; supply frequency: 18 kHz; modulation frequency: 800 Hz)

图10 调制脉冲频率对臭氧产生及SEI的影响

Fig.10 Effect of modulation frequency on O3 generation and SEI(discharge gap: 0.75 mm； discharge length: 80 mm; Pdis: (6.7 ± 0.2) W; residence time: 1.4 s; supply frequency: 18 kHz; duty cycle: 60%)

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O₂介质阻挡放电微等离子体制备O₃

Preparation of O₃ by O₂ DBD microplasma

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