Investigation was made into the degradation of organic compounds by a dielectric barrier corona discharge (DBCD) system. The DBCD, consisting of a quartz tube, a concentric high voltage electrode and a net wrapped t...Investigation was made into the degradation of organic compounds by a dielectric barrier corona discharge (DBCD) system. The DBCD, consisting of a quartz tube, a concentric high voltage electrode and a net wrapped to the external wall (used as ground electrode), was introduced to generate active species which were sprayed into the organic solution through an aerator fixed on the bottom of the tube. The effect of four factors-the discharge voltage, gas flow rate, solution conductivity, and pH of wastewater, on the degradation efficiency of phenol was assessed. The obtained results demonstrated that this process was an effective method for phenol degradation. The degradation rate was enhanced with the increase in power supplied. The degradation efficiency in alkaline conditions was higher than those in acid and neutral conditions. The optimal gas flow rate for phenol degradation in the system was 1.6 L/min, while the solution conductivity had little effect on the degradation.展开更多
The multifunctionality and the advantages of thermal plasma for the fast inactivation of viable cells and degradation of organic compounds dissolved in waste water are presented.A complete bacterial inactivation proce...The multifunctionality and the advantages of thermal plasma for the fast inactivation of viable cells and degradation of organic compounds dissolved in waste water are presented.A complete bacterial inactivation process was observed and studied using a thermal plasma treatment source with very short application times,in particular for Staphylococcus aureus bundle spore survival.The survival curves and analyses of the experimental data of the initial and final densities of S.aureus bacteria show a dramatic inhibitory effect of the plasma discharge on the residual bacteria survival ratio.As the exposure time increased,the inactivation process rate increased for direct exposure more than it did for indirect exposure.The evaluation of direct and indirect exposure was based on the analysis of the ultraviolet spectrum from the absorbance spectra of the organic compound dye called benzene sulfonate(C(16)H(11)N2Na O4S)and of viable cells called S.aureus.Organic compounds were degraded and viable cells were killed in a short time by thermal plasma.Moreover,analyses of total carbon,total organic carbon,and total inorganic carbon showed a fast decrease in organically bound carbon,however,this was not as fast as the absorbance spectra revealed by the exposure time increasing more for direct exposure than indirect exposure.After 100 s of exposure to the organic compound dye the removal had a maximun of 40%for samples with indirect exposure to the plasma and a maximum of 90%for samples with the direct exposure.For both samples,where some organic contaminants still remained in treated water,four electrolytes(KCl,Na Cl,Na2SO4,and CH3COONa)were added to be effective for complete sterilization,reaching a purity of 100%.A proposal is made for an optimized thermal plasma water purification system(TPWPS)to improve fast inactivation of microbes and the degradation of organic compounds dissolved in water(especially for direct exposure rather than indirect exposure)using a hybrid plasma torch with an electrical power of 125 kW(500 V–250 A)producing a high-temperature(10 000 K–19 000 K)plasma jet with a maximum gas consumption of 28 mg s^-1.展开更多
Metal-based perovskite oxides have contributed significantly to the advanced oxidation processes(AOPs)due to their diverse active sites and excellent compositional/structural flexibility.In this study,we specially des...Metal-based perovskite oxides have contributed significantly to the advanced oxidation processes(AOPs)due to their diverse active sites and excellent compositional/structural flexibility.In this study,we specially designed a perovskite oxide with abundant oxygen vacancies,SrCo_(0.8)Fe_(0.2)O_(3)(SCF),and firstly applied it as a catalyst in peroxymonosulfate(PMS) activation towards organic pollutants degradation.The result revealed that the prepared SCF catalyst exhibited excellent performance on organic compounds degradation.Besides,SCF showed much better activity than La_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3)(LSCF) in terms of reaction rate and stability for the degradation of the organic compounds.Based on the analysis of scanning electron microscope,transmission electron microscope,X-ray diffraction,N_(2) adsorption-desorption,X-ray photoelectron spectroscopy and electron paramagnetic resonance,it was confirmed that the perovskite catalysts with high content of Sr doping at A-site could effectively create a defect-rich surface and optimize its physicochemical properties,which was responsible for the excellent heterogeneous catalytic activity of SCF.SCF can generate three highly active species:~1 O_(2),SO_(4)^(-)· and ·OH in PMS activation,revealing the degradation process of organic compounds was a coupled multiple active species in both radical and nonradical pathway.Moreover,it was mainly in a radical pathway in the degradation through PMS activation on SCF and SO_(4)^(-)· radicals produced were the dominant species in SCF/PMS system.This study demonstrated that perovskite-type catalysts could enrich OVs efficiently by doping strategy and regulate the PMS activation towards sulfate radical-based AOPs.展开更多
Photocatalytic oxidation process for the degradation of volatile organic compounds(VOCs)contaminants is a promising technology.But until now,the low photocatalytic activity of the conventional TiO_(2) photocatalyst un...Photocatalytic oxidation process for the degradation of volatile organic compounds(VOCs)contaminants is a promising technology.But until now,the low photocatalytic activity of the conventional TiO_(2) photocatalyst under visible-light irradia-tion hinders the deployment of this technique for VOCs degradation.WO_(3) has been proved to be a suitable photocatalytic material for degradation of various VOCs as its appropriate band-gap,high stability and great capability.Nevertheless,the actual implementation of WO_(3) is still restricted by short lifetime of photoexcited charge carriers and low light energy conver-sion efficiency:its photocatalytic performance is needed to be improved.This review discusses the process of tungsten-based photocatalyst for removal of VOCs and summarizes a variety of strategies to improve the VOCs oxidation performances of WO_(3),such as controlling the morphology structure,engendering chemical defects,coupling heterojunction,doping suitable dopants and loading a co-catalyst.In addition,the practical application of tungsten-based photocatalyst is discussed.展开更多
The study herein investigated the effectiveness of simultaneous use of ozone and hydrogen peroxide(O_3/H_2O_2 process) to degrade o-phenylenediamine(o-PDA) in a simulated wastewater. A rotor–stator reactor(RSR) was e...The study herein investigated the effectiveness of simultaneous use of ozone and hydrogen peroxide(O_3/H_2O_2 process) to degrade o-phenylenediamine(o-PDA) in a simulated wastewater. A rotor–stator reactor(RSR) was employed to create a high-gravity environment in order to enhance ozone-liquid mass transfer rate and possibly improve the degradation rate of o-PDA. The degradation efficiency of o-PDA(η) as well as the overall gas-phase volumetric mass transfer coefficient(KGa) were determined under different operating conditions of H_2O_2 concentration, initial o-PDA concentration, temperature of reaction, initial p H and rotation speed of RSR in attempt to establish the optimal conditions. Chemical oxygen demand reduction rate(rCOD) of wastewater treated at a particular set of conditions was also analyzed. Additionally, the intermediate products of degradation were identified using a gas chromatography-mass spectrometer(GC/MS) to further evaluate the extent of o-PDA degradation as well as establish its possible degradation pathway. Results were validated by comparison with those of sole use of ozone(O_3 process), and it was noted that η, KGa and rCODachieved by O_3/H_2O_2 process was 24.4%,31.6% and 25.2% respectively higher than those of O_3 process, indicating that H_2O_2 can greatly enhance ozonation of o-PDA. This work further demonstrates that an RSR can significantly intensify ozone-liquid mass transfer rate and thus provides a feasible intensification means for the ozonation of o-PDA as well as other recalcitrant organics.展开更多
A field measurement campaign for ozone and ozone precursors (VOCs and NOx) was conducted in summer 2011 around a petroleum refinery in the Beijing rural region. Three observation sites were arranged, one at southwes...A field measurement campaign for ozone and ozone precursors (VOCs and NOx) was conducted in summer 2011 around a petroleum refinery in the Beijing rural region. Three observation sites were arranged, one at southwest of the refinery as the background, and two at northeast of the refinery as the downwind receptors. Monitoring data revealed the presence of serious surface 03 pollution with the characteristics of high average daily mean and maximum concentrations (64.0 and 145.4 ppbV in no-rain days, respectively) and multi-peak diurnal variation. For NOx, the average hourly concentrations of NO2 and NO were in the range of 20.546.1 and 1.8-6.4 ppbV, respectively. For VOC measurement, a total of 51 compounds were detected. Normally, TVOCs at the background site was only dozens of ppbC, while TVOCs at the downwind sites reached several hundreds of ppbC. By subtracting the VOC concentrations at background, chemical profiles of VOC emission from the refinery were obtained, mainly including alkanes (60.0% ± 4.3%), alkenes (21.1% ± 5.5%) and aromatics (18.9% ±3.9%). Moreover, some differences in chemical profiles for the same measurement hours were observed between the downwind sites; the volume ratios of alkanes with low reactivity and those of alkenes with high reactivity respectively showed an increasing trend and a decreasing trend. Finally, based on temporal and spatial variations of VOC mixing ratios, their photochemical degradations and dispersion degradations were estimated to be 0.15-0.27 and 0.42-0.62, respectively, by the photochemical age calculation method, indicating stronger photochemical reactions around the refinery.展开更多
基金supported by Ministry of Education of the People's Republic of China (20070141004)
文摘Investigation was made into the degradation of organic compounds by a dielectric barrier corona discharge (DBCD) system. The DBCD, consisting of a quartz tube, a concentric high voltage electrode and a net wrapped to the external wall (used as ground electrode), was introduced to generate active species which were sprayed into the organic solution through an aerator fixed on the bottom of the tube. The effect of four factors-the discharge voltage, gas flow rate, solution conductivity, and pH of wastewater, on the degradation efficiency of phenol was assessed. The obtained results demonstrated that this process was an effective method for phenol degradation. The degradation rate was enhanced with the increase in power supplied. The degradation efficiency in alkaline conditions was higher than those in acid and neutral conditions. The optimal gas flow rate for phenol degradation in the system was 1.6 L/min, while the solution conductivity had little effect on the degradation.
基金financial support from MEPhI in the framework of the Russian Academic Excellence Project
文摘The multifunctionality and the advantages of thermal plasma for the fast inactivation of viable cells and degradation of organic compounds dissolved in waste water are presented.A complete bacterial inactivation process was observed and studied using a thermal plasma treatment source with very short application times,in particular for Staphylococcus aureus bundle spore survival.The survival curves and analyses of the experimental data of the initial and final densities of S.aureus bacteria show a dramatic inhibitory effect of the plasma discharge on the residual bacteria survival ratio.As the exposure time increased,the inactivation process rate increased for direct exposure more than it did for indirect exposure.The evaluation of direct and indirect exposure was based on the analysis of the ultraviolet spectrum from the absorbance spectra of the organic compound dye called benzene sulfonate(C(16)H(11)N2Na O4S)and of viable cells called S.aureus.Organic compounds were degraded and viable cells were killed in a short time by thermal plasma.Moreover,analyses of total carbon,total organic carbon,and total inorganic carbon showed a fast decrease in organically bound carbon,however,this was not as fast as the absorbance spectra revealed by the exposure time increasing more for direct exposure than indirect exposure.After 100 s of exposure to the organic compound dye the removal had a maximun of 40%for samples with indirect exposure to the plasma and a maximum of 90%for samples with the direct exposure.For both samples,where some organic contaminants still remained in treated water,four electrolytes(KCl,Na Cl,Na2SO4,and CH3COONa)were added to be effective for complete sterilization,reaching a purity of 100%.A proposal is made for an optimized thermal plasma water purification system(TPWPS)to improve fast inactivation of microbes and the degradation of organic compounds dissolved in water(especially for direct exposure rather than indirect exposure)using a hybrid plasma torch with an electrical power of 125 kW(500 V–250 A)producing a high-temperature(10 000 K–19 000 K)plasma jet with a maximum gas consumption of 28 mg s^-1.
基金supported by the National Key Research and Development Program of China (Project No.2018YFB1502903)。
文摘Metal-based perovskite oxides have contributed significantly to the advanced oxidation processes(AOPs)due to their diverse active sites and excellent compositional/structural flexibility.In this study,we specially designed a perovskite oxide with abundant oxygen vacancies,SrCo_(0.8)Fe_(0.2)O_(3)(SCF),and firstly applied it as a catalyst in peroxymonosulfate(PMS) activation towards organic pollutants degradation.The result revealed that the prepared SCF catalyst exhibited excellent performance on organic compounds degradation.Besides,SCF showed much better activity than La_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3)(LSCF) in terms of reaction rate and stability for the degradation of the organic compounds.Based on the analysis of scanning electron microscope,transmission electron microscope,X-ray diffraction,N_(2) adsorption-desorption,X-ray photoelectron spectroscopy and electron paramagnetic resonance,it was confirmed that the perovskite catalysts with high content of Sr doping at A-site could effectively create a defect-rich surface and optimize its physicochemical properties,which was responsible for the excellent heterogeneous catalytic activity of SCF.SCF can generate three highly active species:~1 O_(2),SO_(4)^(-)· and ·OH in PMS activation,revealing the degradation process of organic compounds was a coupled multiple active species in both radical and nonradical pathway.Moreover,it was mainly in a radical pathway in the degradation through PMS activation on SCF and SO_(4)^(-)· radicals produced were the dominant species in SCF/PMS system.This study demonstrated that perovskite-type catalysts could enrich OVs efficiently by doping strategy and regulate the PMS activation towards sulfate radical-based AOPs.
基金This work was financially supported by the National Natural Science Foundation of China(NSFC,Grant No.51472194)the NSF of Hubei Province(Grant No.2016CFA078)the National Basic Research Program of China(973 Program,Grant No.2013CB632402).
文摘Photocatalytic oxidation process for the degradation of volatile organic compounds(VOCs)contaminants is a promising technology.But until now,the low photocatalytic activity of the conventional TiO_(2) photocatalyst under visible-light irradia-tion hinders the deployment of this technique for VOCs degradation.WO_(3) has been proved to be a suitable photocatalytic material for degradation of various VOCs as its appropriate band-gap,high stability and great capability.Nevertheless,the actual implementation of WO_(3) is still restricted by short lifetime of photoexcited charge carriers and low light energy conver-sion efficiency:its photocatalytic performance is needed to be improved.This review discusses the process of tungsten-based photocatalyst for removal of VOCs and summarizes a variety of strategies to improve the VOCs oxidation performances of WO_(3),such as controlling the morphology structure,engendering chemical defects,coupling heterojunction,doping suitable dopants and loading a co-catalyst.In addition,the practical application of tungsten-based photocatalyst is discussed.
基金Supported by the National Natural Science Foundation of China(21276013,21676008)Specialized Research Fund for the Doctoral Program of Higher Education of China(20130010110001)
文摘The study herein investigated the effectiveness of simultaneous use of ozone and hydrogen peroxide(O_3/H_2O_2 process) to degrade o-phenylenediamine(o-PDA) in a simulated wastewater. A rotor–stator reactor(RSR) was employed to create a high-gravity environment in order to enhance ozone-liquid mass transfer rate and possibly improve the degradation rate of o-PDA. The degradation efficiency of o-PDA(η) as well as the overall gas-phase volumetric mass transfer coefficient(KGa) were determined under different operating conditions of H_2O_2 concentration, initial o-PDA concentration, temperature of reaction, initial p H and rotation speed of RSR in attempt to establish the optimal conditions. Chemical oxygen demand reduction rate(rCOD) of wastewater treated at a particular set of conditions was also analyzed. Additionally, the intermediate products of degradation were identified using a gas chromatography-mass spectrometer(GC/MS) to further evaluate the extent of o-PDA degradation as well as establish its possible degradation pathway. Results were validated by comparison with those of sole use of ozone(O_3 process), and it was noted that η, KGa and rCODachieved by O_3/H_2O_2 process was 24.4%,31.6% and 25.2% respectively higher than those of O_3 process, indicating that H_2O_2 can greatly enhance ozonation of o-PDA. This work further demonstrates that an RSR can significantly intensify ozone-liquid mass transfer rate and thus provides a feasible intensification means for the ozonation of o-PDA as well as other recalcitrant organics.
基金supported by the National Natural Science Foundation of China (No. 51108006)Ph.D. Programs Foundation of the Ministry of Education of China (No. 20111103120008)the State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex
文摘A field measurement campaign for ozone and ozone precursors (VOCs and NOx) was conducted in summer 2011 around a petroleum refinery in the Beijing rural region. Three observation sites were arranged, one at southwest of the refinery as the background, and two at northeast of the refinery as the downwind receptors. Monitoring data revealed the presence of serious surface 03 pollution with the characteristics of high average daily mean and maximum concentrations (64.0 and 145.4 ppbV in no-rain days, respectively) and multi-peak diurnal variation. For NOx, the average hourly concentrations of NO2 and NO were in the range of 20.546.1 and 1.8-6.4 ppbV, respectively. For VOC measurement, a total of 51 compounds were detected. Normally, TVOCs at the background site was only dozens of ppbC, while TVOCs at the downwind sites reached several hundreds of ppbC. By subtracting the VOC concentrations at background, chemical profiles of VOC emission from the refinery were obtained, mainly including alkanes (60.0% ± 4.3%), alkenes (21.1% ± 5.5%) and aromatics (18.9% ±3.9%). Moreover, some differences in chemical profiles for the same measurement hours were observed between the downwind sites; the volume ratios of alkanes with low reactivity and those of alkenes with high reactivity respectively showed an increasing trend and a decreasing trend. Finally, based on temporal and spatial variations of VOC mixing ratios, their photochemical degradations and dispersion degradations were estimated to be 0.15-0.27 and 0.42-0.62, respectively, by the photochemical age calculation method, indicating stronger photochemical reactions around the refinery.