In the present work,pulsed gas–liquid hybrid discharge plasma coupled with graphene/Cd S catalyst was evaluated to eliminate bisphenol A(BPA)in wastewater.The optimization of a series of process parameters was perfor...In the present work,pulsed gas–liquid hybrid discharge plasma coupled with graphene/Cd S catalyst was evaluated to eliminate bisphenol A(BPA)in wastewater.The optimization of a series of process parameters was performed in terms of BPA degradation performance.The experimental results demonstrated that nearly 90%of BPA(20 mg l^(-1))in the synthetic wastewater(p H=7.5,σ=10μS m^(-1))was degraded by the plasma catalytic system over 0.2 g l^(-1)graphene/Cd S at 19k V with a 4 l min^(-1)air flow rate and 10 mm electrode gap within 60 min.The BPA removal rate increased with increasing the discharge voltage and decreasing the initial BPA concentration or solution conductivity.Nevertheless,either too high or too low an air flow rate,electrode gap,catalyst dosage or initial solution p H would lead to a decrease in BPA degradation.Moreover,optical emission spectroscopy was used to gain information on short-lived reactive species formed from the pulsed gas–liquid hybrid discharge plasma system.The results indicated the existence of several highly oxidative free radicals such as·O and·OH.Finally,the activation pathway of O_(3)on the catalyst surface was analyzed by density functional theory.展开更多
Pulsed discharge in water and over water surfaces generates ultraviolet radiation,local high temperature,shock waves,and chemical reactive species,including hydroxyl radicals,hydrogen peroxide,and ozone.Pulsed dischar...Pulsed discharge in water and over water surfaces generates ultraviolet radiation,local high temperature,shock waves,and chemical reactive species,including hydroxyl radicals,hydrogen peroxide,and ozone.Pulsed discharge plasma(PDP) can oxidize and mineralize pollutants very efficiently,but high energy consumption restricts its application for industrial wastewater treatment.A novel method for improving the energy efficiency of wastewater treatment by PDP was proposed,in which peroxydisulfate(PDS) was added to wastewater and PDS was activated by PDP to produce more strong oxidizing radicals,including sulfate radicals and hydroxyl radicals,leading to a higher oxidation capacity for the PDP system.The experimental results show that the increase in solution conductivity slightly decreased the discharge power of the pulse discharge over the water surface.An increase in the discharge intensity improved the activation of PDS and therefore the degradation efficiency and energy efficiency of p-nitrophenol(PNP).An increase in the addition dosage of PDS greatly facilitated the degradation of PNP at a molar ratio of PDS to PNP of lower than 80:1,but the performance enhancement was no longer obvious at a dosage of more than 80:1.Under an applied voltage of 20 kV and a gas discharge gap of 2 mm,the degradation efficiency and energy efficiency of the PNP reached 90.7%and45.0 mg kWh^(-1) for the plasma/PDS system,respectively,which was 34%and 18.0 mg kWh^(-1)higher than for the discharge plasma treatment alone.Analysis of the physical and chemical effects indicated that ozone and hydrogen peroxide were important for PNP degradation and UV irradiation and heat from the discharge plasma might be the main physical effects for the activation of PDS.展开更多
The plasma characteristics of a gas-liquid phase discharge reactor were investigated by optical and electrical methods.The nozzle-cylinder electrode in the discharge reactor was supplied witha negative nanosecond puls...The plasma characteristics of a gas-liquid phase discharge reactor were investigated by optical and electrical methods.The nozzle-cylinder electrode in the discharge reactor was supplied witha negative nanosecond pulsed generator.The optical emission spectrum diagnosis revealed that OH(A2∑+ → X2Π,306–309 nm),N32(CΠ→B3Πg,337 nm),O(3p5p→3s-5s-0,777.2 nm)and O(3p3p→3s3s0,844.6 nm)were produced in the discharge plasma channels.The electron temperature(Te)was calculated from the emission relative intensity ratio between the atomic O 777.2 nm and 844.6 nm,and it increased with the applied voltage and the pulsed frequency and fell within the range of 0.5–0.8 e V.The gas temperature(Tg)that was measured by Lifbase was in a range from 400 K to 600 K.展开更多
A new process for removing the pollutants in aqueous solution-activated alumina bed in pulsed high-voltage electric field was investigated for the removal of phenol under different conditions. The experimental results...A new process for removing the pollutants in aqueous solution-activated alumina bed in pulsed high-voltage electric field was investigated for the removal of phenol under different conditions. The experimental results indicated the increase in removal rate with increasing applied voltage, increasing pH value of the solution, aeration, and adding Fe^2+. The removal rate of phenol could reach 72.1% when air aeration flow rate was 1200 ml/min, and 88.2% when 0.05 mmol/L Fe^2+ was added into the solution under the conditions of applied voltage 25 kV, initial phenol concentration of 5 mg/L, and initial pH value 5.5. The addition of sodium carbonate reduced the phenol removal rate. In the pulsed high-voltage electric field, local discharge occurred at the surface of activated alumina, which promoted phenol degradation in the thin water film. At the same time, the space-time distribution of gas-liquid phases was more uniform and the contact areas of the activated species generated from the discharge and the pollutant molecules were much wider due to the effect of the activated alumina bed. The synthetical effects of the pulsed high-voltage electric field and the activated alumina particles accelerated phenol degradation.展开更多
Atmospheric gas-liquid discharge with argon as a working gas is presented by employed nanosecond pulse power. The discharge is presented in a glow-like mode. The discharge powers are determined to be less than 1 W, an...Atmospheric gas-liquid discharge with argon as a working gas is presented by employed nanosecond pulse power. The discharge is presented in a glow-like mode. The discharge powers are determined to be less than 1 W, and remains almost constant when the discharge duration time increases. Bountiful active species are determined by capturing optical emission spectra, and their main generation processes are also discussed. The plasma gas temperature is calculated as 350 K by comparing the experimental spectra and the simulated ones of N2(C3Ⅱg→B3Ⅱg, △v=-2). The time resolved vibrational and rotational temperature is researched to present the stability of discharge when pulse voltage and discharge duration vary. The electron density is determined to be 1016 cm-3 according to the Stark broadening effect of the Ha line.展开更多
In this paper,unipolar pulse(including positive pulse and negative pulse)and bipolar pulse voltage are employed to generate diffuse gas–liquid discharge in atmospheric N2with a rumpetshaped quartz tube.The current–v...In this paper,unipolar pulse(including positive pulse and negative pulse)and bipolar pulse voltage are employed to generate diffuse gas–liquid discharge in atmospheric N2with a rumpetshaped quartz tube.The current–voltage waveforms,optical emission spectra of excited state active species,FTIR spectra of exhaust gas components,plasma gas temperature,and aqueous H2O2,NO2-,andNO3-production are compared in three pulse modes,meanwhile,the effects of pulse peak voltage and gas flow rate on the production of reactive species are studied.The results show that two obvious discharges occur in each voltage pulse in unipolar pulse driven discharge,differently,in bipolar pulse driven discharge,only one main discharge appears in a single voltage pulse time.The intensities of active species(OH(A),and O(3p))in all three pulsed discharge increase with the rise of pulse peak voltage and have the highest value at 200 ml min-1of gas flow rate.The absorbance intensities of NO2and N2O increase with the increase of pulse peak voltage and decrease with the increase of gas flow rate.Under the same discharge conditions,the bipolar pulse driven discharge shows lower breakdown voltage,and higher intensities of excited species(N2(C),OH(A),and O(3p)),nitrogen oxides(NO2,NO,and N2O),and higher production of aqueous H2O2,NO2-,andNO3-compared with both unipolar positive and negative discharges.展开更多
基金supported by the Open Fund for State Environmental Protection Key Laboratory of Synergetic Control and Joint Remediation for Soil&Water Pollution(No.GHBK-2020-006)National Natural Science Foundation of China(No.21876070)。
文摘In the present work,pulsed gas–liquid hybrid discharge plasma coupled with graphene/Cd S catalyst was evaluated to eliminate bisphenol A(BPA)in wastewater.The optimization of a series of process parameters was performed in terms of BPA degradation performance.The experimental results demonstrated that nearly 90%of BPA(20 mg l^(-1))in the synthetic wastewater(p H=7.5,σ=10μS m^(-1))was degraded by the plasma catalytic system over 0.2 g l^(-1)graphene/Cd S at 19k V with a 4 l min^(-1)air flow rate and 10 mm electrode gap within 60 min.The BPA removal rate increased with increasing the discharge voltage and decreasing the initial BPA concentration or solution conductivity.Nevertheless,either too high or too low an air flow rate,electrode gap,catalyst dosage or initial solution p H would lead to a decrease in BPA degradation.Moreover,optical emission spectroscopy was used to gain information on short-lived reactive species formed from the pulsed gas–liquid hybrid discharge plasma system.The results indicated the existence of several highly oxidative free radicals such as·O and·OH.Finally,the activation pathway of O_(3)on the catalyst surface was analyzed by density functional theory.
基金supported by National Natural Science Foundation of China(Grant No.21577011)the Fundamental Research Funds for the Central Universities(Grant No. DUT15QY23)
文摘Pulsed discharge in water and over water surfaces generates ultraviolet radiation,local high temperature,shock waves,and chemical reactive species,including hydroxyl radicals,hydrogen peroxide,and ozone.Pulsed discharge plasma(PDP) can oxidize and mineralize pollutants very efficiently,but high energy consumption restricts its application for industrial wastewater treatment.A novel method for improving the energy efficiency of wastewater treatment by PDP was proposed,in which peroxydisulfate(PDS) was added to wastewater and PDS was activated by PDP to produce more strong oxidizing radicals,including sulfate radicals and hydroxyl radicals,leading to a higher oxidation capacity for the PDP system.The experimental results show that the increase in solution conductivity slightly decreased the discharge power of the pulse discharge over the water surface.An increase in the discharge intensity improved the activation of PDS and therefore the degradation efficiency and energy efficiency of p-nitrophenol(PNP).An increase in the addition dosage of PDS greatly facilitated the degradation of PNP at a molar ratio of PDS to PNP of lower than 80:1,but the performance enhancement was no longer obvious at a dosage of more than 80:1.Under an applied voltage of 20 kV and a gas discharge gap of 2 mm,the degradation efficiency and energy efficiency of the PNP reached 90.7%and45.0 mg kWh^(-1) for the plasma/PDS system,respectively,which was 34%and 18.0 mg kWh^(-1)higher than for the discharge plasma treatment alone.Analysis of the physical and chemical effects indicated that ozone and hydrogen peroxide were important for PNP degradation and UV irradiation and heat from the discharge plasma might be the main physical effects for the activation of PDS.
基金supported by National Natural Science Foundation of China(Grant No.51207089)
文摘The plasma characteristics of a gas-liquid phase discharge reactor were investigated by optical and electrical methods.The nozzle-cylinder electrode in the discharge reactor was supplied witha negative nanosecond pulsed generator.The optical emission spectrum diagnosis revealed that OH(A2∑+ → X2Π,306–309 nm),N32(CΠ→B3Πg,337 nm),O(3p5p→3s-5s-0,777.2 nm)and O(3p3p→3s3s0,844.6 nm)were produced in the discharge plasma channels.The electron temperature(Te)was calculated from the emission relative intensity ratio between the atomic O 777.2 nm and 844.6 nm,and it increased with the applied voltage and the pulsed frequency and fell within the range of 0.5–0.8 e V.The gas temperature(Tg)that was measured by Lifbase was in a range from 400 K to 600 K.
基金Project supported by the Technology Innovation Project of University (No. 705013)
文摘A new process for removing the pollutants in aqueous solution-activated alumina bed in pulsed high-voltage electric field was investigated for the removal of phenol under different conditions. The experimental results indicated the increase in removal rate with increasing applied voltage, increasing pH value of the solution, aeration, and adding Fe^2+. The removal rate of phenol could reach 72.1% when air aeration flow rate was 1200 ml/min, and 88.2% when 0.05 mmol/L Fe^2+ was added into the solution under the conditions of applied voltage 25 kV, initial phenol concentration of 5 mg/L, and initial pH value 5.5. The addition of sodium carbonate reduced the phenol removal rate. In the pulsed high-voltage electric field, local discharge occurred at the surface of activated alumina, which promoted phenol degradation in the thin water film. At the same time, the space-time distribution of gas-liquid phases was more uniform and the contact areas of the activated species generated from the discharge and the pollutant molecules were much wider due to the effect of the activated alumina bed. The synthetical effects of the pulsed high-voltage electric field and the activated alumina particles accelerated phenol degradation.
基金supported by National Natural Science Foundation of China(Grant Nos.51677019)National Key Research and Development Program of China(2016YFC0207200)
文摘Atmospheric gas-liquid discharge with argon as a working gas is presented by employed nanosecond pulse power. The discharge is presented in a glow-like mode. The discharge powers are determined to be less than 1 W, and remains almost constant when the discharge duration time increases. Bountiful active species are determined by capturing optical emission spectra, and their main generation processes are also discussed. The plasma gas temperature is calculated as 350 K by comparing the experimental spectra and the simulated ones of N2(C3Ⅱg→B3Ⅱg, △v=-2). The time resolved vibrational and rotational temperature is researched to present the stability of discharge when pulse voltage and discharge duration vary. The electron density is determined to be 1016 cm-3 according to the Stark broadening effect of the Ha line.
基金supported by National Natural Science Foundation of China(Nos.51977023,51677019,and 11965018)Fundamental Research Funds for the Central Universities in China(No.DUT18LK42)。
文摘In this paper,unipolar pulse(including positive pulse and negative pulse)and bipolar pulse voltage are employed to generate diffuse gas–liquid discharge in atmospheric N2with a rumpetshaped quartz tube.The current–voltage waveforms,optical emission spectra of excited state active species,FTIR spectra of exhaust gas components,plasma gas temperature,and aqueous H2O2,NO2-,andNO3-production are compared in three pulse modes,meanwhile,the effects of pulse peak voltage and gas flow rate on the production of reactive species are studied.The results show that two obvious discharges occur in each voltage pulse in unipolar pulse driven discharge,differently,in bipolar pulse driven discharge,only one main discharge appears in a single voltage pulse time.The intensities of active species(OH(A),and O(3p))in all three pulsed discharge increase with the rise of pulse peak voltage and have the highest value at 200 ml min-1of gas flow rate.The absorbance intensities of NO2and N2O increase with the increase of pulse peak voltage and decrease with the increase of gas flow rate.Under the same discharge conditions,the bipolar pulse driven discharge shows lower breakdown voltage,and higher intensities of excited species(N2(C),OH(A),and O(3p)),nitrogen oxides(NO2,NO,and N2O),and higher production of aqueous H2O2,NO2-,andNO3-compared with both unipolar positive and negative discharges.