• <tr id="yyy80"></tr>
  • <sup id="yyy80"></sup>
  • <tfoot id="yyy80"><noscript id="yyy80"></noscript></tfoot>
  • 99热精品在线国产_美女午夜性视频免费_国产精品国产高清国产av_av欧美777_自拍偷自拍亚洲精品老妇_亚洲熟女精品中文字幕_www日本黄色视频网_国产精品野战在线观看 ?

    Degradation of antibiotic contaminants from water by gas-liquid underwater discharge plasma

    2023-03-15 00:54:36FuLU盧伏JianZHOU周建andZhengweiWU吳征威
    Plasma Science and Technology 2023年3期

    Fu LU (盧伏), Jian ZHOU (周建) and Zhengwei WU (吳征威),2,*

    1 School of Nuclear Science and Technology, University of Science and Technology of China, Hefei 230026, People’s Republic of China

    2 Institute of Advanced Technology, University of Science and Technology of China, Hefei 230022,People’s Republic of China

    Abstract Antibiotic contamination adversely affects human health and ecological balance.In this study,gasliquid underwater discharge plasma was employed to simultaneously degrade three antibiotics,sulfadiazine(SDZ),tetracycline(TC),and norfloxacin(NOR),to address the growing problem of antibiotic contaminants in water.The effects of various parameters on the antibiotic degradation efficiency were evaluated,including the discharge gas type and flow rate,the initial concentration and pH of the solution,and the discharge voltage.Under the optimum parameter configuration,the average removal rate of the three antibiotics was 54.0% and the energy yield was 8.9 g(kW·h)-1 after 5 min treatment; the removal efficiency was 96.5% and the corresponding energy yield was 4.0 g(kW·h)-1 after 20 min treatment.Reactive substance capture and determination experiments indicated that·OH and O3 played a vital role in the decomposition of SDZ and NOR,but the role of reactive substances in TC degradation was relatively less significant.

    Keywords: antibiotic contamination, non-thermal plasma, gas-liquid underwater discharge,degradation efficiency, plasma reactive substances

    1.Introduction

    Since antibiotics with strong antibacterial effects were introduced in 1928, humans have been able to avoid suffering bacterial infections [1].However, the substantial increase in the use of antibiotics in human medicine, livestock husbandry, and aquaculture has increased the antibiotic content in the water body.Overabundant antibiotics in the water environment can accumulate in the body through the food chain, which has adverse effects on the bacterial flora in the human body [2], disrupting the colony dynamic balance and leading to drug-resistant bacteria.The World Health Organization has long recognized the proliferation of antibiotics as one of the challenges to human health [3].Therefore, it is necessary to degrade and remove antibiotic pollutants from the environment.

    Many treatment technologies have been developed to treat antibiotic pollutants in the aqueous environment,such as absorption processes, advanced oxidation processes (AOPs),advanced biological treatment,and hybrid technologies[4-6].However, all of them have some problems; for example, the removal rate of adsorption processes is low, causing secondary pollution, and oxidation processes generally require additional oxidation reagents which are uneconomical [7].Thus, there is a need to develop a new technology to treat antibiotics in wastewater.

    Non-thermal plasma, as one type of AOP, has been widely noticed in the field of environmental remediation.Non-thermal plasmas have various designs,such as dielectric barrier discharge (DBD), glow discharge, and corona discharge.In recent years, DBD as a non-thermal plasma technology has been widely used to degrade pollutants in the environment.DBD can evoke various chemical and physical effects in situ, like forming oxidation reactive substances(RSs) (O3, H2O2, ·OH, ·O), high-energy electrons, shock waves,ultraviolet(UV)radiation,electrohydraulic cavitation,etc.It has many advantages, such as high degradation efficiency, simple equipment, non-selective degradation of organics, and a mild treatment process.However, current plasma degradation technology faces difficulties such as poor energy efficiency and incomplete mineralization.Novel discharge reactors or combination with other degradation processes should be the route of the future [8, 9].

    Table 1.Chemo-physical characteristics of antibiotics.

    At present, the most common contaminants in water in China are tetracyclines, fluoroquinolones, and sulfonamides[10-12].Some researchers have reported using plasma to degrade antibiotics [13-15].However, most existing works using plasma to treat antibiotic contaminants have two shortcomings.On one hand, conventional experiments deal with a single antibiotic solution, which oversimplifies the problem of managing antibiotics in an aqueous environment.On the other hand, although it is effective to couple the plasma and catalysts to improve the degradation efficiency,secondary pollution of the catalysts cannot be avoided.We believe that it is difficult for existing experiments to support plasma technology application in practice.Therefore, we attempt to maximize the degradation capacity of the plasma itself to treat wastewater containing multiple antibiotics.We hope to facilitate the development of plasma technology towards practical applications.

    This study used plasma to simultaneously treat three common antibiotic pollutants,sulfadiazine(SDZ),norfloxacin(NOR), and tetracycline (TC).The effects of different operating parameters, such as the initial concentration of antibiotics,the initial pH of the antibiotic solution,the voltage of the discharge,the type of working gas, and the gas flow rate,on the removal efficiency of pollutants were determined.The critical roles of O3and ·OH in the degradation of SDZ and NOR were confirmed by RS scavenging experiments.In addition, the concentration of RSs was tested, further explaining that RSs produced by plasma play an important role in antibiotic degradation.

    Figure 1.Overview of the plasma discharge treatment system used in antibiotic degradation experiments.

    2.Experimental details

    2.1.Materials and reagents

    The antibiotics SDZ, NOR, and TC were purchased from Aladdin,China,and the chemical and physical characteristics are listed in table 1.They were above 96%purity and directly used in the experiments without further purification.Methanol(HPLC purity) and formic acid (HPLC purity) were also obtained from Aladdin,China.The antibiotics were dissolved in 1 l of deionized water to prepare three antibiotic stock solutions with a 100 mg l-1concentration.The stock solutions were stored at 4°C for further use.Analytical grade uric acid(UA),isopropanol(IPA),sodium pyruvate(SP),titanium sulfate (Ti(SO4)2), sodium indigo disulfonate, terephthalic acid (TA), 2-hydroxyterephthalic acid (HTA), sulfuric acid(H2SO4), phosphoric acid (H3PO4), hydrochloric acid (HCl),and sodium hydroxide (NaOH) were purchased from Macklin, China.

    2.2.Plasma treatment apparatus

    Figure 1 displays a schematic of the plasma treatment apparatus.The apparatus can be subdivided into the reaction container, the plasma generation, and the working gas input section.A 50 ml experimental beaker was used as the reaction vessel to contain the antibiotic solution.The plasma generation section comprised a power supply and a plasma nozzle.The high-voltage and high-frequency AC power supply featured the CTP-2000 K provided by Nanjing Suman Electronics Co.Ltd,China,with an adjustable output frequency of 10-45 kHz.A digital oscilloscope (GW Instek, GDS-2104) was used to monitor the voltage and current waveforms and the Lissajous figure.Figure 2 presents the typical voltage and current output waveforms during operation.The plasma nozzle was manufactured from cylindrical,coaxial quartz and copper tubes.The copper tube was embedded in the quartz tube and supplied with working gas at the inlet port, while the other port was inserted into the solution.The high-voltage electrode of the power supply was connected to the high-voltage port of the copper tube, and the low-voltage electrode was connected to the copper sheet at the bottom of the reaction vessel to generate a high-strength electric field in the copper tube.When the gas passed through the copper tube, it was excited by the electric field to generate plasma.The plasma was sprayed into the solution from the outlet and then interacted with the antibiotics.An oxygen or argon cylinder, or an air compressor (Jieba,JB12), and a flow meter constituted the gas input section.

    Figure 2.Waveforms of typical discharge voltage and current recorded by the oscilloscope during discharge.The input discharge voltage was 15 kV.

    2.3.Plasma treatment and analytical methods

    The reaction vessel was filled with 20 ml of antibiotic solution each time, diluted to the appropriate concentration, and the initial pH was adjusted by 0.1 mol l-1HCl and 0.1 mol l-1NaOH.The initial concentration, pH, discharge voltage, type of pumped gas, and flow rate were varied to determine the optimal degradation parameters.

    After plasma treatment, the antibiotic levels in the water were determined using an ultra-high-performance liquid chromatograph (Water, ACQUITY UPLC H-class) equipped with a UV detector and a T3 column (2.1 mm × 100 mm,1.8 μm).The mobile phases were 0.1% formic acid aqueous solution (Phase A) and methanol (Phase B).Table 2 shows the mobile phase gradient settings,with the mobile phase flow rate maintained at 0.3 ml min-1, which allowed the simultaneous determination of the three antibiotics from one sample.The sample volume was 10 μl, and the retention time was 10 min.The column temperature was maintained at room temperature, and the concentrations of SDZ, NOR, and TC were detected at 265, 278, and 355 nm, respectively.

    The removal efficiency (DE) of antibiotics treated was calculated by equation (1) [16, 17]:

    where C0represents the concentration of antibiotics before degradation, and Ctrepresents the concentration after t min.The energy yield(EY)of plasma treatment was calculated byequation (2):

    Table 2.Mobile phase establishment for detecting residual antibiotic concentrations in aqueous solutions via UPLC.

    where C0refers to the initial concentration of antibiotics,V is the volume of solution,DE is the removal efficiency,and P is the output power of the power supply, which could be calculated by the Lissajous figure(figure S1),and t is the time of plasma treatment.

    where U is the output voltage,dUc/dtis the current of the sampling capacitor,f is the discharge frequency,C=0.47 μF is the sampling capacitance of the power supply,k=1000 is the voltage sampling ratio,and S is the area of the Lissajous figure.

    2.4.Reactive substance capture and measurement experiments

    In order to understand the contribution of RSs to the degradation, RS scavengers UA, IPA, and SP were used to demonstrate the roles of O3[16], ·OH (reactions (4) and (5))[18], and H2O2[19] in the degradation process, respectively.

    The selective indigo method was used to determine the O3level after plasma treatment [20].The amount of H2O2was detected by titanium sulfate photometry [21].The ·OH can react with TA to produce HTA,which emits fluorescence at 450 nm when excited by light at a wavelength of 315 nm.The content of ·OH in the solution can be quantified as the fluorescence intensity of HTA, which was detected by a fluorescent microplate reader (Molecular Devices, SpectraMax iD5) [15].

    3.Results and discussion

    3.1.Effect of working gas types and flow rates on removal efficiency

    Argon,oxygen,and air were used to excite plasma to observe the effect of gas type on the degradation efficiency.The mixed solutions with a concentration of 20 mg l-1were treated with plasma generated by different gases, and the treatment time ranged from 0 to 25 min.The voltage used was maintained at 15 kV.The results show that the degradation efficiency continues to increase with the extension of treatment time regardless of the gas used (figure 3).After 5 min plasma treatment, 96.5% SDZ and 93.6% NOR removal could be achieved using O2.However, when air was used as the feed gas,the degradation efficiency dropped to 60.7%and 51.7%, respectively.When argon was used, the removal efficiency further declined to 10.1% and 7.8%.The result implies that for SDZ and NOR, the type of gas significantly affects the degradation efficiency.This phenomenon is attributed to the fact that the plasma removal ability of antibiotics is dependent on the oxidation of RSs in water.The more RSs, the more efficient the degradation of antibiotics.Using O2as the filling gas generates more reactive oxygen substances in water, explaining the strongest scavenging effect of the O2plasma [16, 17, 22, 23].

    Figure 3.Effect of different working gas types on the degradation efficiency of different antibiotics.Treatments were performed with(a)an SDZ solution, (b) a TC solution, (c) a NOR solution, and (d) a mixture of SDZ, TC, and NOR solution.The solution concentration was 20 mg l-1, the discharge voltage was 15 kV, and the treatment time was 0-25 min.Working gases were O2, argon, and air, respectively.

    Filling with different working gases has much less effect on TC degradation efficiency (figure 3(b)).It is possible because its structure is more unstable and susceptible to other factors, such as the photodegradation of TC by the light emitted by the plasma.Figure 3(d) depicts the average degradation efficiency by different input gases, showing that O2had the fastest degradation rate.After 10 min,the average degradation efficiency of the antibiotics was 99.5%using O2.Air took 20 min to remove ~95%of antibiotics.Only 66.4%of the total antibiotics were removed using argon after 25 min.Considering the use of air as the working gas, a satisfactory treatment effect with low cost was achieved, so the air was used as the working gas for subsequent experiments.

    The flow rate of gas can affect the degradation of antibiotics in two ways.It can affect the direct interaction between plasma and antibiotics, like the direct collision between high-energy electrons and antibiotic molecules.It can also change the content of RSs in water and affect the indirect interaction.After identical treatment time, with an increase in the air filling speed,the treatment effects of SDZ,TC, and NOR increase first and then decrease, and the treatment effect is best at 3 l min-1(figure 4).Corresponding to the air filling speeds of 1, 3, and 5 l min-1, the average degradation efficiency after 25 min is 82.7%, 96.5%, and 94.9%, respectively (figure 4(d)).When the air velocity is small, a larger air velocity is conducive to bringing the exciting RSs into the solution, thus playing a better role in degrading antibiotics [24, 25].However, too fast an air velocity may cause air molecules to be discharged before being converted into RSs, resulting in reduced RSs.It is also possible to generate larger bubbles in the water and reduce the contact between RSs and antibiotic molecules.As a result,an excessive gas flow rate reduces the degradation efficiency[26-28].In conclusion, 3 l min-1of air flow is the most suitable for degrading antibiotics.

    3.2.Effect of initial concentration and pH of antibiotics solution

    The concentration of antibiotics significantly impacts the degradation efficiency.When the discharge voltage was immobilized at 15 kV, air at 3 l min-1was used as the discharge gas.The quantities of RSs produced by the plasma discharge over a period of time are limited.If the concentration of antibiotics in the water is too low, the RSs will be underutilized, resulting in a waste of energy.Conversely,too high a concentration of antibiotics will result in a large number of byproducts.Therefore, the competition between the byproducts and the target antibiotic molecules will accentuate the scarcity of RSs, resulting in inadequate degradation of the antibiotics [29-31].

    Figure 4.Effect of the gas flow rate on the degradation efficiency of different antibiotics.Treatments were conducted with (a) an SDZ solution,(b)a TC solution,(c)a NOR solution,and(d)a mixture of SDZ,TC,and NOR solution.The solution concentration was 20 mg l-1,the working gas was air, the discharge voltage was 15 kV, and the treatment time was 0-25 min.Flow rates were 1, 3, and 5 l min-1,respectively.

    The results of different initial concentrations of antibiotic treatment are displayed in figure 5,and figure 5(d)graphs the evolution of the average degradation efficiency with treatment time for the mixed solution.The lower initial concentrations increase the treatment efficiency.Following a treatment time of 25 min,a treatment efficiency of 95.4%was achieved using an initial concentration of 10 mg l-1.When the concentration was 20 mg l-1, the treatment efficiency decreased to 94.8%,and further increasing the concentration to 30 mg l-1only removed 92.9% of the antibiotic.

    Nevertheless, this does not mean that lower initial concentrations are desired.Figure 6 presents the energy efficiency when treating different initial concentrations of antibiotics, showing that the energy efficiency tendency decreased over time, as most antibiotics were removed in the first 10 min.The energy yield of the plasma decreases as the concentration of the antibiotic decreases.In broad terms, an initial concentration of 20 mg l-1is appropriate to obtain an acceptable degradation and energy efficiency.

    In addition, experiments with different initial pH values were conducted to investigate the effect of pH on degradation efficiency.The output voltage was 15 kV, the air rate was 3 l min-1,and the initial concentration of antibiotics was also fixed at 20 mg l-1.The initial pH values varied from 3 to 11,and the experimental results are exhibited in figure 7.SDZ is more readily degraded in acidic solutions (figure 7(a)).In contrast, an alkaline environment is more favorable for the degradation of TC(figure 7(b))and NOR(figure 7(c)),which is consistent with the experimental results of He D et al [32]and Tang S et al[28].After 5 min,the degradation efficiency of TC in solution at pH value of 11 was 1.9 and 2.2 times higher than those at pH values of 7 and 3,and the degradation efficiency of NOR in solution at pH value of 11 was 2.8 and 4.9 times as effective as those at pH values of 7 and 3,respectively.

    On one hand, the pH of antibiotic-contaminated wastewater can play an essential role in producing RSs.Alkalinity or neutrality is preferable for converting O3to ·OH [21, 33-35].Among the RSs, ·OH has the most oxidizing power with the highest oxidation potential,implying that more·OH will cause faster degradation [36].On the other hand, the TC molecule will convert from the cationic state to the more unstable anionic form when shifting from acidic to alkaline solutions[32].These factors explain the accelerated removal efficiency of TC and NOR with increasing pH value.In contrast, SDZ was more easily removed in an acidic environment.The reason for this is probably that an acidic environment enables more powerful oxidation of ·OH [26, 31, 37-39], and O3is more easily concentrated in acidic conditions [29, 40].Overall,regarding the overall antibiotic degradation level(figure 7(d)),antibiotic degradation at alkaline pH conditions was deemed more beneficial in our experiments.

    Figure 5.Effect of the initial concentration on the degradation efficiency of different antibiotics.Treatment was applied with (a) an SDZ solution, (b) a TC solution, (c) a NOR solution, and (d) a mixture of SDZ, TC, and NOR solution.The working gas was air,the flow rate was 3 l min-1,the discharge voltage was 15 kV,and the treatment time was 0-25 min.The solution concentrations were 10,20, and 30 mg l-1, respectively.

    Figure 6.Influence of the concentration of antibiotic solution on the energy utilization efficiency (EY) with the same other parameters.Air was used as the working gas, the flow rate was set at 3 l min-1,and the discharge voltage was 15 kV.The solution concentrations were 10, 20, and 30 mg l-1, respectively.

    Figure 7.Effect of the solution pH on the degradation efficiency of different antibiotics.Treatment was conducted with(a)an SDZ solution,(b)a TC solution,(c)a NOR solution,and(d)a mixture of SDZ,TC,and NOR solution.The solution concentration was 20 mg l-1,the working gas was air,the flow rate was 3 l min-1,the discharge voltage was 15 kV,and the treatment time was 0-25 min.The initial pH settings were 3,7,and 11,respectively.

    3.3.Effect of applied voltage

    The effect of discharge voltages on the degradation was investigated.The results are depicted in figure 8.The initial concentration of 20 mg l-1,the air flow rate of 3 l min-1,and the initial pH of 12 were fixed, while different discharge voltages of 15 kV, 18 kV, and 21 kV were used.Figure 8(a)shows that after 10 min of treatment,the average degradation efficiency increases from 71.7% with 15 kV to 86.8% with 18 kV and subsequently to 88.5% with 21 kV.Extending the treatment time to 25 min increases the degradation efficiency from 96.4%at 15 kV to 96.6%at 18 kV and then to 97.4%at 21 kV.The results indicate that the degradation efficiency will enhance as the discharge voltage increases.The physicochemical effects in the discharge were enhanced with increased input energy.In addition to more RSs, higher voltages accelerate the electrons in the plasma, emitting more intense UV light and stronger shock waves, all of which increase the degradation efficiency of antibiotics [16, 41].

    Figure 8.Impact of discharge voltage on the (a) degradation efficiency (DE) and (b) energy utilization efficiency (EY) of the antibiotic mixture.The solution was a mixture of SDZ,TC,and NOR at a concentration of 20 mg l-1,the pH value was set to 12,and 3 l min-1 of air was used as the working gas.

    Figure 8(b)illustrates the energy efficiency with different discharge voltages.Because more than half of the antibiotics were removed within the first 5 min,the proportion of energy effectively utilized fell as the treatment time progressed regardless of the discharge voltage.Therefore, continuously increasing the discharge voltage is not recommended.Furthermore, as the discharge time increased to 25 min, the degradation efficiency at 21 kV was only 1%higher than that at 15 kV.A minimum operating voltage of 15 kV was considered to achieve the appropriate degradation efficiency and the best energy consumption and economy.

    3.4.Reactive substance trapping agent experiment

    During the gas-liquid discharge plasma, RSs such as H2O2,O3,and·OH are initiated through reactions(6)-(12)[42,43].These RSs often have strong oxidation potentials and react non-selectively with antibiotic molecules, eventually giving rise to their decomposition.SP, UA, and IPA were added to the antibiotic solution as H2O2,O3,and·OH trapping agents,respectively, to determine the role of RSs in the degradation.These agents reacted with the RSs in the solution while competing with the antibiotic molecules.

    Figure 9 illustrates the effect of adding trapping agents at 1, 5, and 10 mmol l-1on the treatment of the SDZ(figure 9(a)), TC (figure 9(b)), and NOR (figure 9(c)).The results show that for SDZ and NOR,the addition of IPA and UA significantly decreased the degradation, and the addition of 1 mmol l-1UA and IPA decreased the degradation efficiency by 9.0%and 13.6%for SDZ and 15.6%and 21.4%for NOR.The degradation efficiency of antibiotics decreased as the number of added scavengers increased.The degradation rate of NOR decreased by 15.6%after adding 1 mmol l-1UA,and the addition of UA at concentrations of 5 and 10 mmol l-1corresponded to 30.9% and 53.5% decrease,respectively.Notably, the inhibitory effect of UA was stronger than that of IPA when the dosages of UA and IPA were higher, probably because UA also scavenged ·OH from the water.In addition, the addition of SP had a negligible effect on the degradation efficiency.These indicate that·OH and O3are the major degradation RSs.Figure 9(b) illustrates the degradation of TC with the addition of scavengers and shows that their impact on the degradation of TC is negligible.Other effects in the plasma discharge might play a more significant role in the degradation of TC, analogous to that discussed in section 3.1.

    Figure 9.Outcomes of the RS capture experiments carried out with(a)an SDZ solution,(b)a TC solution,and(c)a NOR solution.The discharge voltage was 15 kV, 3 l min-1 of air was used as the working gas, the initial concentration was set at 20 mg l-1, and the pH value was 12.

    In overview,O3and·OH influence the decomposition of the antibiotic SDZ and NOR, while H2O2plays a minor role.The role of RSs in TC decomposition is not obvious.

    3.5.Quantity of reactive substances in the antibiotic solution

    The discharge voltage was 15 kV, the feeding air rate was 3 l min-1, the initial concentration of antibiotics was 20 mg l-1, and the initial pH was 12.The concentrations of O3, H2O2, and ·OH in the antibiotic solutions and the blank deionized water were analyzed after 5, 10, and 20 min, as demonstrated in figure 10.For the same plasma discharge time, more O3and ·OH were produced than H2O2.For example, when the underwater plasma was discharged for 5 min, the concentrations of O3and ·OH in the blank water group were 2.8 μmol l-1and 3.1 μmol l-1, while the concentration of H2O2was 9.0 nmol l-1.The ·OH content we measured was close to that measured by Duan L et al [44],but different from that reported by Guo H [26] and Shang K et al [45].This is attributable to the transition of O3to ·OH(reactions (13)-(15)).Research has shown that an alkaline environment will be more favorable for converting O3to·OH[21, 35].

    Figure 10.Concentrations of (a) O3, (b) H2O2, and (c) ·OH in the antibiotic solutions and blank deionized water.The discharge voltage was 15 kV,3 l min-1 of air was used as the working gas,the initial concentration was set at 20 mg l-1, and the pH value was 12.

    In addition, the concentration of these RSs increased with the discharge time.The concentration of O3in the treated blank deionized water changed from 2.8 μmol l-1at 5 min to 3.2 μmol l-1at 10 min, then to 4.5 μmol l-1when treated for 20 min(figure 10(a)).Moreover, as represented by O3, the 5 min treatment produced 2.8 μmol l-1of O3in the blank group,while the O3concentration was reduced to 2.6 μmol l-1in the SDZ solution,1.8 μmol l-1in the NOR solution,and 1.5 μmol l-1in the mixture solution.The concentration of RSs in the antibiotic solution was reduced compared to that within the blank group,supporting the involvement of RSs in antibiotic degradation.

    4.Conclusion

    In this study, we successfully removed three antibiotics, SDZ,TC, and NOR, simultaneously through gas-liquid underwater plasma discharge in water.Antibiotic degradation was differently affected based on the type and flow rate of the working gas, the initial concentration, the pH value, and the discharge voltage.O2exhibited the most effective degradation,and high or low gas flow rates reduced degradation efficiency.The lower the initial concentration, the higher the degradation efficiency but the lower the energy efficiency.TC and NOR preferred rapid degradation in alkaline solutions,whereas an acidic environment promoted SDZ degradation.A higher discharge voltage promoted degradation, but energy utilization efficiency decreased with increasing voltage.The most desirable degradation conditions were selected as: discharge voltage of 15 kV, air injection rate of 3 l min-1, pH value of 12, and initial concentration of 20 m l-1.Under such conditions,the average removal rate of the three antibiotics was 54.0% and the energy efficiency was 8.9 g(kW·h)-1for 5 min;and for 20 min of processing time,the removal efficiency was 96.5% and the corresponding energy utilization efficiency was 4.0 g(kW·h)-1.Experiments on the capture and detection of RSs demonstrated that O3and ·OH contribute to dissociating antibiotic molecules, but the role of H2O2was negligible.The study suggested that the role of RSs in TC degradation is unclear, probably because other effects influenced its degradation.The study showed that using underwater plasma to treat antibiotic contaminants possesses many merits and attractive prospects.Future research will focus on exploring the detailed evolution of antibiotic disintegration.Improving the experimental set-up and changing the discharge form will increase its efficiency while keeping it cost-effective.

    Acknowledgments

    This work was supported by the Key R&D Plan of Anhui Province (No.201904a07020013), Collaborative Innovation Program of Hefei Science Center,CAS(No.CX2140000018),and the Funding for Joint Lab of Applied Plasma Technology(No.JL06120001H).

    亚洲在线自拍视频| 性插视频无遮挡在线免费观看| a级毛片免费高清观看在线播放| 我要搜黄色片| 久久久久久久午夜电影| 久久99热6这里只有精品| 一本久久精品| 日韩强制内射视频| 我要看日韩黄色一级片| 久久久久久久午夜电影| 国产精品国产三级国产av玫瑰| 免费av毛片视频| 久久精品久久久久久噜噜老黄 | 亚洲性久久影院| 国产精品不卡视频一区二区| 久久久精品大字幕| 99热精品在线国产| 男女那种视频在线观看| 丝袜喷水一区| 真实男女啪啪啪动态图| 精品国内亚洲2022精品成人| 18+在线观看网站| 国产毛片a区久久久久| 全区人妻精品视频| 国产精品国产高清国产av| 亚洲欧美日韩东京热| 成人永久免费在线观看视频| 国产成人午夜福利电影在线观看| 久久久久久久亚洲中文字幕| 男女那种视频在线观看| 联通29元200g的流量卡| 麻豆成人av视频| 好男人视频免费观看在线| 亚洲国产色片| 亚洲精品影视一区二区三区av| 亚洲av男天堂| 午夜a级毛片| 国内揄拍国产精品人妻在线| 国产不卡一卡二| 精品一区二区免费观看| 深夜精品福利| 国产亚洲91精品色在线| 国产国拍精品亚洲av在线观看| 亚洲自偷自拍三级| av又黄又爽大尺度在线免费看 | 成人毛片a级毛片在线播放| 99久国产av精品国产电影| 毛片一级片免费看久久久久| 一个人免费在线观看电影| 床上黄色一级片| 亚洲精品粉嫩美女一区| 欧美激情国产日韩精品一区| 一级黄色大片毛片| av国产免费在线观看| 国产伦精品一区二区三区视频9| 国产一区二区亚洲精品在线观看| 久久久久久国产a免费观看| 亚洲七黄色美女视频| 美女内射精品一级片tv| 午夜福利在线观看吧| 国产精品一二三区在线看| 亚洲精品乱码久久久v下载方式| 十八禁国产超污无遮挡网站| 国产黄片美女视频| 天天躁夜夜躁狠狠久久av| 男女下面进入的视频免费午夜| 九色成人免费人妻av| 日韩av在线大香蕉| 一进一出抽搐动态| 国产在视频线在精品| 欧美日本视频| 三级国产精品欧美在线观看| 91久久精品电影网| 欧美日韩在线观看h| 自拍偷自拍亚洲精品老妇| 99热这里只有是精品在线观看| 精品久久久久久久久久免费视频| 色综合色国产| 日本免费一区二区三区高清不卡| 天天躁夜夜躁狠狠久久av| 久久亚洲精品不卡| 久久久精品94久久精品| 美女内射精品一级片tv| 国产麻豆成人av免费视频| 久久久久久久久久久丰满| 欧美最黄视频在线播放免费| 日韩国内少妇激情av| 麻豆久久精品国产亚洲av| 国产成人精品久久久久久| 1000部很黄的大片| 亚洲精品乱码久久久久久按摩| 26uuu在线亚洲综合色| 亚洲熟妇中文字幕五十中出| 国模一区二区三区四区视频| 精品久久久久久久久久免费视频| 午夜福利高清视频| 亚洲av一区综合| 如何舔出高潮| 婷婷精品国产亚洲av| 国产精品一及| 国产精华一区二区三区| 欧洲精品卡2卡3卡4卡5卡区| 亚洲第一电影网av| 国产高潮美女av| 熟女电影av网| 熟妇人妻久久中文字幕3abv| av天堂中文字幕网| 婷婷精品国产亚洲av| 午夜福利高清视频| 99国产极品粉嫩在线观看| 亚洲美女视频黄频| 一级二级三级毛片免费看| 插阴视频在线观看视频| 欧美成人一区二区免费高清观看| 成人午夜高清在线视频| 99久国产av精品国产电影| 91久久精品国产一区二区成人| 精品一区二区三区视频在线| 欧美丝袜亚洲另类| 成人美女网站在线观看视频| 看十八女毛片水多多多| 黄色日韩在线| 狂野欧美白嫩少妇大欣赏| 直男gayav资源| 亚洲性久久影院| 久久精品人妻少妇| 国产成人精品婷婷| 亚洲精品影视一区二区三区av| 久99久视频精品免费| 国产精品一二三区在线看| 99热精品在线国产| 在线天堂最新版资源| 亚洲成人中文字幕在线播放| 哪里可以看免费的av片| 男人的好看免费观看在线视频| 国产精品久久久久久久久免| 天堂av国产一区二区熟女人妻| 又粗又爽又猛毛片免费看| 在线免费观看的www视频| 91久久精品国产一区二区成人| 国产精品一二三区在线看| 国产精品电影一区二区三区| 亚洲中文字幕一区二区三区有码在线看| 久久人人精品亚洲av| 全区人妻精品视频| 深夜a级毛片| 国产成人91sexporn| 久久久久久国产a免费观看| 精品一区二区三区视频在线| 亚洲在线自拍视频| 一级黄色大片毛片| 最新中文字幕久久久久| 淫秽高清视频在线观看| 免费在线观看成人毛片| 18+在线观看网站| 精品人妻偷拍中文字幕| АⅤ资源中文在线天堂| 欧美一区二区国产精品久久精品| 淫秽高清视频在线观看| 69av精品久久久久久| 日本一二三区视频观看| 精品99又大又爽又粗少妇毛片| 国产在线男女| 亚洲精品日韩av片在线观看| 最后的刺客免费高清国语| 国内久久婷婷六月综合欲色啪| 亚洲国产日韩欧美精品在线观看| 久久精品久久久久久噜噜老黄 | 国产一区二区亚洲精品在线观看| 老司机福利观看| 在线观看66精品国产| 天堂√8在线中文| 夜夜夜夜夜久久久久| 免费av不卡在线播放| 国产一区二区在线av高清观看| 又爽又黄无遮挡网站| 九九在线视频观看精品| 欧美性猛交黑人性爽| 成熟少妇高潮喷水视频| 国内精品美女久久久久久| 欧美性感艳星| 真实男女啪啪啪动态图| 亚洲成人精品中文字幕电影| 久久久久九九精品影院| 国产伦在线观看视频一区| 日日撸夜夜添| 成年免费大片在线观看| 中文亚洲av片在线观看爽| 久久久久久大精品| 又爽又黄a免费视频| 午夜福利高清视频| 亚洲高清免费不卡视频| 日韩在线高清观看一区二区三区| 日日撸夜夜添| 日韩一区二区三区影片| 亚洲经典国产精华液单| 亚洲国产欧美人成| 亚洲美女搞黄在线观看| 亚洲精品久久久久久婷婷小说 | 老司机影院成人| 欧美+日韩+精品| 高清日韩中文字幕在线| 成人鲁丝片一二三区免费| 国产老妇女一区| 欧美一区二区国产精品久久精品| 高清毛片免费看| 亚洲一区二区三区色噜噜| 亚洲国产欧洲综合997久久,| 亚洲四区av| 国产又黄又爽又无遮挡在线| 麻豆一二三区av精品| 在线观看66精品国产| 婷婷色综合大香蕉| 乱人视频在线观看| 1024手机看黄色片| 一卡2卡三卡四卡精品乱码亚洲| av专区在线播放| 91午夜精品亚洲一区二区三区| 国产精品精品国产色婷婷| 久久久久久久久久久丰满| 此物有八面人人有两片| 一级毛片我不卡| 免费av观看视频| 久久久久久伊人网av| 日本撒尿小便嘘嘘汇集6| 高清午夜精品一区二区三区 | 欧美最新免费一区二区三区| 黄色视频,在线免费观看| 国产又黄又爽又无遮挡在线| 婷婷色综合大香蕉| 秋霞在线观看毛片| 夜夜看夜夜爽夜夜摸| 午夜亚洲福利在线播放| 国产伦精品一区二区三区四那| 婷婷六月久久综合丁香| 国产69精品久久久久777片| 成人特级黄色片久久久久久久| 欧美一区二区亚洲| 高清在线视频一区二区三区 | 免费一级毛片在线播放高清视频| 日韩人妻高清精品专区| 日韩强制内射视频| 国产69精品久久久久777片| 国产成人a∨麻豆精品| 51国产日韩欧美| 啦啦啦韩国在线观看视频| av天堂中文字幕网| 26uuu在线亚洲综合色| 女人十人毛片免费观看3o分钟| 三级毛片av免费| 尾随美女入室| 久久国产乱子免费精品| av卡一久久| 老师上课跳d突然被开到最大视频| 人体艺术视频欧美日本| 久久久久久久久久黄片| 国产精品嫩草影院av在线观看| 亚洲第一电影网av| 九草在线视频观看| 一进一出抽搐gif免费好疼| 国产精品国产三级国产av玫瑰| 久久久久九九精品影院| 欧美最黄视频在线播放免费| www日本黄色视频网| 午夜爱爱视频在线播放| 高清午夜精品一区二区三区 | 成人永久免费在线观看视频| 97在线视频观看| 级片在线观看| 日韩精品有码人妻一区| 99热这里只有是精品在线观看| 狂野欧美白嫩少妇大欣赏| 国产老妇女一区| 综合色丁香网| 97超碰精品成人国产| 亚洲国产欧美在线一区| 乱码一卡2卡4卡精品| 哪个播放器可以免费观看大片| 51国产日韩欧美| 午夜福利在线观看免费完整高清在 | 国产成人aa在线观看| 国产高清不卡午夜福利| 国产高清视频在线观看网站| 午夜爱爱视频在线播放| 国产日韩欧美在线精品| 夫妻性生交免费视频一级片| 97人妻精品一区二区三区麻豆| 亚洲国产精品成人综合色| 亚洲天堂国产精品一区在线| 人妻夜夜爽99麻豆av| 国产一区二区三区在线臀色熟女| 免费看av在线观看网站| 国产精品.久久久| 丰满的人妻完整版| 人妻少妇偷人精品九色| 成人永久免费在线观看视频| 美女国产视频在线观看| 亚洲成人久久爱视频| 欧美+日韩+精品| 黑人高潮一二区| 日本黄色片子视频| 亚洲av二区三区四区| 国产av不卡久久| 一进一出抽搐动态| 久久精品国产亚洲av涩爱 | 亚洲久久久久久中文字幕| 国产极品精品免费视频能看的| 亚洲精品国产成人久久av| 九九爱精品视频在线观看| av在线蜜桃| а√天堂www在线а√下载| 亚洲av电影不卡..在线观看| 欧美三级亚洲精品| 久久久久久大精品| 亚洲久久久久久中文字幕| 人妻夜夜爽99麻豆av| 校园人妻丝袜中文字幕| 尤物成人国产欧美一区二区三区| 国产精品av视频在线免费观看| 国产中年淑女户外野战色| 久久精品久久久久久久性| av天堂中文字幕网| 黄色视频,在线免费观看| 十八禁国产超污无遮挡网站| 色吧在线观看| 99久久成人亚洲精品观看| 亚洲精品日韩av片在线观看| 男人狂女人下面高潮的视频| 欧美日韩在线观看h| 日本撒尿小便嘘嘘汇集6| 男女啪啪激烈高潮av片| 国产美女午夜福利| 欧美+亚洲+日韩+国产| 国产真实乱freesex| 久久精品91蜜桃| 性色avwww在线观看| 国产精品一区二区在线观看99 | 日本色播在线视频| 国产精品伦人一区二区| 自拍偷自拍亚洲精品老妇| 男人的好看免费观看在线视频| 亚洲国产日韩欧美精品在线观看| 日韩欧美三级三区| 女人被狂操c到高潮| 看免费成人av毛片| 又粗又硬又长又爽又黄的视频 | 草草在线视频免费看| 性插视频无遮挡在线免费观看| 日本一本二区三区精品| 免费看a级黄色片| 插阴视频在线观看视频| 中文在线观看免费www的网站| 啦啦啦啦在线视频资源| 尾随美女入室| 亚洲av男天堂| 麻豆av噜噜一区二区三区| 欧美三级亚洲精品| 激情 狠狠 欧美| 亚洲精品乱码久久久v下载方式| 中文字幕av成人在线电影| 久久6这里有精品| 亚洲在线自拍视频| 少妇丰满av| 国产淫片久久久久久久久| 亚洲av二区三区四区| 激情 狠狠 欧美| 国产片特级美女逼逼视频| 国产亚洲欧美98| 日本黄大片高清| 欧美激情在线99| 可以在线观看毛片的网站| www日本黄色视频网| 免费观看的影片在线观看| 亚洲无线观看免费| 99热只有精品国产| 又爽又黄无遮挡网站| 永久网站在线| 亚洲七黄色美女视频| 联通29元200g的流量卡| 变态另类丝袜制服| 久久久久久久久中文| 噜噜噜噜噜久久久久久91| 久久亚洲国产成人精品v| 中文字幕熟女人妻在线| 91狼人影院| 在线观看美女被高潮喷水网站| 欧美激情国产日韩精品一区| 亚洲国产精品成人综合色| 波野结衣二区三区在线| 国产亚洲av嫩草精品影院| 国产极品精品免费视频能看的| 国产精品嫩草影院av在线观看| 成人毛片60女人毛片免费| 日韩欧美精品免费久久| 欧美+日韩+精品| 亚洲欧洲日产国产| 又黄又爽又刺激的免费视频.| 日本与韩国留学比较| 日本一二三区视频观看| 熟妇人妻久久中文字幕3abv| 欧美一区二区国产精品久久精品| 成年av动漫网址| 最好的美女福利视频网| 高清毛片免费观看视频网站| 国产伦一二天堂av在线观看| 日韩制服骚丝袜av| 好男人在线观看高清免费视频| 欧美变态另类bdsm刘玥| 蜜臀久久99精品久久宅男| 日韩亚洲欧美综合| 看黄色毛片网站| 国产三级在线视频| 国产成人aa在线观看| 在线a可以看的网站| 丰满乱子伦码专区| 日韩欧美国产在线观看| 大型黄色视频在线免费观看| 亚洲欧美清纯卡通| 日本熟妇午夜| 淫秽高清视频在线观看| 成人美女网站在线观看视频| 久久亚洲精品不卡| 蜜桃亚洲精品一区二区三区| 日本免费一区二区三区高清不卡| 一本一本综合久久| 此物有八面人人有两片| 精品日产1卡2卡| 日韩制服骚丝袜av| 亚洲国产欧洲综合997久久,| 国产精品人妻久久久久久| 免费大片18禁| 欧美最新免费一区二区三区| 欧美色视频一区免费| 日韩人妻高清精品专区| 男人狂女人下面高潮的视频| 日韩欧美一区二区三区在线观看| 啦啦啦观看免费观看视频高清| 国产精品三级大全| 精品少妇黑人巨大在线播放 | 国产真实乱freesex| 2022亚洲国产成人精品| 午夜精品国产一区二区电影 | 久久精品综合一区二区三区| 国产91av在线免费观看| 精华霜和精华液先用哪个| 国产视频内射| 欧美+亚洲+日韩+国产| 亚洲四区av| 一个人看的www免费观看视频| 亚洲最大成人av| 啦啦啦观看免费观看视频高清| 国产不卡一卡二| 又爽又黄无遮挡网站| 午夜福利高清视频| 18禁在线无遮挡免费观看视频| 国产伦一二天堂av在线观看| 最近视频中文字幕2019在线8| 成人欧美大片| 国产精品,欧美在线| 国产91av在线免费观看| 91午夜精品亚洲一区二区三区| 1024手机看黄色片| 欧美日韩一区二区视频在线观看视频在线 | eeuss影院久久| 亚洲不卡免费看| 波多野结衣高清作品| 赤兔流量卡办理| 狠狠狠狠99中文字幕| 九九在线视频观看精品| 日本午夜av视频| 好男人视频免费观看在线| 色94色欧美一区二区| av不卡在线播放| 人妻夜夜爽99麻豆av| 久久99热6这里只有精品| 人人妻人人澡人人看| 国产高清三级在线| 搡老乐熟女国产| 国产精品.久久久| 免费日韩欧美在线观看| av播播在线观看一区| 国产在线一区二区三区精| 2018国产大陆天天弄谢| 亚洲久久久国产精品| 丰满少妇做爰视频| 国产永久视频网站| 三上悠亚av全集在线观看| 国产欧美另类精品又又久久亚洲欧美| 97超碰精品成人国产| 美女福利国产在线| 满18在线观看网站| 国产精品久久久久久精品电影小说| 免费观看av网站的网址| 狂野欧美白嫩少妇大欣赏| 国产精品无大码| 亚洲图色成人| 有码 亚洲区| 国产探花极品一区二区| 亚洲,一卡二卡三卡| 亚洲国产日韩一区二区| 免费av中文字幕在线| 成人综合一区亚洲| 亚洲精品久久久久久婷婷小说| 国内精品宾馆在线| av.在线天堂| 亚洲精品国产av成人精品| 成人亚洲欧美一区二区av| 久久青草综合色| 黄色一级大片看看| 日本av手机在线免费观看| 国产精品人妻久久久久久| 丰满乱子伦码专区| 人妻 亚洲 视频| 国产精品欧美亚洲77777| 久久这里有精品视频免费| 国产精品免费大片| 久久这里有精品视频免费| 免费av中文字幕在线| 午夜免费男女啪啪视频观看| 男女国产视频网站| 日韩在线高清观看一区二区三区| 在线观看国产h片| 国产精品不卡视频一区二区| 成人亚洲精品一区在线观看| 成人影院久久| 久久久欧美国产精品| 搡老乐熟女国产| 少妇的逼水好多| 激情五月婷婷亚洲| 蜜桃在线观看..| 人人澡人人妻人| 国产探花极品一区二区| 日日爽夜夜爽网站| 波野结衣二区三区在线| 亚洲欧美清纯卡通| 人妻夜夜爽99麻豆av| 亚洲欧美一区二区三区国产| 日产精品乱码卡一卡2卡三| 性色av一级| 久久久久久久久大av| 久热这里只有精品99| 91精品伊人久久大香线蕉| 日韩av不卡免费在线播放| 国产爽快片一区二区三区| 男女边吃奶边做爰视频| 免费av不卡在线播放| 欧美日韩av久久| freevideosex欧美| 婷婷色av中文字幕| 亚洲国产精品国产精品| 亚洲国产精品专区欧美| 精品亚洲乱码少妇综合久久| 亚洲综合色惰| 又黄又爽又刺激的免费视频.| 最新的欧美精品一区二区| 99热这里只有是精品在线观看| 街头女战士在线观看网站| 天堂俺去俺来也www色官网| 91国产中文字幕| 美女视频免费永久观看网站| 又大又黄又爽视频免费| 极品少妇高潮喷水抽搐| xxx大片免费视频| 秋霞伦理黄片| 久久影院123| 伊人久久精品亚洲午夜| 大片免费播放器 马上看| 日韩av在线免费看完整版不卡| 伊人久久国产一区二区| 9色porny在线观看| 亚洲欧美精品自产自拍| 91精品国产九色| 午夜激情久久久久久久| 久久精品人人爽人人爽视色| 久久人人爽人人片av| 99热网站在线观看| 国产毛片在线视频| 女性被躁到高潮视频| 免费播放大片免费观看视频在线观看| 午夜免费男女啪啪视频观看| 亚洲精品国产av成人精品| 欧美日韩视频精品一区| 国产淫语在线视频| 18禁在线无遮挡免费观看视频| 久久99精品国语久久久| 久久国产精品男人的天堂亚洲 | 老司机亚洲免费影院| 国产一区二区在线观看日韩| 国产av一区二区精品久久| 精品卡一卡二卡四卡免费| av播播在线观看一区| 大又大粗又爽又黄少妇毛片口| 免费观看无遮挡的男女| 久久久午夜欧美精品| 日本91视频免费播放| 久久青草综合色| 男女啪啪激烈高潮av片| av在线老鸭窝| 久久精品久久精品一区二区三区| 男女边摸边吃奶| av在线老鸭窝| 久久国产亚洲av麻豆专区| 蜜臀久久99精品久久宅男| 国产免费又黄又爽又色| 99久久综合免费| 日本av免费视频播放| 久久狼人影院| 99九九在线精品视频| 亚洲精品日韩av片在线观看| 两个人免费观看高清视频| 春色校园在线视频观看| 国产欧美日韩综合在线一区二区| 国产精品不卡视频一区二区| 亚洲精品日本国产第一区| 精品一区二区免费观看|