Comparative study on discharge characteristics of low pressure CO<sub>2</sub> driven by sinusoidal AC voltage: DBD and bare electrode structure

Fu Qiang; Wang Cong; Wang Yu-Fei; Chang Zheng-Shi

doi:10.7498/aps.71.20220086

Abstract

The low-pressure atmosphere rich in CO₂ (~95%) on Mars makes the in-situ resource utilization of Martian CO₂ and the improvement of oxidation attract widespread attention. It contributes to constructing the Mars base which will support the deep space exploration. Conversion of CO₂ based on high voltage discharge has the advantages of environmental friendliness, high efficiency and long service life. It has application potential in the in-situ conversion and utilization of Martian CO₂ resources. We simulate the CO₂ atmosphere of Mars where the pressure is fixed at 1 kPa and the temperature is maintained at room temperature. A comparative study is carried out on the discharge characteristics of two typical electrode structures (with/without barrier dielectric) driven by 20 kHz AC voltage. Combined with numerical simulations, the CO₂ discharge characteristics, products and their conversion pathways are analyzed. The results show that the discharge mode changes from single discharge during each half cycle into multi discharge pulses after adding the barrier dielectric. Each discharge pulse of the multi pulses corresponds to a random discharge channel, which is induced by the distorted electric field of accumulated charge on the dielectric surface and the space charge. The accumulated charge on the dielectric surface promotes the primary discharge and inhibits the secondary discharge. Space charge will be conducive to the occurrence of secondary discharge. The main products in discharge process include ${\rm{CO}}^+_2 $, CO, O₂, C, and O. Among the products, CO is produced mainly by the attachment decomposition reaction between energetic electrons and CO₂ at the boundary of cathode falling zone, and the contribution rate of the reaction can reach about 95%. The O₂ is generated mainly by the compound decomposition reaction between electrons and ${\rm{CO}}^+_2 $ near the instantaneous anode surface or instantaneous anode side dielectric surface, and the contribution rate of the reaction can reach about 98%. It is further found that the dielectric does not change the generation position nor dominant reaction pathway of the two main products, but will reduce the electron density from 5.6×10¹⁶ m⁻³ to 0.9×10¹⁶ m⁻³ and electron temperature from 17.2 eV to 11.7 eV at the boundary of the cathode falling region, resulting in the reduction of CO production. At the same time, the deposited power is reduced, resulting in insufficient $ {\rm{CO}}^+_2 $ yield near the instantaneous anode surface and instantaneous anode side dielectric surface and further the decrease of O₂ generation.

Keywords:

Authors and contacts

1.
School of Electrical Engineering, Xi’an Jiaotong University, Xi’an 710049, China
2.
Linyi Power Supply Company, State Grid Shandong Electric Power Company, Linyi 276000, China

Corresponding author: Chang Zheng-Shi, changzhsh1984@163.com

Funds: Project supported by the Fundamental Research Funds for the Central Universities of Ministry of Education of China (Grant No. xzy012021014), the Beijing Institute of Spacecraft Environment Engineering Innovation Fund, China (Grant No. CAST-BISEE2019-021), and the Beijing Institute of Aerospace Systems Engineering Innovation Fund, China (Grant No. CALTJS2017-0031).

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Cited By

图 1 平行板电极实验装置图　(a) 裸电极型; (b) DBD型

Figure 1. Diagram of parallel plate electrode: (a) Bare copper electrode; (b) copper electrode with dielectric barrier.

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图 2 CO₂放电转化特性检测平台

Figure 2. Platform of CO₂ discharge characteristic detection.

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图 3 4 mm间隙不同电极结构CO₂放电电流波形　(a) 裸电极结构; (b) DBD结构

Figure 3. CO₂ discharge current waveforms with different electrode structures when d = 4 mm: (a) Bare copper electrode; (b) copper electrode with dielectric barrier.

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图 4 DBD不同放电电流脉冲的放电图像

Figure 4. Discharge images of different current pulses in DBD.

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图 5 DBD放电参数分布

Figure 5. Distribution of discharge parameters in DBD.

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图 6 270—620 nm发射光谱

Figure 6. Optical emission spectra ranging from 270 to 620 nm

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图 7 270—570 nm裸电极与DBD发射光谱对比

Figure 7. Comparison of discharge optical spectra between copper electrode and DBD structure: 270–570 nm.

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图 8 750—900 nm裸电极与DBD发射光谱对比:

Figure 8. Comparison of discharge optical spectra between copper electrode and DBD structure: 750–900 nm.

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图 9 模型中CO和O₂不同产生路径的贡献　(a) CO; (b) O₂

Figure 9. Contribution of different production paths of CO and O₂ in model: (a) CO; (b) O₂.

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图 10 反应路径E9和E23在稳定周期下的反应速率

Figure 10. Reaction rate of path E9 and E23 at stable period.

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图 C1 270—620 nm发射光谱

Figure C1. Optical spectra ranging from 270 to 620 nm.

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图 C2 750—900 nm发射光谱

Figure C2. Optical spectra ranging from 750 to 900 nm.

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图 C3 200—280 nm裸电极发射光谱

Figure C3. Emission spectrum of bare copper electrode: 200–280 nm.

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图 D1 4 mm间隙裸电极放电峰值时刻n_e, n_i, E和T_e分布　(a) 正放电; (b)负放电

Figure D1. Distribution of n_e, n_i, E and T_e at the peak time of discharge current of bare electrode when d = 4 mm: (a) Positive discharge; (b) negative discharge.

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图 D2 4 mm间隙DBD正放电放电峰值时刻n_e, n_i, E和T_e分布　(a)第1个脉冲; (b)第2个脉冲

Figure D2. Distribution of n_e, n_i, E and T_e at the peak time of positive discharge current of DBD when d = 4 mm: (a) First pulse; (b) second pulse.

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表 1 模型中包括的粒子

Table 1. Types of particles included in the model.

中性粒子	CO₂, CO, O, C, O₂
离子	CO${}^+_2 $, O^–, O${}^+_2 $, O${}^-_2 $, CO${}^-_3 $
激发态粒子	CO₂e, CO₂v1, CO₂v2, CO₂v3, CO₂v4

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表 2 模型中考虑的振动态

Table 2. Vibrational particles considered in the model.

基态	模型中的符号	对应振动态
CO₂	CO₂v1	(010)
	CO₂v2	(100), (020)
	CO₂v3	(001)
	CO₂v4	(n00), (0n0)

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表 3 模型中裸电极与DBD放电参数和产物对比

Table 3. Comparison of discharge parameters and products in model: bare copper electrode & DBD.

放电参数和产物	裸电极	DBD
功率/W	1.0	0.06
电子密度/m^–3	1.1 × 10¹⁶	3.6 × 10¹⁵
振动态密度和/m^–3	1.0 × 10²¹	3.1 × 10¹⁹
CO密度/m^–3	2.2 × 10¹⁷	7.0 × 10¹⁵
O₂密度/m^–3	8.8 × 10¹⁶	2.7 × 10¹⁵
O密度/m^–3	4.2 × 10¹⁶	1.5 × 10¹⁵
C密度/m^–3	3.5 × 10¹⁵	6.3 × 10¹⁴

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表 B2 模型中的电子附着反应和电子-离子复合反应

Table B2. Electron attachment reactions and electron-ion recombination reactions in the model.

序号	反应	速率系数	参考文献
E22	e + CO${}_2^+ $ → CO + O	2.0 × 10^–11T_e^–0.5/T_g	[35]
E23	e + CO${}_2^+ $ → C + O₂	3.94 × 10^–13T_e^–0.4	[36]
E24	e + O${}_2^+ $ → O + O	6.0 × 10^–13T_e^–0.5T_g^–0.5	[35]
E25	e + O₂ + M → M + O${}_2^- $	3.0 × 10^–42(M = CO₂)	[37]
E25	e + O₂ + M → M + O${}_2^- $	2.0 × 10^–42(M = CO, O₂)	[37]
E26	e + O + M → M + O^–	1.0 × 10^–43	[37]
E27	e + O${}_2^+ $ + M → M + O₂	1.0 × 10^–38	[31, 38]

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表 B3 模型中的离子-中性粒子反应和离子-离子反应

Table B3. Ion-neutral particle reactions and ion-ion reactions in the model.

序号	反应	速率系数	参考文献
I1	O^– + CO₂ +M→ CO${}_3^- $ + M	9.0 × 10^–41 (M = CO₂)	[35, 39]
I1	O^– + CO₂ +M→ CO${}_3^- $ + M	3.0 × 10^–40 (M = CO, O₂)	[35, 39]
I2	O^– + CO → CO₂ + e	5.5 × 10^–16	[36]
I3	CO${}_3^- $ + CO → CO₂ + CO₂ + e	5.0 × 10^–19	[35]
I4	O^– + M → O + M + e	4.0 × 10^–18	[39]
I5	O^– + O → O₂ + e	2.3 × 10^–16	[40]
I6	O${}_2^- $ + CO${}_2^+ $ → CO + O₂ + O	6.0 × 10^–13	[35]
I7	O + CO${}_2^+ $ → CO + O${}_2^+ $	1.64 × 10^–16	[31, 41]
I8	O₂ + CO${}_2^+ $ → CO₂ + O${}_2^+ $	5.3 × 10^–17	[31, 41]
I9	CO${}_3^- $ + CO${}_2^+ $ → CO₂ + CO₂ + O	5.0 × 10^–13	[35]
I10	CO${}_3^- $ + O${}_2^+ $ → CO₂ + O₂ + O	3.0 × 10^–13	[35]
I11	CO${}_3^- $ + O → CO₂ + O${}_2^- $	8.0 × 10^–17	[35]
I12	O${}_2^- $ + O${}_2^+ $ → O₂ + O₂	2.0 × 10^–13	[40]
I13	O${}_2^- $ + O${}_2^+ $ → O + O + O₂	4.2 × 10^–13	[35]
I14	O${}_2^- $ + O${}_2^+ $ + M → O₂ + O₂ + M	2.0 × 10^–37	[38]
I15	O^– + O${}_2^+ $ → O + O₂	1.0 × 10^–13	[35]
I16	O^– + O${}_2^+ $ → O + O + O	2.6 × 10^–14	[40]
I17	O${}_2^- $ + O → O^– + O₂	3.3 × 10^–16	[38]
I18	O${}_2^- $ + O₂ → O₂ + O₂ +e	2.18 × 10^–24	[38]
I19	O${}_2^- $ +M → O₂ + M +e	2.7 × 10^–16(T_g/300)^0.5exp(–5590/T_g)	[36]

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表 B4 模型中中性粒子之间的反应

Table B4. Reactions between neutral particles in the model.

序号	反应	速率系数	α	参考文献
N1	CO₂ +M → CO + O + M	3.91 × 10^–16exp(–49430/T_g)	0.8	[31]
N2	CO₂ + O → CO + O₂	2.8 × 10^–17exp(–26500/T_g)	0.5	[31, 36]
N3	CO₂ + C→ CO + CO	1.0 × 10^–21	—	[39]
N4	O + CO +M → CO₂ + M	1.6 × 10^–45exp(–1510/T_g) (M=CO₂)		[37]
N4	O + CO +M → CO₂ + M	8.2 × 10^–46exp(–1510/T_g) (M=CO, O₂)		[37]
N5	O + C +M → CO + M	2.14 × 10^–41(T_g/300)^–3.08exp(–2114/T_g)		[36]
N6	O + O +M → O₂ + M	1.27 × 10^–44(T_g/300)^–1exp(–170/T_g)		[42]
N7	O₂ + CO → CO₂ + O	4.2 × 10^–18exp(–24000/T_g)		[36]
N8	O₂ + C → CO + O	3.0 × 10^–17		[37]

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表 B5 模型中的振动能量传递反应

Table B5. Vibration energy transfer reactions in the model.

序号	反应	速率系数	参考文献
V1	CO₂v1 + CO₂ → CO₂ + CO₂	7.14 × 10^–14exp(–177 T_g^–1/3+451 T_g^–2/3)	[43]
V2	CO₂v1 + CO → CO + CO₂	0.7 × 7.14 × 10^–14exp(–177 T_g^–1/3+451 T_g^–2/3)	[43]
V3	CO₂v1 + O₂ → O₂ + CO₂	0.7 × 7.14 × 10^–14exp(–177 T_g^–1/3+451 T_g^–2/3)	[43]
V4	CO₂v2 + CO₂ → CO₂ + CO₂	1.071 × 10^–15exp(–137 T_g^–1/3)	[43]
V5	CO₂v2 + CO → CO + CO₂	3.1 × 1.071 × 10^–15exp(–137 T_g^–1/3)	[43]
V6	CO₂v2 + O₂ → O₂ + CO₂	3.1 × 1.071 × 10^–15exp(–137 T_g^–1/3)	[43]
V7	CO₂v2 + CO₂ → CO₂ + CO₂v1	1.942 × 10^–13exp(–177 T_g^–1/3+451 T_g^–2/3)	[43]
V8	CO₂v2 + CO → CO + CO₂v1	0.7 × 1.942 × 10^–13exp(–177 T_g^–1/3+451 T_g^–2/3)	[43]
V9	CO₂v2 + O₂ → O₂ + CO₂v1	0.7 × 1.942 × 10^–13exp(–177 T_g^–1/3+451 T_g^–2/3)	[43]
V10	CO₂v3 + CO₂ → CO₂ + CO₂v2	8.57 × 10^–7exp(–404 T_g^–1/3+1096 T_g^–2/3)	[43]
V11	CO₂v3 + CO → CO + CO₂v2	0.3 × 8.57 × 10^–7exp(–404 T_g^–1/3+1096 T_g^–2/3)	[43]
V12	CO₂v3 + O₂ → O₂ + CO₂v2	0.4 × 8.57 × 10^–7exp(–404 T_g^–1/3+1096 T_g^–2/3)	[43]
V13	CO₂v3 + CO₂ → CO₂ + CO₂v4	1.431 × 10^–11exp(–252 T_g^–1/3+685 T_g^–2/3)	[43]
V14	CO₂v3 + CO → CO + CO₂v4	0.3 × 1.431 × 10^–11exp(–252 T_g^–1/3+685 T_g^–2/3)	[43]
V15	CO₂v3 + O₂ → O₂ + CO₂v4	0.4 × 1.431 × 10^–11exp(–252 T_g^–1/3+685 T_g^–2/3)	[43]
V16	CO₂v3 + CO₂ → CO₂v1 + CO₂v2	1.06 × 10^–11exp(–242 T_g^–1/3+633 T_g^–2/3)	[43]
V17	CO₂v3 + CO₂ → CO₂ + CO₂v1	4.25 × 10^–7exp(–407 T_g^–1/3+824 T_g^–2/3)	[43]
V18	CO₂v3 + CO → CO + CO₂v1	0.3 × 4.25 × 10^–7exp(–407 T_g^–1/3+824 T_g^–2/3)	[43]
V19	CO₂v3 + O₂ → O₂ + CO₂v1	0.4 × 4.25 × 10^–7exp(–407 T_g^–1/3+824 T_g^–2/3)	[43]
V20	CO₂v4 + CO₂ → CO₂ + CO₂v2	2.897 × 10^–13exp(–177 T_g^–1/3+451 T_g^–2/3)	[43]
V21	CO₂v4 + CO → CO + CO₂v2	0.7 × 2.897 × 10^–13exp(–177 T_g^–1/3+451 T_g^–2/3)	[43]
V22	CO₂v4 + O₂ → O₂ + CO₂v2	0.7 × 2.897 × 10^–13exp(–177 T_g^–1/3+451 T_g^–2/3)	[43]
V23	CO₂v4 + CO₂ → CO₂ + CO₂v1	1.071 × 10^–15exp(–137 T_g^–1/3)	[43]
V24	CO₂v4 + CO → CO + CO₂v1	3.1 × 1.071 × 10^–15exp(–137 T_g^–1/3)	[43]
V25	CO₂v4 + O₂ → O₂ + CO₂v1	3.1 × 1.071 × 10^–15exp(–137 T_g^–1/3)	[43]

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表 B1 模型中的电子碰撞反应

Table B1. Electron impact reactions in the model.

序号	反应	速率系数	参考文献
E1	e + CO₂ → e + CO₂	f (σ)	[32]
E2	e + CO₂vi → e + CO₂vi	f (σ)	[32]
E3	e + CO₂ → 2e + CO${}_2^+ $	f (σ)	[32]
E4	e + CO₂vi → 2e + CO${}_2^+ $	f (σ)	[32]
E5	e + CO₂ → e + CO₂e	f (σ)	[32]
E6	e + CO₂vi → e + CO₂e	f (σ)	[32]
E7	e + CO₂ → e + O + CO	f (σ)	[32]
E8	e + CO₂vi → e + O + CO	f (σ)	[32]
E9	e + CO₂ → O^– + CO	f (σ)	[32]
E10	e + CO₂vi → O^– + CO	f (σ)	[32]
E11	e + CO₂ → e + CO₂v1	f (σ)	[32]
E12	e + CO₂ → e + CO₂v2	f (σ)	[32]
E13	e + CO₂ → e + CO₂v3	f (σ)	[32]
E14	e + CO₂ → e + CO₂v4	f (σ)	[32]
E15	e + CO → e + CO	f (σ)	[33]
E16	e + CO → e + C + O	f (σ)	[33]
E17	e + CO → C + O^–	f (σ)	[33]
E18	e + O₂ → e + O₂	f (σ)	[34]
E19	e + O₂ → e + O + O	f (σ)	[34]
E20	e + O₂ → O + O^–	f (σ)	[34]
E21	e + O₂ → 2e + O${}_2^+ $	f (σ)	[34]

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表 C3 CO(A¹Π→X¹Σ)第四正带系的光谱参数

Table C3. Spectral parameters of the fourth positive band system of CO(A¹Π→X¹Σ).

波长/nm	振动能级(ν'→ν'')	Δν
200.5	1→8	7
208.9	5→12	7
221.6	3→12	9
224.7	8→16	8
228.6	6→15	9
235.6	5→15	10

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表 C4 CO⁺(B²Σ⁺→X²Σ⁺)第一负带系的光谱参数

Table C4. Spectral parameters of the first negative band system of CO⁺(B²Σ⁺→X²Σ⁺).

波长/nm	振动能级(ν'→ν'')	Δν
244.5	1→3	2
247.4	2→4	2
253.0	4→6	2
257.7	1→4	3

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表 C1 CO(b³Σ→a³Π)第三正带系的光谱参数

Table C1. Spectral parameters of the third positive band system of CO(b³Σ→a³Π).

波长/nm	振动能级(ν'→ν'')	Δν
283	0→0	0
297	0→1	1
313	0→2	2

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表 C2 CO(B¹Σ→A¹Π)Angstrom系的光谱参数

Table C2. Spectral parameters of the Angstrom system of CO(B¹Σ→A¹Π).

波长/nm	振动能级(ν'→ν'')	Δν
451	0→0	0
483	0→1	1
520	0→2	2
561	0→3	3
608	0→4	4

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Comparative study on discharge characteristics of low pressure CO₂ driven by sinusoidal AC voltage: DBD and bare electrode structure

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Comparative study on discharge characteristics of low pressure CO2 driven by sinusoidal AC voltage: DBD and bare electrode structure

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Comparative study on discharge characteristics of low pressure CO₂ driven by sinusoidal AC voltage: DBD and bare electrode structure