蔡加禾; 戴栋; 潘泳全

doi:10.7498/aps.74.20250827

摘要
在大气压介质阻挡放电的某些应用场景中, 待处理物表面附着的水滴会改变气隙宽度、介电分布、气相成分等条件, 进而影响低温等离子体的应用效果. 本文建立了大气压氦气介质阻挡放电仿真模型, 探究了接触角为45°, 90°和135°的水滴附着于待处理物表面时稳态放电结构与活性粒子分布受到的影响及其背后机制. 结果表明, 水滴表面与上方区域的稳态放电强度受到削弱, 这是因为在负击穿中, 水滴表面的极化电场增强了等离子体双极性扩散, 促成环形放电抑制区; 在次正放电阶段, 水滴极化导致的种子电子清除效应抑制了水滴上方区域放电, 上述放电抑制作用随水滴接触角变大而提升. 在化学分布部分, 待处理物和水滴表面的活性粒子与电子存在着协同分布关系, 其中O与N的分布会因O₂与N₂键能的不同产生差异, OH与He⁺的分布则分别受到水滴蒸发与电场的影响. 本文系统地阐述了水滴附着对介质阻挡放电电化学过程的影响机制, 为等离子体-液滴系统的相关应用提供了理论指导.

关键词:
介质阻挡放电 /

水滴 /

放电结构 /

活性粒子
Abstract
Dielectric barrier discharge technology can generate cold plasma at atmospheric pressure, which contains abundant active particles and shows great potential for fresh produce sterilization applications. However, water droplets frequently adhere to the surfaces of fruits and vegetables, which changes key parameters including the gas gap width, dielectric distribution, and gas-phase composition, consequently affecting the effectiveness of plasma applications. Currently, plasma-droplet interactions with contact angle as a variable remain unexplored, and the underlying mechanisms by which adhering droplets affect the electrochemical characteristics of dielectric barrier discharge require further investigation. In this work, we develop an atmospheric-pressure helium dielectric barrier discharge simulation model with an He-O₂-N₂-H₂O reaction system. This model is used to study how water droplets (with contact angles of 45°, 90°, and 135°) adhering to the surface of the specimens affect both the steady-state discharge structure and active particle distribution, as well as their underlying mechanisms. The results show that the steady-state discharge intensity is significantly weakened both at the droplet surface and in the region above it, with the greatest reduction occurring at a contact angle of 135°. During the main positive breakdown phase, the polarized electric field at the droplet surface significantly enhances both electron impact ionization and secondary electron emission, thereby promoting gas-phase breakdown in the region above the water droplet. During the main negative breakdown phase, this polarized electric field accelerates electron migration toward the liquid surface, which intensifies plasma ambipolar diffusion and consequently leads to the formation of an annular discharge suppression zone around the water droplet. During the secondary positive discharge phase, even though the water droplet becomes polarized and a radially inward electric field is generated near the liquid surface, the resulting seed electron scavenging effect suppresses discharge in the region above the water droplet. Due to the stronger polarized electric fields generated at the surfaces of water droplets with larger contact angles, both the discharge enhancement and suppression effects become more pronounced with the increase of contact angle. Regarding the chemical species distribution, active particles and electrons exhibit a synergistic distribution relationship. On the surface of the specimens, He⁺ ions undergo electric field-driven migration, resulting in a highly non-uniform spatial distribution. The evaporation of water droplets provides more reactant sources for OH generation, thereby increasing its total deposition quantity. Because the bond energy of O₂ is lower than that of N₂, oxygen (O) demonstrates a more uniform distribution and a greater total deposition quantity than nitrogen (N). On the surfaces of water droplets, the active particles exhibit a gradually decreasing distribution from the center to the edge. Notably, the total deposition quantity of He⁺ continuously increases with larger contact angles increasing due to the aggregation effect of the polarized electric field. This study systematically elucidates the influence mechanisms of adhering water droplets on the electrochemical processes in dielectric barrier discharge, providing theoretical guidance for relevant applications of plasma-droplet systems.

Keywords:
dielectric barrier discharge /

water droplet /

discharge structure /

active particle
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序号	反应式	速率系数	焓变/eV	参考文献
1	$ {\text{e}}+{\text{He}} \to {\text{e} + \text{He}} $	f(c, ε)	—	[43]
2	$ {\text{e}}+{\text{He}} \to {\text{e} + \text{H}}{{\text{e}}^ * } $	f(c, ε)	19.82	[43]
3	$ {\text{e}}+{{\text{He}}^ * } \to {\text{e} + \text{He}} $	2.9×10^–15	–19.82	[43]
4	$ {\text{e}}+{\text{He}} \to 2{\text{e} + \text{H}}{{\text{e}}^ + } $	f(c, ε)	24.58	[43]
5	$ {\text{e}}+{{\text{He}}^ * } \to 2{\text{e} + \text{H}}{{\text{e}}^ + } $	4.661×10^–16×T_e^0.6×exp(–4.78/T_e)	4.78	[43]
6	$ {\text{e}}+{\text{He}}_2^ * \to 2{\text{e} + \text{He}}_2^ + $	1.268×10^–18×T_e^0.71×exp(–3.4/T_e)	3.4	[43]
7	$ {\text{e}}+{\text{He}}_2^ + \to {{\text{He}}^ * }+{\text{He}} $	5.386×10^–13×T_e^–0.5	—	[10]
8	$ {\text{e}}+{{\text{He}}^ + } \to {\mathrm{He}}^ * $	6.76×10^–19×T_e^–0.5	—	[10]
9	$ 2{\text{e}} + {{\text{He}}^ + } \to {\text{e}}+{{\text{He}}^ * } $	6.186×10^–39×T_e^–4.4	—	[10]
10	$ {\text{e} + \text{He}}+{{\text{He}}^ + } \to \text{He}+{{\text{He}}^ * } $	6.66×10^–42×T_e^–2	—	[10]
11	$ 2 {\text{e} + \text{He}}_2^ + \to \text{He}_2^ * + {\text{e}} $	1.2×10^–33	—	[10]
12	$ {\text{e} + \text{He} + \text{He}}_2^ + \to \text{He}_2^ * + {\text{He}} $	1.5×10^–39	—	[10]
13	$ {\text{e} + \text{He} + \text{He}}_2^ + \to {\mathrm{He}}^ * + 2 {\text{He}} $	3.5×10^–39	—	[10]
14	$ 2 {\text{e} + \text{He}}_2^ + \to \text{He}^ * +{\text{He} + \text{e}} $	2.8×10^–32	—	[10]
15	$ {\text{e}}+{{\text{N}}_2} \to {\text{e}}+{{\text{N}}_2} $	f(c, ε)	—	[43]
16	$ {\text{e}}+{{\text{N}}_2} \to {\text{e}}+{{\text{N}}_2} $ (v = 1)	f(c, ε)	0.29	[55]
17	$ {\text{e}}+{{\text{N}}_2} \to {\text{e}}+{{\text{N}}_2} $ (v = 2)	f(c, ε)	0.59	[55]
18	$ {\text{e}}+{{\text{N}}_2} \to {\text{e}}+{{\text{N}}_2} $ (v = 3)	f(c, ε)	0.856	[10]
19	$ {\text{e}}+{{\text{N}}_2} \to {\text{e}}+{{\text{N}}_2} $ (v = 4)	f(c, ε)	1.134	[10]
20	$ {\text{e}}+{{\text{N}}_2} \to {\text{e}}+{{\text{N}}_2} $ (v = 5)	f(c, ε)	1.4088	[43]
21	$ {\text{e}}+{{\text{N}}_2} \to 2{\text{e} + \text{N}}_2^ + $	f(c, ε)	15.6	[55]
22	$ {\text{e} + \text{N}}_4^ + \to 2\text{N}_2 $	3.18×10^–13×T_e^–0.5	—	[10]
23	$ {\text{e} + \text{N}}_2^ + \to 2 N $	4.8×10^–13×T_e^–0.5	—	[10]
24	$ {\text{e} + \text{N}}_2^ + \to \text{N}_2 $	7.72×10^–14×T_e^–0.5	—	[10]
25	$ {\text{e}}+{{\text{O}}_2} \to {\text{e}}+{{\text{O}}_2} $	f(c, ε)	—	[55]
26	$ {\text{e}}+{{\text{O}}_2} \to {\mathrm{O}}+{{\text{O}}^ - } $	f(c, ε)	—	[55]
27	$ {\text{e}}+{{\text{O}}_2} \to {\text{e}}+{{\text{O}}_2} $ (v = 3)	f(c, ε)	0.57	[55]
28	$ {\text{e}}+{{\text{O}}_2} \to {\text{e}}+{{\text{O}}_2} $ (v = 4)	f(c, ε)	0.75	[55]
29	$ {\text{e}}+{{\text{O}}_2} \to {\text{e}}+{{\text{O}}_2} $ (a1)	f(c, ε)	0.977	[55]
30	$ {\text{e}}+{{\text{O}}_2} \to {\text{e}}+{{\text{O}}_2} $	f(c, ε)	–0.977	[10]
31	$ {\text{e}}+{{\text{O}}_2} \to {\text{e}}+{{\text{O}}_2} $ (b1)	f(c, ε)	1.627	[55]
32	$ {\text{e}}+{{\text{O}}_2} \to {\text{e}}+{{\text{O}}_2} $	f(c, ε)	–1.627	[10]
33	$ {\text{e}}+{{\text{O}}_2} \to {\text{e}}+{{\text{O}}_2} $ (EXC)	f(c, ε)	4.5	[55]
34	$ {\text{e}}+{{\text{O}}_2} \to {\text{O}}_2^ - $	f(c, ε)	—	[43]
35	$ {\text{e}}+{{\text{O}}_2} \to {\text{e + O + O}} $	f(c, ε)	5.58	[10]
36	$ {\text{e}}+{{\text{O}}_2} \to {\text{e + O + O}} $ (¹D)	f(c, ε)	8.4	[10]
37	$ {\text{e}}+{{\text{O}}_2} \to 2{\text{e} + \text{O}}_2^ + $	f(c, ε)	12.06	[55]
38	$ {\text{e}} + 2{{\text{O}}_2} \to \text{O}_2+{\text{O}}_2^ - $	5.17×10^–43×T_e^–1	–0.43	[43]
39	$ {\text{e} + \text{O}}_2^ + \to 2{\text{O}} $	6×10^–11×T_e^–1	–6.91	[43]
40	$ {\text{e} + \text{O}}_2^ + \to \text{O}_2 $	4×10^–18	—	[43]
41	$ {\text{e} + \text{O}}_4^ + \to 2\text{O}_2 $	2.25×10^–13×T_e^–0.5	—	[10]
42	$ {\text{e}}+{{\text{H}}_2}{\text{O}} \to {\text{e}}+{{\text{H}}_2}{\text{O}} $	f(c, ε)	—	[10]
43	$ {\text{e}}+{{\text{H}}_2}{\text{O}} \to {\text{e + e + }}{{\text{H}}_2}{{\text{O}}^ + } $	f(c, ε)	13.76	[10]
44	$ {\text{e}}+{{\text{H}}_2}{\text{O}} \to {\text{e + H + OH}} $	f(c, ε)	7	[10]
45	$ {\text{e + H + OH}} \to {\text{e}}+{{\text{H}}_2}{\text{O}} $	f(c, ε)	–7	[10]
46	$ {\text{e}}+{{\text{H}}_2}{{\text{O}}^ + } \to {\mathrm{OH}} + {\text{H}} $	6.6×10^–12×T_e^–0.5	—	[10]
47	$ {\text{H}}{{\text{e}}^ * }{\text{ + H}}{{\text{e}}^ * } \to {\text{e + He + H}}{{\text{e}}^ + } $	4.5×10^–16	–15	[10]
48	$ {\text{H}}{{\text{e}}^ * } + 2 {\text{He}} \to {\text{He}}_2^ * +{\text{He}} $	1.3×10^–45	—	[10]
49	$ {\text{H}}{{\text{e}}^ + } + 2 {\text{He}} \to {\text{He}}_2^ + +{\text{He}} $	1×10^–43	—	[10]
50	$ {{\text{O}}^ - }+{\text{O}}_2^ + \to {\mathrm{O}}+{{\text{O}}_2} $	2×10^–13	—	[10]
51	$ {\text{O}}_2^ - +{\text{O}}_2^ + \to 2{{\text{O}}_2} $	2×10^–13	—	[10]
52	$ {\text{O}}_2^ - +{\text{O}}_2^ + +{{\text{O}}_2} \to 3{{\text{O}}_2} $	2×10^–37	—	[10]
53	$ {\text{O}}_2^ - +{\text{O}}_4^ + +{{\text{O}}_2} \to 4{{\text{O}}_2} $	2×10^–37	—	[10]
54	$ {{\text{O}}_2}+{{\text{O}}_2}+{\text{O}}_2^ + \to {{\text{O}}_2}+{\text{O}}_4^ + $	2.4×10^–42	—	[10]
55	$ {\text{H}}{{\text{e}}^ * }+{{\text{N}}_2} \to {\mathrm{e}}{\text{ + N}}_2^ + +{\text{He}} $	7×10^–17	—	[10]
56	$ {\text{He}}_2^ * +{{\text{N}}_2} \to {\mathrm{e}}{\text{ + N}}_2^ + + 2 {\text{He}} $	7×10^–17	—	[10]
57	$ {\text{He}}_2^ * +{{\text{O}}_2} \to {\mathrm{e}}+{\text{O}}_2^ + + 2 {\text{He}} $	3.6×10^–16	—	[10]
58	$ {\text{H}}{{\text{e}}^ * }+{{\text{O}}_2} \to {\mathrm{e}}+{\text{O}}_2^ + +{\text{He}} $	2.6×10^–16	—	[10]
59	$ {\text{He}}_2^ + +{{\text{N}}_2} \to {\mathrm{N}}_2^ + + 2 {\text{He}} $	5×10^–16	—	[10]
60	$ {\text{H}}{{\text{e}}^ + }+{{\text{N}}_2} \to {\mathrm{N}}_2^ + +{\text{He}} $	5×10^–16	—	[10]
61	$ {\text{He + }}{{\text{N}}_2}{\text{ + N}}_2^ + \to \text{He}{\text{ + N}}_4^ + $	8.9×10^–42	—	[10]
62	$ {\text{He + }}{{\text{O}}_2}+{\text{O}}_2^ + \to {\mathrm{He}}+{\text{O}}_4^ + $	5.8×10^–43	—	[10]
63	$ {\text{O + O + N}} \to \text{O}_2 + {\text{N}} $	3.2×10^–45	—	[10]
64	$ {{\text{O}}_2}{\text{ + N + N}} \to \text{O}_2+{{\text{N}}_2} $	3.9×10^–45	—	[10]
65	$ {{\text{O}}_2}{\text{ + N}}_4^ + \to 2\text{N}_2+{\text{O}}_2^ + $	2.5×10^–16	—	[43]
66	$ {{\text{N}}_2}+{{\text{O}}_2}{\text{ + N}}_2^ + \to \text{O}_2{\text{ + N}}_4^ + $	5×10^–41	—	[10]
67	$ {\text{O}}_2^ - +{\text{O}}_4^ + +{{\text{N}}_2} \to 3\text{O}_2+{{\text{N}}_2} $	2×10^–37	—	[10]
68	$ {\text{O}}_2^ - +{\text{O}}_2^ + +{{\text{N}}_2} \to 2\text{O}_2+{{\text{N}}_2} $	2×10^–37	—	[10]
69	$ {\text{O}}_2^ - +{\text{O}}_2^ + + {\text{He}} \to 2\text{O}_2 + {\text{He}} $	2×10^–37	—	[10]
70	$ {\text{He + O + H}} \to \text{He}{\text{ + OH}} $	3.2×10^–45×T^–1	—	[10]
71	$ {\text{O + 2}}{{\text{O}}_2} \to {\mathrm{O}}_3+{{\text{O}}_2} $	6×10^–46×(T/300)^–2.8	—	[56]
72	$ 2 {\text{O}} + {{\text{O}}_2} \to {{\mathrm{O}}_3}+{\text{O}} $	3.4×10^–46×(T/300)^–1.2	—	[56]
73	$ {\text{O + }}{{\text{O}}_2}+{{\text{N}}_2} \to \text{N}_2+{{\text{O}}_3} $	1.1×10^–46×exp(510/T)	—	[56]
74	$ {\text{O + }}{{\text{O}}_2}+{\text{He}} \to \text{He}+{{\text{O}}_3} $	3.4×10^–46×(T/300)^–1.2	—	[56]
75	$ {{\text{O}}_3}+{\text{O}} \to 2{{\text{O}}_2} $	8×10^–18×exp(–2060/T)	—	[56]
76	$ {2}{{\text{O}}_3} \to {\text{O + }}{{\text{O}}_2}+{{\text{O}}_3} $	1.6×10^–15×exp(–11400/T)	—	[56]
77	$ {{\text{O}}_3}+{{\text{N}}_2} \to {\text{O}} + {{\text{O}}_2}+{{\text{N}}_2} $	1.6×10^–15×exp(–11400/T)	—	[56]
78	$ {\text{He}} + {{\text{O}}_3} \to \text{He} + {\text{O}} + {{\text{O}}_2} $	1.56×10^–15×exp(–11400/T)	—	[56]
注: f(c, ε)代表该反应的速率系数是使用碰撞横截面与电子能的函数和电子能量分布函数计算得到的; T_e为电子温度, 单位为eV; He^代表He(2³S)和He(2¹S); He₂^代表He₂(a³Σ_u⁺); N₂代表N₂(v = 1), N₂(v = 2), N₂(v = 3), N₂(v = 4)和N₂(v = 5); O₂代表O₂(v = 3), O₂(v = 4), O₂(a1), O₂(b1)和O₂(EXC); O代表O(¹D); 双体和三体反应的速率系数单位分别为m³·s^–1和m⁶·s^–1[10,43].

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Influence of surface-adhered water droplets on discharge characteristics and chemical species distribution in atmospheric-pressure helium dielectric barrier discharge system

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Influence of surface-adhered water droplets on discharge characteristics and chemical species distribution in atmospheric-pressure helium dielectric barrier discharge system

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