纳秒脉冲液相放电耦合微气泡固氮影响因素分析

doi:10.19595/j.cnki.1000-6753.tces.221939

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摘要由气液等离子体放电产生的活化水富含活性氧和活性氮（$\text{NO}_{\text{2}}^{-}$、$\text{NO}_{\text{3}}^{-}$、H₂O₂、O₃等）,在环境治理、材料合成和医疗卫生等领域有着广泛的应用前景。该文提出了一种“多微孔-同轴式”的微气泡等离子体放电结构,微孔和微气泡的引入降低了在液相中的击穿场强,并且微气泡增加了气液界面的化学反应和活性物质的溶解。以空气为放电气体,主要探究了正、负极性脉冲参数对活化水固氮特性的影响。此外,还考察了气体流速、温度等因素对活化水中的氮特性的影响,并诊断了电学特性。结果表明,正极性放电下$\text{NO}_{\text{2}}^{-}$产量和$\text{NO}_{\text{3}}^{-}$产量分别为7.2 mg、28.8 mg,相比负极性放电分别高出0.43 mg、3 mg,经计算正极性放电能量效率高达15.02 g/(kW·h)。同时研究发现,当气流流速为2 L/min时,固氮性能最佳;水温越高,氮含量会随着液相分解动力学温度的降低而减弱。

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关键词 ：纳秒脉冲放电, 微气泡, 等离子体, 固氮

Abstract：Plasma-activated water produced by gas-liquid plasma discharge is rich in reactive oxygen species and reactive nitrogen, and it has a wide application prospect in the fields of environmental treatment, material synthesis, and medical health. However, how quickly preparing large volumes and high concentrations of activated water of RNOS is still a difficult problem, and the design of a gas-liquid plasma reactor is one of the key factors to solve this problem. In order to solve these problems, this paper designed a "multi-microporous coaxial" microbubble plasma reactor, which uses multi-microporous microbubbles to reduce the breakdown field strength of the liquid phase, and forms multi-spark discharge channels in the liquid phase, so that rich active oxygen and nitrogen can be generated in the liquid phase. Under the excitation of nanosecond pulses, the factors influencing the nitrogen fixation of microbubbles by coupling nanosecond pulse liquid discharge in a microbubble plasma reactor were investigated.
Firstly, this paper explored the influence of positive and negative pulse parameters on the nitrogen fixation characteristics of activated water. The results showed that the output of $\text{NO}_{\text{2}}^{-}$ and $\text{NO}_{\text{3}}^{-}$ under positive discharge was 7.2 mg and 28.8 mg respectively. Because of the voltage polarity effect and the different development of positive and negative currents, the output of $\text{NO}_{\text{2}}^{-}$ and $\text{NO}_{\text{3}}^{-}$ were 0.43 mg and 3 mg higher than that of negative discharge, respectively. The energy efficiency of positive discharge was calculated to be 15.02 g/(kW·h). At the same time, it was found that the airflow rate affected the nitrogen fixation efficiency, and the best flow rate for nitrogen fixation performance was 2 L/min. In addition, nitrogen fixation efficiency is also affected by water temperature. In this paper, the lower the water temperature is, the higher the nitrogen fixation efficiency is. Because the solubility of oxygen and other gases will decrease with the increase in temperature, affecting the process of N₂ and O₂ discharging to generate NO_x. Secondly, this paper measured the plasma emission spectrum during discharge, analyzed the physical and chemical reactions at the gas-liquid interface according to spectral characteristics, and deduced the reaction path of nitrogen and oxygen. The physical and chemical characteristics of activated water during the discharge were investigated. It was known that the generation of active substances in the gas and liquid phases was also an accumulation process. The liquid phase spark discharge produced a large number of active particles to dissolve the water, resulting in a decrease in the pH of the solution, an increase in ORP, and an increase in conductivity. The water temperature rises about 5℃ due to the "hydroelectric effect". Finally, the analysis of electrical characteristics showed that microbubbles and micropores distort the electric field in the liquid phase, making the liquid phase discharge more likely to occur.
The following conclusions can be drawn from the analysis: (1) The microbubble coupled plasma discharge device is designed, which can continuously generate microbubbles and reduce the breakdown field strength; and it can also reduce the loss of metal electrodes and discharge in the liquid with high conductivity, forming a multi-electrode spark discharge channel. (2) The nitrogen fixation efficiency of positive discharge is higher than that of negative discharge. The main reason is that the voltage polarity effect is different from the development of positive and negative currents. (3) The nitrogen fixation efficiency of the activated water increases with time, but it is lost in the form of heat energy due to the polarity effect during discharge. Setting a lower water temperature can reduce the energy loss due to heat during discharge, and the number of active particles generated is higher. This paper provides a new way for the nitrogen fixation model.

Key words： Nanosecond pulsed discharge microbubbles plasma nitrogen fixation

收稿日期: 2022-10-09

PACS:

TM215

基金资助:国家自然科学基金资助项目（52022096, 52177164）

通讯作者: 章程男,1982年生,博士,研究员,研究方向为高电压与等离子体技术。E-mail：zhangcheng@mail.iee.ac.cn

作者简介: 邝勇男,1997年生,硕士研究生,研究方向为放电等离子体。E-mail：kuangyong@mail.iee.ac.cn

引用本文:

邝勇, 章程, 胡修翠, 任晨华, 陈根永, 邵涛. 纳秒脉冲液相放电耦合微气泡固氮影响因素分析[J]. 电工技术学报, 2023, 38(15): 3960-3971. Kuang Yong, Zhang Cheng, Hu Xiucui, Ren Chenhua, Chen Genyong, Shao Tao. Factors Influencing Nitrogen Fixation by Microbubbles Coupled with Nanosecond-Pulse Liquid Phase Discharges. Transactions of China Electrotechnical Society, 2023, 38(15): 3960-3971.

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[1] 邵涛, 严萍. 大气压气体放电及其等离子体应用[M]. 北京: 科学出版社, 2015.
[2] 戴栋, 宁文军, 邵涛. 大气压低温等离子体的研究现状与发展趋势[J]. 电工技术学报, 2017, 32(20): 1-9.
Dai Dong, Ning Wenjun, Shao Tao.A review on the state of art and future trends of atmospheric pressure low temperature plasmas[J]. Transactions of China Electrotechnical Society, 2017, 32(20): 1-9.
[3] 赵鸣鸣, 于维鑫, 孔飞, 等. 基于二元布气的大气压等离子体沉积TiO₂功能层提高陶瓷表面绝缘性能[J]. 电工技术学报, 2022, 37(13): 3404-3412.
Zhao Mingming, Yu Weixin, Kong Fei, et al.Improvement of surface insulating properties of ceramics by deposition of TiO₂ functional layer by atmospheric pressure plasma with binary gas distribution[J]. Transactions of China Electrotechnical Society, 2022, 37(13): 3404-3412.
[4] 黑雪婷, 高远, 窦立广, 等. 纳秒脉冲介质阻挡放电等离子体驱动CH₄-CH₃OH转化制备液态化学品的特性研究[J]. 电工技术学报, 2022, 37(15): 3941-3950.
Hei Xueting, Gao Yuan, Dou Liguang, et al.Study on plasma enhanced CH₄-CH₃OH conversion to liquid chemicals by nanosecond pulsed dielectric barrier discharge[J]. Transactions of China Electrotechnical Society, 2022, 37(15): 3941-3950.
[5] 杨波, 仲崇山, 王维洲, 等. 等离子体活性水用于农业领域的研究进展[J]. 农业工程, 2019, 9(2): 101-107.
Yang Bo, Zhong Chongshan, Wang Weizhou, et al.Research progress of plasma activated water used in agriculture[J]. Agricultural Engineering, 2019, 9(2): 101-107.
[6] 徐晗, 陈泽煜, 刘定新. 大气压冷等离子体处理水溶液:液相活性粒子检测方法综述[J]. 电工技术学报, 2020, 35(17): 3561-3582.
Xu Han, Chen Zeyu, Liu Dingxin.Aqueous solutions treated by cold atmospheric plasmas: a review of the detection methods of aqueous reactive species[J]. Transactions of China Electrotechnical Society, 2020, 35(17): 3561-3582.
[7] 蔡勇, 梁闯, 罗勇, 等. 气液冷等离子体多相反应器基础研究与应用进展[J]. 化工学报, 2019, 70(10): 3847-3858.
Cai Yong, Liang Chuang, Luo Yong, et al.Fundamental study and application progress in gas-liquid non-thermal plasma multiphase reactors[J]. CIESC Journal, 2019, 70(10): 3847-3858.
[8] 邵涛, 章程, 王瑞雪, 等. 大气压脉冲气体放电与等离子体应用[J]. 高电压技术, 2016, 42(3): 685-705.
Shao Tao, Zhang Cheng, Wang Ruixue, et al.Atmospheric-pressure pulsed gas discharge and pulsed plasma application[J]. High Voltage Engineering, 2016, 42(3): 685-705.
[9] Machala Z, Tarabová B, Sersenová D, et al.Chemical and antibacterial effects of plasma activated water: correlation with gaseous and aqueous reactive oxygen and nitrogen species, plasma sources and air flow conditions[J]. Journal of Physics D: Applied Physics, 2019, 52(3): 034002.
[10] Kutasi K, Popović D, Krstulović N, et al.Tuning the composition of plasma-activated water by a surface-wave microwave discharge and a kHz plasma jet[J]. Plasma Sources Science and Technology, 2019, 28(9): 095010.
[11] Terebun P, Kwiatkowski M, Hensel K, et al.Influence of plasma activated water generated in a gliding arc discharge reactor on germination of beetroot and carrot seeds[J]. Applied Sciences, 2021, 11(13): 6164.
[12] Fang Haiqin, Zhang Cheng, Sun Ao, et al.Effect of reactive chemical species on the degradation of deoxynivalenol, 3-acetyldeoxynivalenol, and 15-acetyldeoxynivalenol in low-temperature plasmas[J]. ACS Food Science & Technology, 2022, 2(3): 558-567.
[13] 满晨曦, 黄邦斗, 章程, 等. 不同脉冲参数下等离子体活化水活性氮特性[J]. 高电压技术, 2022, 48(6): 2326-2335.
Man Chenxi, Huang Bangdou, Zhang Cheng, et al.Reactive nitrogen species characteristic of plasma-activated water under different pulsed parameters[J]. High Voltage Engineering, 2022, 48(6): 2326-2335.
[14] Sun Jing, Alam D, Daiyan R, et al.A hybrid plasma electrocatalytic process for sustainable ammonia production[J]. Energy & Environmental Science, 2021, 14(2): 865-872.
[15] Liu Zhijie, Gao Yuting, Pang Bolun, et al.Comparison of the physicochemical properties and inactivation against tumor cells of PAW induced by underwater single-hole and multi-hole bubble plasma[J]. Journal of Physics D: Applied Physics, 2022, 55(29): 095202.
[16] Oh J S, Szili E J, Gaur N, et al.How to assess the plasma delivery of RONS into tissue fluid and tissue[J]. Journal of Physics D: Applied Physics, 2016, 49(30): 304005.
[17] Gromov M, Leonova K, de Geyter N, et al. N₂ oxidation kinetics in a ns-pulsed discharge above a liquid electrode[J]. Plasma Sources Science and Technology, 2021, 30(6): 065024.
[18] Pang Bolun, Liu Zhijie, Zhang Huaiyan, et al.Investigation of the chemical characteristics and anticancer effect of plasma-activated water: the effect of liquid temperature[J]. Plasma Processes and Polymers, 2022, 19(1): e2100079.
[19] 童得恩, 朱鑫磊, 邹晓兵, 等. 水中放电预加热过程的数值模拟研究[J]. 高电压技术, 2019, 45(5): 1461-1467.
Tong De’en, Zhu Xinlei, Zou Xiaobing, et al.Numerical simulation of the preheating process of pulse discharge in water[J]. High Voltage Engineering, 2019, 45(5): 1461-1467.
[20] Li X D, Liu Y, Zhou G, et al.Subsonic streamers in water: initiation, propagation and morphology[J]. Journal of Physics D: Applied Physics, 2017, 50(25): 255301.
[21] Hamdan A, Ridani D A, Diamond J, et al.Pulsed nanosecond air discharge in contact with water: influence of voltage polarity, amplitude, pulse width, and gap distance[J]. Journal of Physics D: Applied Physics, 2020, 53(35): 355202.
[22] 温嘉烨, 李元, 倪正全, 等. 水中负极性灌木状放电特性研究[J]. 中国电机工程学报, 2021, 41(17): 6108-6116.
Wen Jiaye, Li Yuan, Ni Zhengquan, et al.Study on characteristics of negative bushy discharges in water[J]. Proceedings of the CSEE, 2021, 41(17): 6108-6116.
[23] Shu Zhan, Wang Chuanqi, Hossain I, et al.Preliminary study of an open-air water-contacting discharge for direct nitrogen fixation[J]. Plasma Science and Technology, 2021, 23(3): 95-103.
[24] Wu S, Thapa B, Rivera C, et al.Nitrate and nitrite fertilizer production from air and water by continuous flow liquid-phase plasma discharge[J]. Journal of Environmental Chemical Engineering, 2021, 9(2): 104761.
[25] Martynov S B, Porter R T J, Mahgerefteh H. Henry’s law constants and vapor-liquid distribution coefficients of noncondensable gases dissolved in carbon dioxide[J]. ACS Omega, 2022, 7(10): 8777-8788.
[26] Aquilanti V, Coutinho N D, Carvalho-Silva V H. Kinetics of low-temperature transitions and a reaction rate theory from non-equilibrium distributions[J]. Philosophical Transactions Series A, Mathematical, Physical, and Engineering Sciences, 2017, 375(2092): 20160201.
[27] 张梦瑶, 温嘉烨, 李元, 等. 气液混相水中脉冲放电过氧化氢生成规律的研究[J]. 高电压技术, 2019, 45(12): 4130-4136.
Zhang Mengyao, Wen Jiaye, Li Yuan, et al.Study on hydrogen peroxide formation during pulsed discharge in gas-liquid mixed phase[J]. High Voltage Engineering, 2019, 45(12): 4130-4136.
[28] Xu Zimu, Cheng Cheng, Shen Jie, et al.In vitro antimicrobial effects and mechanisms of direct current air-liquid discharge plasma on planktonic Staphylococcus aureus and Escherichia coli in liquids[J]. Bioelectrochemistry, 2018, 121: 125-134.
[29] Traylor M J, Pavlovich M J, Karim S, et al.Long-term antibacterial efficacy of air plasma-activated water[J]. Journal of Physics D: Applied Physics, 2011, 44(47): 472001.
[30] Šimečková J, Krčma F, Klofáč D, et al.Influence of plasma-activated water on physical and physical-chemical soil properties[J]. Water, 2020, 12(9): 2357.
[31] Sivachandiran L, Khacef A.Enhanced seed germination and plant growth by atmospheric pressure cold air plasma: combined effect of seed and water treatment[J]. RSC Advances, 2017, 7(4): 1822-1832.
[32] Zhou Renwu, Zhou Rusen, Wang Peiyu, et al.Microplasma bubbles: reactive vehicles for biofilm dispersal[J]. ACS Applied Materials & Interfaces, 2019, 11(23): 20660-20669.
[33] Ganesh Subramanian P S, Ananthanarasimhan J, Leelesh P, et al. Plasma-activated water from DBD as a source of nitrogen for agriculture: specific energy and stability studies[J]. Journal of Applied Physics, 2021, 129(9): 093303.
[34] Man Chenxi, Zhang Cheng, Fang Haiqin, et al.Nanosecond-pulsed microbubble plasma reactor for plasma-activated water generation and bacterial inactivation[J]. Plasma Processes and Polymers, 2022, 19(6): e2200004.
[35] 孟国栋, 折俊艺, 应琪, 等. 微米尺度气体击穿的数值模拟研究进展[J]. 电工技术学报, 2022, 37(15): 3857-3875.
Meng Guodong, She Junyi, Ying Qi, et al.Research progress on numerical simulation of gas breakdown at microscale[J]. Transactions of China Electrotechnical Society, 2022, 37(15): 3857-3875.