Optimization of tetracycline degradation by nanosecond pulsed gas-liquid discharge with needle-water configuration
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摘要: 过度使用抗生素导致的水污染，对自然环境和人类健康造成了重大威胁。低温等离子体作为一种绿色环保的高级氧化技术，被认为是一种最具前景的抗生素降解方法之一，然而在降解效率和能量效率方面还有待进一步提高。利用纳秒脉冲放电激励针-水结构气液放电，获得了一种能产生高活性等离子体的瞬态火花模式放电，并应用于水中四环素降解，研究了脉冲电压、频率、初始浓度、初始pH值等参数对四环素降解的影响，结果表明初始浓度50 mg/L，脉冲电压9 kV、频率2 kHz，初始pH值为中性的条件下四环素的降解率最高，处理时间10 min时降解率达到了91.6%，能量效率和每阶电能分别为0.165 g·kW−1·h−1和0.78 kW·h·m−3。自由基淬灭实验表明羟基自由基 (·OH) 在四环素降解过程中起主要作用，而H2O2和O3的作用稍弱。细胞毒性实验也表明气液放电处理10 min后的溶液毒性显著下降。Abstract: Water pollution caused by the overuse of antibiotics poses a major threat to the natural environment and human health. As a green and environmentally friendly advanced oxidation technology, low-temperature plasma is considered to be one of the most promising antibiotic degradation methods, but it needs to be further improved in terms of degradation efficiency and energy efficiency. In this study, transient spark discharge was obtained by using nanosecond pulse power supply with a needle-water electrode configuration, and applied to tetracycline degradation in water. The effect of pulse voltage, frequency, initial concentration, initial pH value on tetracycline degradation was studied, and the results show that the degradation rate of tetracycline was the highest under the condition that the initial concentration was 50 mg/L, the pulse voltage was 9 kV, the frequency was 2 kHz, the initial pH is neutral, and the degradation rate reached 91.6% when the processing time was 10 min. The energy efficiency and electrical energy per order are 0.165 g·kW−1·h−1 and 0.78 kW·h·m−3, respectively. Free radical quenching experiments showed that hydroxyl radicals (·OH) played a major role in the degradation of tetracycline, while H2O2 and O3 played a slightly weaker role. Cytotoxicity experiments also showed that the toxicity of the solution decreased significantly after 10 min of gas-liquid discharge treatment.
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图 2 脉冲电压对四环素降解率的影响
Figure 2. Effect of pulse voltage on the degradation rate of tetracycline
图 3 频率对四环素降解率的影响
Figure 3. Effect of frequency on the degradation rate of tetracycline
图 4 初始浓度对四环素降解率的影响
Figure 4. Effect of initial concentration on the degradation rate of tetracycline
图 6 每阶电能和能量效率随处理时间的变化
Figure 6. Variation of electrical energy per order and energy efficiency with processing time
图 8 去离子水与四环素溶液中长寿命物种的浓度
Figure 8. Concentration of long-lived species in deionized water and tetracycline solution
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[1] Dai Yingjie, Liu Mei, Li Jingjing, et al. A review on pollution situation and treatment methods of tetracycline in groundwater[J]. Separation Science and Technology, 2020, 55(5): 1005-1021. doi: 10.1080/01496395.2019.1577445 [2] 梅丹华, 方志, 邵涛. 大气压低温等离子体特性与应用研究现状[J]. 中国电机工程学报, 2020, 40(4):1339-1358Mei Danhua, Fang Zhi, Shao Tao. Recent progress on characteristics and applications of atmospheric pressure low temperature plasmas[J]. Proceedings of the CSEE, 2020, 40(4): 1339-1358 [3] 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):1-9Dai 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 [4] 孔刚玉, 刘定新. 气体等离子体与水溶液的相互作用研究——意义、挑战与新进展[J]. 高电压技术, 2014, 40(10):2956-2965Kong Gangyu, Liu Dingxin. Researches on the interaction between gas plasmas and aqueous solutions: significance, challenges and new progresses[J]. High Voltage Engineering, 2014, 40(10): 2956-2965 [5] Miruka A C, Zhang Ai, Wang Qiancheng, et al. Degradation of glucocorticoids in water by a synergistic system of peroxymonosulfate, microbubble and dielectric barrier discharges[J]. Journal of Water Process Engineering, 2021, 42: 102175. doi: 10.1016/j.jwpe.2021.102175 [6] 武海霞, 陈卫刚, 方志, 等. 介质阻挡放电优化激活过硫酸盐处理四环素废水[J]. 高电压技术, 2019, 45(5):1387-1395Wu Haixia, Chen Weigang, Fang Zhi, et al. Optimized activation of persulfate by dielectric barrier discharge for the treatment of tetracycline wastewater[J]. High Voltage Engineering, 2019, 45(5): 1387-1395 [7] Li Wenshao, Zhou Renwu, Zhou Rusen, et al. Insights into amoxicillin degradation in water by non-thermal plasmas[J]. Chemosphere, 2022, 291: 132757. doi: 10.1016/j.chemosphere.2021.132757 [8] Wei Ying, Lu Guanglu, Xie Dongrun, et al. Degradation of enrofloxacin in aqueous by DBD plasma and UV: degradation performance, mechanism and toxicity assessment[J]. Chemical Engineering Journal, 2022, 431: 133360. doi: 10.1016/j.cej.2021.133360 [9] Sar A B, Shabani E G, Haghighi M, et al. Synergistic catalytic degradation of ciprofloxacin using magnetic carbon nanomaterial/NiFe2O4 promoted cold atmospheric pressure plasma jet: Influence of charcoal, multi walled carbon nanotubes and walnut shell[J]. Journal of the Taiwan Institute of Chemical Engineers, 2022, 132: 104131. doi: 10.1016/j.jtice.2021.10.031 [10] 谢瑞, 陈超, 李武华, 等. 气液相等离子体放电水处理反应器及苯酚降解分析[J]. 高电压技术, 2010, 36(11):2791-2796Xie Rui, Chen Chao, Li Wuhuan, et al. Analysis on gas-liquid hybrid plasma discharge reactor for wastewater treatment and phenol degradation[J]. High Voltage Engineering, 2010, 36(11): 2791-2796 [11] Liu Xinghao, Cheng Cheng, Xu Zimu, et al. Degradation of tetracycline in water by gas–liquid plasma in conjunction with rGO-TiO2 nanocomposite[J]. Plasma Science and Technology, 2021, 23: 115503. doi: 10.1088/2058-6272/ac1323 [12] Chandana L, Ray D, Subrahmanyam C, et al. Physicochemical process of non-thermal plasma at gas-liquid interface and synergistic effect of plasma with catalyst[J]. Current Applied Physics, 2022, 36: 16-26. doi: 10.1016/j.cap.2022.01.006 [13] Zhou Xiongfeng, Xiang Hongfu, Yang Minghao, et al. Temporal evolution characteristics of the excited species in a pulsed needle-water discharge: effect of voltage and frequency[J]. Journal of Physics D:Applied Physics, 2023, 56(45): 455202. doi: 10.1088/1361-6463/acec81 [14] 张波, 周若瑜, 汪立峰, 等. 脉冲参数对大气压He中一维射流阵列放电特性的影响[J]. 电工技术学报, 2018, 33(21):5109-5118Zhang Bo, Zhou Ruoyu, Wang Lifeng, et al. Influence of pulse parameters discharge characteristics of one-dimensional plasma jet array in heat atmospheric pressure[J]. Transactions of China Electrotechnical Society, 2018, 33(21): 5109-5118 [15] 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):2326-2335Man 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 [16] Xiang Liangrui, Xie Zhehao, Guo He, et al. Efficient removal of emerging contaminant sulfamethoxazole in water by ozone coupled with calcium peroxide: Mechanism and toxicity assessment[J]. Chemosphere, 2021, 283: 131156. doi: 10.1016/j.chemosphere.2021.131156 [17] 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: 2200004. doi: 10.1002/ppap.202200004 [18] Zhang Tianqi, Zhou Renwu, Wang Peiyu, et al. Degradation of cefixime antibiotic in water by atmospheric plasma bubbles: performance, degradation pathways and toxicity evaluation[J]. Chemical Engineering Journal, 2021, 421: 127730. doi: 10.1016/j.cej.2020.127730 [19] 孙明, 郝夏桐, 鲁晓辉, 等. 气液两相脉冲放电反应器的设计及其对酸性橙Ⅱ的降解效果[J]. 高电压技术, 2015, 41(2):498-503Sun Ming, Hao Xiatong, Lu Xiaohui, et al. A reactor design of gas-liquid two-phase pulse discharge and its performance in degrading acid orange Ⅱ[J]. High Voltage Engineering, 2015, 41(2): 498-503 [20] Wang Chao, Qu Guangzhou, Wang Tiecheng, et al. Removal of tetracycline antibiotics from wastewater by pulsed corona discharge plasma coupled with natural soil particles[J]. Chemical Engineering Journal, 2018, 346: 159-170. doi: 10.1016/j.cej.2018.03.149 [21] Mouele E S M, Myo T Z M, Kyaw H H, et al. Degradation of sulfamethoxazole by double cylindrical dielectric barrier discharge system combined with Ti/C-N-TiO2 supported nanocatalyst[J]. Journal of Hazardous Materials Advances, 2022, 5: 100051. doi: 10.1016/j.hazadv.2022.100051 [22] 孙明, 金宏力, 杨颜颜, 等. 脉冲放电等离子体协同二氧化钛降解偶氮类染料废水[J]. 高电压技术, 2015, 41(9):2862-2867Sun Ming, Jin Hongli, Yang Yanyan, et al. Degradation of azo dye wastewater using pulsed discharge plasma with TiO2[J]. High Voltage Engineering, 2015, 41(9): 2862-2867 [23] Wu Haixia, Fan Jiawei, Liu Feng, et al. Degradation of tetracycline in aqueous solution by persulphate assisted gas–liquid dielectric barrier discharge[J]. Water and Environment Journal, 2021, 35(3): 902-912. doi: 10.1111/wej.12678 [24] Li Zhen, Wang Yawen, Guo He, et al. Insights into water film DBD plasma driven by pulse power for ibuprofen elimination in water: performance, mechanism and degradation route[J]. Separation and Purification Technology, 2021, 277: 119415. doi: 10.1016/j.seppur.2021.119415 [25] Li Hu, Li Tengfei, He Sitong, et al. Efficient degradation of antibiotics by non-thermal discharge plasma: highlight the impacts of molecular structures and degradation pathways[J]. Chemical Engineering Journal, 2020, 395: 125091. doi: 10.1016/j.cej.2020.125091 [26] 王芝, 韩若愚, 李显东, 等. 水中针-板结构小能量脉冲火花放电特性[J]. 强激光与粒子束, 2022, 34:095006 doi: 10.11884/HPLPB202234.220022Wang Zhi, Han Ruoyu, Li Xiandong, et al. Low-energy pulsed spark discharge characteristics of pin-plate structure in water[J]. High Power Laser and Particle Beams, 2022, 34: 095006 doi: 10.11884/HPLPB202234.220022 [27] Gong Shi, Sun Yabing, Zheng Ke, et al. Degradation of levofloxacin in aqueous solution by non-thermal plasma combined with Ag3PO4/activated carbon fibers: Mechanism and degradation pathways[J]. Separation and Purification Technology, 2020, 250: 117264. doi: 10.1016/j.seppur.2020.117264 [28] 刘亚韪, 周子凯, 王森, 等. 大气压空气针-水结构脉冲气-液放电特性研究[J]. 强激光与粒子束, 2021, 33:065008 doi: 10.11884/HPLPB202133.210020Liu Yawei, Zhou Zikai, Wang Sen, et al. Research on the characteristics of atmospheric pressure air pulse gas-liquid discharge using a needle-water electrode[J]. High Power Laser and Particle Beams, 2021, 33: 065008 doi: 10.11884/HPLPB202133.210020 [29] Zheng Ke, Sun Yabing, Gong Shi, et al. Degradation of sulfamethoxazole in aqueous solution by dielectric barrier discharge plasma combined with Bi2WO6–rMoS2 nanocomposite: mechanism and degradation pathway[J]. Chemosphere, 2019, 222: 872-883. doi: 10.1016/j.chemosphere.2019.02.004 [30] Zhou Renwu, Zhou Rusen, Alam D, et al. Plasmacatalytic bubbles using CeO2 for organic pollutant degradation[J]. Chemical Engineering Journal, 2021, 403: 126413. doi: 10.1016/j.cej.2020.126413 [31] Hao Chunjing, Yan Zeyao, Liu Kefu, et al. Degradation of pharmaceutical contaminant tetracycline in aqueous solution by coaxial-type DBD plasma reactor[J]. IEEE Transactions on Plasma Science, 2020, 48(2): 471-481. doi: 10.1109/TPS.2020.2964612 [32] Brisset J L, Hnatiuc E. Peroxynitrite: a re-examination of the chemical properties of non-thermal discharges burning in air over aqueous solutions[J]. Plasma Chemistry and Plasma Processing, 2012, 32(4): 655-674. doi: 10.1007/s11090-012-9384-x -
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