Physico-chemical mechanism of surface dielectric barrier discharge product change based on spectral diagnosis

Liu Kun; Zuo Jie; Zhou Xiong-Feng; Ran Cong-Fu; Yang Ming-Hao; Geng Wen-Qiang

doi:10.7498/aps.72.20222236

Abstract

To gain an insight into the interaction mechanism among the gaseous products of atmospheric pressure air plasma, a surface dielectric barrier discharge is used as a study object. The dynamic processes of characteristic products (nitric oxide NO and ozone O₃) are measured by in-situ Fourier infrared spectroscopy and UV absorption spectroscopy. The real energy density of the plasma is calculated by Lissajous figure and ICCD optical image. The gas temperature is obtained by fitting the emission spectrum of the second positive band of the nitrogen molecule. The results show that the real energy density and gas temperature are highly positively correlated with the applied voltage and frequency. Higher applied voltages and frequencies can lead to lower peak absorbance of O₃ and higher absorbance of NO, and accelerate the conversion of the products from O₃-containing state into O₃-free state. The microscopic mechanism of the product change is revealed by analyzing the effects of the real energy density and gas temperature on the major generation and quenching chemical reactions of the characteristic products. The analysis points out that there are two major reasons for the disappearance of O₃, i.e. the quenching effect of O and O/O₂ excited state particles on O₃ and the quenching effect of NO on O₃. And the mechanism that the disappearance of O₃ accelerates with the increase of energy density and gas temperature, is as follows. The increase of real energy density means that the energy injected into the discharge region is enhanced, which intensifies the collision reaction, thereby producing more energetic electrons and reactive oxygen and nitrogen particles. Since the discharge cavity is gas-tight, the rapid generation of O leads to a rapid increase in the ratio of O to O₂, which accelerates the decomposition of O₃; besides, the gas temperature is raised due to the intensification of the collision reaction. Whereas the gas temperature can change the rate coefficients of the chemical reactions involving the excited state particles of nitrogen and oxygen to regulate the production and quenching of the products. The increase of gas temperature has a negative effect on O₃. The higher the gas temperature, the lower the rate of O₃ generation reaction is but the higher the rate of dissociation, which is thought to be the endogenous cause of the rapid disappearance of O₃. In contrast, the gas temperature rising can significantly elevate the reaction rate of NO production and reduces its dissociation rate. This contributes to the faster production of massive NO, resulting in an accelerated quenching process of NO to O₃, which can be considered as the exogenous cause of the rapid disappearance of O₃. In a word, the present study contributes to a better understanding of the physico-chemical process in atmospheric pressure low-temperature plasma.

Keywords:

Authors and contacts

School of Electrical Engineering, Chongqing University, Chongqing 400044, China

Corresponding author: Liu Kun, liukun@cqu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 51877021).

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References

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[30]	Yin S E, Sun B M, Gao X D, Xiao H P 2009 Plasma Chem. Plasma Process. 29 421 Google Scholar
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[32]	陈忠琪, 钟安, 戴栋, 宁文军 2022 71 165201 Google Scholar Chen Z Q, Zhong A, Dai D, Ning W J 2022 Acta Phys. Sin. 71 165201 Google Scholar
[33]	Eliasson B, Hirth M, Kogelschatz U 1987 J. Phys. D Appl. Phys. 20 1421 Google Scholar
[34]	Vervloessem E, Aghaei M, Jardali F, Hafezkhiabani N, Bogaerts A 2020 ACS Sustainale Chem. Eng. 8 9711 Google Scholar
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图 1 (a)实验装置; (b)气体温度拟合

Figure 1. (a) Experimental setup; (b) gas temperature fitting.

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图 2 放电6 kHz, 6 kV条件时的原位FTIR结果

Figure 2. In-situ FTIR results with discharge at 6 kHz, 6 kV.

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图 3 特征产物随电压和频率的变化

Figure 3. Variation of the characteristic products with voltage and frequency.

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图 4 SDBD放电图像　(a) 6 kHz, 5.5 kV; (b) 6 kHz, 6.0 kV; (c) 6 kHz, 6.5 kV; (d) 6 kHz, 7.0 kV; (e) 7 kHz, 5.5 kV; (f) 8 kHz, 5.5 kV; (g) 9 kHz, 5.5 kV; (h) 10 kHz, 5.5 kV

Figure 4. SDBD discharge images: (a) 6 kHz, 5.5 kV; (b) 6 kHz, 6.0 kV; (c) 6 kHz, 6.5 kV; (d) 6 kHz, 7.0 kV; (e) 7 kHz, 5.5 kV; (f) 8 kHz, 5.5 kV; (g) 9 kHz, 5.5 kV; (h) 10 kHz, 5.5 kV.

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图 5 放电面积、能量和能量密度随电压和频率的变化　(a)频率为变量; (b)电压为变量

Figure 5. Variations of discharge area, energy and energy density with voltage and frequency: (a) Frequency as variable; (b) voltage as variable.

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图 6 气体温度随电压和频率的变化　(a)电压为变量; (b)频率为变量

Figure 6. Variation of gas temperature with voltage and frequency: (a) Voltage as variable; (b) frequency as variable.

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表 1 FTIR中不同物质对应的吸收峰波数

Table 1. Absorption peak wavenumber of differentspecies in FTIR.

化学产物	波数/cm^–1
N₂O	589, 1285, 2224, 2237
N₂O₅	743, 880, 1247, 1355, 1720
HNO₃	762, 896, 1313, 1341, 1700
O₃	1030, 1043, 1055, 2098, 2121
NO₂	1600, 1621, 1627
NO	1876

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表 2 空气放电中的主要化学反应

Table 2. Main chemical reactions in air discharge.

化学反应	速率系数k	编号	文献
e + N₂ → N(²D) + N + e	3.99 × 10^–17 ε^2.24 exp(–9.10/ε)	R1	[27]
e + N₂ → N₂(v) + e	BOLSIG+	R2	[34]
e + O₂ → O + O + e	2.03 × 10^–14 ε^–0.10 exp(–8.47/ε)	R3	[27]
e + O₂ →O(¹D) + O + e	1.82 × 10^–14 ε^–0.13 exp(–10.70/ε)	R4	[27]
e + O₂ → O₂(a) + e	1.04 × 10^–15 exp(–2.59/ε)	R5	[27]
O + O₂+ N₂ → O₃ + N₂	5.8 × 10^–34 × (300/T_g)^2.8	R6	[35]
O + O₂+ O₂ → O₃ + O₂	7.6 × 10^–34 × (300/T_g)^1.9	R7	[35]
O + O₃ → O₂ + O₂	2 × 10^–11 exp(–2300/T_g)	R8	[35]
O + O₃ → O₂ + O₂(a)	2.0 × 10^–11 exp(–2280/T_g)	R9	[34]
O₂(a) + O₃ → O₂ + O₂ + O(¹D)	5.20 × 10^–11 exp(–2480/T_g)	R10	[35]
O₂(a) + O₃ → O + O₂ + O₂	5.20 × 10^–11 exp(–2480/T_g)	R11	[35]
O(¹D) + O₃ → O₂ + O + O	1.20 × 10^–10	R12	[36]
NO + O₃ → O₂ + NO₂	4.30 × 10^–12 exp(–1560/T_g)	R13	[36]
O + NO₂ → NO + O₂	9.10 × 10^–12 × (T_g/300)^0.18	R14	[35]
O + N₂(v) → N + NO	3.01 × 10^–10 exp(–38370/T_g)	R15	[34]
N + O₃ → NO + O₂	5.00 × 10^–12 exp(–650/T_g)	R16	[34]
N + O₂ → O + NO	1.0 × 10^–11 × exp(–3473/T_g)	R17	[35]
N + O₂(a) → NO + O	2.00 × 10^–14 exp(–600/T_g)	R18	[35]
N(²D) + O₂ → NO + O	1.50 × 10^–12 exp(T_g/300)^0.5	R19	[36]
N(²D) + N₂O → N₂ + NO	1.50 × 10^–17 exp(–570/T_g)	R20	[27]
N(²D) + O₂ →NO + O(¹D)	6.00 × 10^–12 exp(T_g/300)^0.5	R21	[36]
O + NO + N₂ → NO₂ + N₂	1.20 × 10^–31 × (300/T_g)^1.7	R22	[35]
O + NO + O₂ → NO₂ + O₂	9.36 × 10^–32 × (300/T_g)^1.7	R23	[35]
注: 二元反应和三元反应的速率系数单位分别为m³/s, m⁶/s.

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[1]	Liu K, Hu Y, Lei J 2017 Phys. Plasmas 24 103513 Google Scholar
[2]	商克峰, 王美威, 鲁娜, 姜楠, 李杰, 吴彦 2021 高电压技术 47 353 Google Scholar Shang K F, Wang M W, Lu N, Jiang N, Li J, Wu Y 2021 High Volt. Eng. 47 353 Google Scholar
[3]	王兴生, 马彦明, 高勋, 林景全 2020 69 029502 Google Scholar Wang X S, Ma Y M, Gao X, Lin J Q 2020 Acta Phys. Sin. 69 029502 Google Scholar
[4]	Liu K, Zheng Z F, Liu S T, Hu Y Y 2019 Plasma Chem. Plasma Process. 39 1255 Google Scholar
[5]	高书涵, 王绪成, 张远涛 2020 69 115204 Google Scholar Gao S H, Wang X C, Zhang Y T 2020 Acta Phys. Sin. 69 115204 Google Scholar
[6]	Pang B L, Liu Z J, Zhang H Y, Wang S T, Gao Y T, Xu D H, Liu D X, Kong M G 2022 Plasma Process. Polym. 19 e2100079 Google Scholar
[7]	Zhao Z L, Wang W C, Yang D Z, Zhou X F, Yuan H 2019 IEEE Trans. Plasma Sci. 47 4219 Google Scholar
[8]	Peng B F, Jiang N, Shang K F, Lu N, Li J, Wu Y 2022 J. Phys. D Appl. Phys. 55 265202 Google Scholar
[9]	Jiang N, Kong X Q, Lu X L, Peng B F, Liu Z Y, Li J, Shang K F, Lu N, Wu Y 2022 J. Clean. Prod. 332 129998 Google Scholar
[10]	Dascalu A, Pohoata V, Shimizu K, Sirghi L 2021 Plasma Chem. Plasma Process. 41 389 Google Scholar
[11]	Park S, Choe W, Jo C 2018 Chem. Eng. J. 352 1014 Google Scholar
[12]	Douat C, Hubner S, Engeln R, Benedikt J 2016 Plasma Sources Sci. Technol. 25 025027 Google Scholar
[13]	Qin H B, Qiu H J, He S T, Hong B X, Liu K, Lou F X, Li M C, Hu P, Kong X H, Song Y J, Liu Y C, Pu M F, Han P J, Li M Z, An X P, Song L H, Tong Y G, Fan H H, Wang R X 2022 J. Hazard. Mater. 430 128414 Google Scholar
[14]	Wang S T, Liu Z J, Pang B L, Gao Y T, Luo S T, Li Q S, Chen H L, Kong M G 2022 Appl. Phys. Lett. 121 144101 Google Scholar
[15]	Shimizu T, Ikehara 2017 J. Phys. D Appl. Phys. 50 503001 Google Scholar
[16]	Shimizu T, Sakiyama Y, Graves D B, Zimmermann J L, Morfill G E 2012 New J. Phys. 14 103028 Google Scholar
[17]	Pavlovich M J, Clark D S, Graves D B 2014 Plasma Sources Sci. Technol. 23 065036 Google Scholar
[18]	Xi W, Wang W, Liu Z J, Wang Z F, Guo L, Wang X H, Rong M Z, Liu D X 2020 Plasma Sources Sci. Technol. 29 095013 Google Scholar
[19]	Waskow A, Ibba L, Leftley M, Howling A, Ambrico P F, Furno I 2021 Int. J. Mol. Sci. 22 11540 Google Scholar
[20]	万海容, 郝艳捧, 房强, 苏恒炜, 阳林, 李立浧 2020 69 145203 Google Scholar Wan H R, Hao Y P, Fang Q, Su H W, Yang L, Li L C 2020 Acta Phys. Sin. 69 145203 Google Scholar
[21]	Yuan H, Wang W C, Yang D Z, Zhao Z L, Zhang L, Wang S 2017 Plasma Sci. Technol. 19 125401 Google Scholar
[22]	Liu K, Ren W, Ran C F, Zhou R S, Tang W B, Zhou R W, Yang Z H, Ostrikov K 2021 J. Phys. D:Appl. Phys. 54 065201 Google Scholar
[23]	Liu K, Xia H T, Yang M H, Geng W Q, Zuo J, Ostrikov K 2022 Vacuum 198 110901 Google Scholar
[24]	Liu K, Duan Q S, Zheng Z F, Zhou R S, Zhou R W, Tang W B, Cullen P, Ostrikov K 2021 Plasma Process. Polym. 18 2100016 Google Scholar
[25]	Liu K, Lei J, Zheng Z, Zhu Z, Liu S 2018 Appl. Surf. Sci. 458 183 Google Scholar
[26]	高坤, 弓丹丹, 刘仁静, 苏泽华, 贾鹏英, 李雪辰 2020 光谱学与光谱分析 40 461 Google Scholar Gao K, Gong D D, Liu R J, Su Z H, Jia P Y, Li X C 2020 Spectrosc. Spect. Anal. 40 461 Google Scholar
[27]	Sakiyama Y, Graves D B, Chang H W, Shimizu T, Morfill G E 2012 J. Phys. D Appl. Phys. 45 425201 Google Scholar
[28]	Park G Y, Park S J, Choi M Y, Koo I G, Byun J H, Hong J W, Sim J Y, Collins G J, Lee J K 2012 Plasma Sources Sci. Technol. 21 043001 Google Scholar
[29]	李森, 王小兵, 马婷婷, 李栋, 戴健男 2021 真空科学与技术学报 41 619 Google Scholar Li S, Wang X B, Ma T T, Li D, Dai J N 2021 Chin. J. Vac. Sci. Technol. 41 619 Google Scholar
[30]	Yin S E, Sun B M, Gao X D, Xiao H P 2009 Plasma Chem. Plasma Process. 29 421 Google Scholar
[31]	Zhou X F, Zhao Z L, Liang J P, Yuan H, Wang W C, Yang D Z 2019 Plasma Process. Polym. 16 e1900001 Google Scholar
[32]	陈忠琪, 钟安, 戴栋, 宁文军 2022 71 165201 Google Scholar Chen Z Q, Zhong A, Dai D, Ning W J 2022 Acta Phys. Sin. 71 165201 Google Scholar
[33]	Eliasson B, Hirth M, Kogelschatz U 1987 J. Phys. D Appl. Phys. 20 1421 Google Scholar
[34]	Vervloessem E, Aghaei M, Jardali F, Hafezkhiabani N, Bogaerts A 2020 ACS Sustainale Chem. Eng. 8 9711 Google Scholar
[35]	Gordillo-Vazquez F J 2008 J. Phys. D Appl. Phys. 41 234016 Google Scholar
[36]	Kossyi I A, Kostinsky A Y, Matveyev A A, Silakov V P 1992 Plasma Sources Sci. Technol. 1 207 Google Scholar

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