The problem of water and sulfur poisoning in flue gas atmosphere remains a significant obstacle for low-temperature deNOx catalysts.This study investigated the sulfation mechanism of the CoMn2O4/CeTiOx(CMC...The problem of water and sulfur poisoning in flue gas atmosphere remains a significant obstacle for low-temperature deNOx catalysts.This study investigated the sulfation mechanism of the CoMn2O4/CeTiOx(CMCT)catalyst during the selective catalytic reduction of NOx with NH3 under conditions containing H2O and SO2 at 150℃.Employing a comprehensive suite of time-resolved analysis and characterization techniques,the evolution of sulfate species was systematically categorized into three stages:initial rapid surface sulfate accumulation,the transformation of surface sulfates to bulk metal sulfates,and partial sulfates decomposition after the removal of H2O and SO2.These findings indicate that bulk metal sulfates irreversibly deactivate the catalyst by distorting active component lattices and consuming oxygen vacancies,whereas surface sulfates(including ammonium sulfates and surface-coordinated metal sulfates)cause reversible performance loss through decomposition.Furthermore,the competitive adsorption of H2O and SO2 significantly influences the catalytic efficiency,with H2O suppressing SO2 adsorption while simultaneously enhancing the formation of Brönsted acid sites.This research underscores the critical role of sulfate dynamics on catalyst performance,revealing the enhanced SO2 resistance of the Eley-Rideal mechanism facilitated by the Ce-Ti support relative to the Langmuir-Hinshelwood pathway.Collectively,the study unravels the complex interplay of sulfate dynamics influencing catalyst performance and provides potential approaches to mitigate deactivation in demanding atmospheric conditions.展开更多
The removal of four dissolved organic matter(DOM) fractions, non-acid hydrophobics,hydrophobic acids, hydrophilics and transphilics, was achieved by coagulation-UV/H_2O_2 oxidation in post-pharmaceutical wastewater(Ph...The removal of four dissolved organic matter(DOM) fractions, non-acid hydrophobics,hydrophobic acids, hydrophilics and transphilics, was achieved by coagulation-UV/H_2O_2 oxidation in post-pharmaceutical wastewater(PhW W). Coagulation with Polyferric chloride(PFC), Polymeric ferric sulfate(PFS) and Polymeric aluminum ferric chloride(PAFC) was studied separately to evaluate the effects of the initial pH and coagulant dosage. The coagulation-UV/H_2O_2 oxidation method resulted in much higher reduction rates for dissolved organic carbon(DOC)(by 75%) and UV254(by 92%) than coagulation or UV/H_2O_2 oxidation alone. The proportion of non-acid hydrophobics, hydrophobic acids, transphilics and hydrophilics removed by coagulation was 54%, 49%, 27% and 12 %, while the combined treatment removed 92%, 87%,70% and 39%, respectively. Parallel factor analysis(PARAFAC) of fluorescence measurements revealed that the humic-like fluorescent component C4 showed the highest removal(by 44%)during the coagulation stage. After coagulation-UV/H_2O_2 treatment, the humic-like fluorescent component C3 had the highest removal(by 72%), whereas xenobiotic organic fluorescent components C1 and C4 remained recalcitrant to decomposition. Significant correlations(R2> 0.8)between C1 and the hydrophobic acids and non-acid hydrophobics suggested the possibility of using fluorescence spectroscopy as an effective tool to assess variations in DOM fraction treatment efficacy in coagulation-UV/H_2O_2 systems. After the combined treatment, toxic inhibition of cellular activity by post PhW W decreased from 88% to 47% and biodegradability increased from 0.1 to 0.52.展开更多
Excessive exposure to ultraviolet(UV)radiation harms humans and ecosystems.The level of surface UV radiation had increased due to declines in stratospheric ozone in the late 1970s in response to emissions of chloroflu...Excessive exposure to ultraviolet(UV)radiation harms humans and ecosystems.The level of surface UV radiation had increased due to declines in stratospheric ozone in the late 1970s in response to emissions of chlorofluorocarbons.Following the implementation of the Montreal Protocol,the stratospheric loading of chlorine/bromine peaked in the late 1990s and then decreased;subsequently,stratospheric ozone and surface UV radiation would be expected to recover and decrease,respectively.Here,we show,based on multiple data sources,that the May–September surface UV radiation in the tropics and Northern Hemisphere mid-latitudes has undergone a statistically significant increasing trend[about 60.0 J m–2(10 yr)–1]at the 2σlevel for the period 2010–20,due to the onset of total column ozone(TCO)depletion[about−3.5 DU(10 yr)–1].Further analysis shows that the declines in stratospheric ozone after 2010 could be related to an increase in stratospheric nitrogen oxides due to increasing emissions of the source gas nitrous oxide(N2O).展开更多
The degradation of Microcystin-LR (MC-LR) in water by hydrogen peroxide assisted ultraviolet (UV/H2O2) process was investigated in this paper. The UV/H2O2 process appeared to be effective in removal of the MC-LR. MC-L...The degradation of Microcystin-LR (MC-LR) in water by hydrogen peroxide assisted ultraviolet (UV/H2O2) process was investigated in this paper. The UV/H2O2 process appeared to be effective in removal of the MC-LR. MC-LR decomposition was primarily ascribed to production of strong and nonselective oxidant-hydroxyl radicals within the system. The intensity of UV radiation, initial concentration of MC-LR, MC-LR purity, dosages of H2O2, the initial solution pH, and anions present in water, to some extent, influenced the degradation rate of MC-LR. A modified pseudo-first-order kinetic model was developed to predict the removal efficiency under different experimental conditions.展开更多
The experiments were performed to investigate the degradation of microcystins in order to assess the effectiveness and feasibility of UV/H2O2 system for the disinfection of water polluted by microcystins. The influenc...The experiments were performed to investigate the degradation of microcystins in order to assess the effectiveness and feasibility of UV/H2O2 system for the disinfection of water polluted by microcystins. The influence factors such as H2O2, pH and UV light intensities were investigated respectively. Degradation of microcystin-RR (MC-RR) could be fitted by either the pseudo-first-order or second-order rate equations. This homogenous system could significantly enhance the degradation rate due to the synergetic effect between UV and H2O2. The degradation mainly followed the mechanism of direct photolysis and .OH oxidation reactions. Experimental results showed that 94.83% of MC-RR was removed under optimal experimental conditions and the UV/H2O2 system provided an alternative to promote the removal of microcystins in drinking water supplies.展开更多
The batch photodegradation reactor was used to investigate the influence of the common coexisting substances in wastewater,such as H+,anions (HCO3-,Cl-and NO3-) and organic compounds (methanol and bisphenol A),on the ...The batch photodegradation reactor was used to investigate the influence of the common coexisting substances in wastewater,such as H+,anions (HCO3-,Cl-and NO3-) and organic compounds (methanol and bisphenol A),on the photodegradation behaviors of EE2 in the UV/H2O2 process.The results indicated that the addition of coexisting substances can influence the photodegradation behaviors of EE2 and it also follows the first-order kinetics.The acidic (pH 2-4) and alkaline (pH 10-12) medium benefit the photodegradation of EE2,but the photodegradation rate constant of EE2 keeps almost constant in the pH value of 4-10.The addition of anions,such as HCO3-,Cl-and NO3-,can inhibit the photodegradation of EE2,and the rate constant has a negative linear relationship with the concentration of the anions.However,the reduction degrees vary with the anions kinds,and the inhibition effect of the three anions is in the order of HCO3->NO3->Cl-.Addition of 5 mg/L methanol and bisphenol A can reduce the photodegradation rate constant of EE2by 84.31% and 72%,respectively.By comparison,the retardant effect of methanol is much more evident.In the studied concentrations range,the photodegradation rate constant of EE2 is the unary quadratic function of the organic compounds concentrations.展开更多
The degradation of formaldehyde gas was studied using UV/TiO2/O3 process under the condition of continuous flow mode. The effects of humidity, initial formaldehyde concentration, residence time and ozone adding amount...The degradation of formaldehyde gas was studied using UV/TiO2/O3 process under the condition of continuous flow mode. The effects of humidity, initial formaldehyde concentration, residence time and ozone adding amount on degradation of formaldehyde gas were investigated. The experimental results indicated that the combination of ozonation with photocatalytic oxidation on the degradation of formaldehyde showed a synergetic action, e.g,, it could considerably increase decomposing of formaldehyde. The degradation efficiency of formaldehyde was between 73.6% and 79.4% while the initial concentration in the range of 1.84--24 mg/m^3 by O3/TiO2flJV process. The optimal humidity was about 50% in UV/TiO2/O3 processs and degradation of formaldehyde increases from 39.0% to 94.1% when the ozone content increased from 0 to 141 mg/m^3. Furthermore, the kinetics of formaldehyde degradation reaction could be described by Langmuir-Hinshelwood model. The rate constant k of 46.72 mg/(m^3.min) and Langmuir adsorption coefficient K of 0.0268 m^3/mg were obtained.展开更多
[Objective] The paper aimed to study on the effects of photocatalytic degradation of microcystins MC-RR and MC-LR by UV/Fenton/TiO2 in depth lake water.[Method] With Fenton-TiO2 as photocatalyst,the influences of diff...[Objective] The paper aimed to study on the effects of photocatalytic degradation of microcystins MC-RR and MC-LR by UV/Fenton/TiO2 in depth lake water.[Method] With Fenton-TiO2 as photocatalyst,the influences of different reaction time,initial pH value,H2O2 concentration,Fe2+ concentration,TiO2 dosage,light intensity,initial concentration of microcystin on UV/Fenton/TiO2 heterogeneous photocatalytic degradation of microcystin were investigated,and removal effects of microcystin between heterogeneous photocatalytic degradation and UV photolysis were compared at the same time.[Result] Under the conditions that the initial concentration of H2O2 was 0.1 mmol/L,[H2O2]/[FeSO4] was 15:1,pH value was 4.0,the distance between the reaction solution and UV lamp tube was 1 cm,TiO2 dosage was 0.05 g/L,reaction temperature was (16±2) ℃,the removal rate of MC-RR with concentration of 0.35 mg/L and MC-LR with concentration of 0.29 mg/L could reach 91.5% and 90.2% after 3 minutes reacting.[Conclusion] UV/Fenton/TiO2 photocatalytic oxidation was proved to be effective in degradating microcystins.展开更多
Photodegradation of nitrobenzene and nitrophenols in aqueous solutions by means of UV/H2 O2 process was studied in the Rayox batch reactors. Three nitrophenol isomers were identified as main photoproducts in the irrad...Photodegradation of nitrobenzene and nitrophenols in aqueous solutions by means of UV/H2 O2 process was studied in the Rayox batch reactors. Three nitrophenol isomers were identified as main photoproducts in the irradiated NB aqueous solutions. The distribution of nitrophenol isomers follows the order p-〉 m-〉 o-nitrophenol. Other intermediates detected include nitrohydroquinone, nitrocatechol, catechol, benzoquinone, phenol, nitrateitrite ions, formic acid, glyoxylic acid, maleic acid, oxalic acid and some aliphatic ketones and aldehydes. The degradation of nitrobenzene and nitrophenols at initial stages follows the first-order kinetics and the decay rate constants for nitrobenzene(NB) are around l0^-3-10^-2 s^-1 and for nitrophenols are around 10^-2 s^-1. The decomposition of H2 O2 in the presence of NB and each nitrophenol isomers follows zero-order kinetics. The quantum yields at initial stages for NB decay were estimated around 0.30 to 0.36, and for NPs decay is around 0.31-0.54.展开更多
Nitric oxide(NO) from flue gas is hard to remove because of low solubility and reactivity. A new technology for photocatalytic oxidation of NO using ultraviolet(UV)/TiO2/H2O2 process is studied in an efficient laborat...Nitric oxide(NO) from flue gas is hard to remove because of low solubility and reactivity. A new technology for photocatalytic oxidation of NO using ultraviolet(UV)/TiO2/H2O2 process is studied in an efficient laboratory-scale reactor. Effects of several key operational parameters on NO removal efficiency are studied, including TiO2 content, H2O2 initial concentration, UV lamp power, NO initial content, oxygen volume fraction and TiO2/H2O2 solution volume. The results illustrate that the NO removal efficiency increases with the increasing of H2O2 initial concentration or UV lamp power. Meanwhile, a lower NO initial content or a higher TiO2/H2O2 solution volume will result in higher NO removal efficiency. In addition, oxygen volume fraction has a little effect.The highest NO removal efficiency is achieved at the TiO2 content of 0.75 g/L, H2O2 initial concentration of 2.5 mol/L, UV lamp power of 36 W, NO initial content of 206×10-6 and TiO2/H2O2 solution volume of 600 m L. It is beneficial for the development and application of NO removal from coal-fired flue gas with UV/TiO2/H2O2 process.展开更多
The comparison of degradation of Acid Yellow 61 as a model dye compound in both oxidation processes of H 2O 2/UV and O 3 has been studied. When the decolorization rate of Acid Yellow 61 in both reactions presented sim...The comparison of degradation of Acid Yellow 61 as a model dye compound in both oxidation processes of H 2O 2/UV and O 3 has been studied. When the decolorization rate of Acid Yellow 61 in both reactions presented similar, it was found there are some differences from the results of AOX removal and production of inorganic ions and organic acids. The results reveal that the H 2O 2/UV has beneficial effect on mineralization than O 3 only for degradation of Acid Yellow 61 solution and it is possible for enhancement of method efficiency by taking longer reaction time and addition of high concentration of oxidants.展开更多
Three types of simulated commercial reactive dye wastewater, separately prepared with FN-2BL red, C-R blue and C-2R yellow, were oxidized with UV/ferrioxalate/H2O2 system, especially by the introduction of Fe2+ ion. T...Three types of simulated commercial reactive dye wastewater, separately prepared with FN-2BL red, C-R blue and C-2R yellow, were oxidized with UV/ferrioxalate/H2O2 system, especially by the introduction of Fe2+ ion. The experimental results show that the optimized experimental conditions are pH=3.5, [Fe2+]=1mM, H2O2782mg/L for FN-2BL red and C-R blue and H2O2646mg/L for C-2R yellow, t=4h and T=80℃ when the concentration of dye is 400mg/L. Under such conditions, the observed COD and color removal efficiencies are above 94% and 99%, respectively for all the cases. This investigation has provided fundamental information for the treatment of wastewater containing reactive dyes using UV/ferrioxalate/H2O2.展开更多
The degradation of atrazine(ATZ),sulfamethoxazole(SMX)and metoprolol(MET)in flowthrough VUV/UV/H2O2reactors was investigated with a focus on the effects of H2O2dosage and reactor internal diameter(ID).Results showed t...The degradation of atrazine(ATZ),sulfamethoxazole(SMX)and metoprolol(MET)in flowthrough VUV/UV/H2O2reactors was investigated with a focus on the effects of H2O2dosage and reactor internal diameter(ID).Results showed that the micropollutants were degraded efficiently in the flow-through VUV/UV/H2O2reactors following the pseudo first-order kinetics(R2>0.92).However,the steady-state assumption(SSA)kinetic model being vital in batch reactors was found invalid in flow-through reactors where fluid mixing was less sufficient.With the increase of H2O2dosage,the ATZ removal efficiency remained almost constant while the SMX and MET removal was enhanced to different extents,which could be explained by the different reactivities of the pollutants towards HO·.A larger reactor ID resulted in lower degradation rate constants for all the three pollutants on account of the lower average fluence rate,but the change in energy efficiency was much more complicated.In reality,the electrical energy per order(EEO)of the investigated VUV/UV/H2O2treatments ranged between 0.14–0.20,0.07–0.14 and 0.09–0.26 k Wh/m3/order for ATZ,SMX and MET,respectively,with the lowest EEOfor each pollutant obtained under varied H2O2dosages and reactor IDs.This study has demonstrated the efficiency of VUV/UV/H2O2process for micropollutant removal and the inadequacy of the SSA model in flow-through reactors,and elaborated the influential mechanisms of H2O2dosage and reactor ID on the reactor performances.展开更多
Tri(2-chloroethyl) phosphate(TCEP) with the initial concentration of 5 mg/L was degraded by UV/H2O2 oxidation process. The removal rate of TCEP in the UV/H2O2 system was 89.1% with the production of Cl-and PO4^3- of 0...Tri(2-chloroethyl) phosphate(TCEP) with the initial concentration of 5 mg/L was degraded by UV/H2O2 oxidation process. The removal rate of TCEP in the UV/H2O2 system was 89.1% with the production of Cl-and PO4^3- of 0.23 and 0.64 mg/L. The removal rate of total organic carbon of the reaction was 48.8% and the pH reached 3.3 after the reaction. The oxidative degradation process of TCEP in the UV/H2O2 system obeyed the first order kinetic reaction with the apparent rate constant of 0.0025 min^-1( R^2 = 0.9788). The intermediate products were isolated and identified by gas chromatography-mass spectrometer. The addition reaction of HO · and H2O and the oxidation reaction with H2O2 were found during the degradation pathway of 5 mg/L TCEP in the UV/H2O2 system. For the first time, environment risk was estimated via the "ecological structure activity relationships" program and acute and chronic toxicity changes of intermediate products were pointed out. The luminescence inhibition rate of photobacterium was used to evaluate the acute toxicity of intermediate products. The results showed that the toxicity of the intermediate products increased with the increase of reaction time, which may be due to the production of chlorine compounds. Some measures should be introduced to the UV/H2O2 system to remove the highly toxic Cl-containing compounds, such as a nanofiltration or reverse osmosis unit.展开更多
摘要The problem of water and sulfur poisoning in flue gas atmosphere remains a significant obstacle for low-temperature deNOx catalysts.This study investigated the sulfation mechanism of the CoMn2O4/CeTiOx(CMCT)catalyst during the selective catalytic reduction of NOx with NH3 under conditions containing H2O and SO2 at 150℃.Employing a comprehensive suite of time-resolved analysis and characterization techniques,the evolution of sulfate species was systematically categorized into three stages:initial rapid surface sulfate accumulation,the transformation of surface sulfates to bulk metal sulfates,and partial sulfates decomposition after the removal of H2O and SO2.These findings indicate that bulk metal sulfates irreversibly deactivate the catalyst by distorting active component lattices and consuming oxygen vacancies,whereas surface sulfates(including ammonium sulfates and surface-coordinated metal sulfates)cause reversible performance loss through decomposition.Furthermore,the competitive adsorption of H2O and SO2 significantly influences the catalytic efficiency,with H2O suppressing SO2 adsorption while simultaneously enhancing the formation of Brönsted acid sites.This research underscores the critical role of sulfate dynamics on catalyst performance,revealing the enhanced SO2 resistance of the Eley-Rideal mechanism facilitated by the Ce-Ti support relative to the Langmuir-Hinshelwood pathway.Collectively,the study unravels the complex interplay of sulfate dynamics influencing catalyst performance and provides potential approaches to mitigate deactivation in demanding atmospheric conditions.
基金supported by the National Key Scientific and Technological Project for Water Pollution Control and Management (Nos.2012ZX07202-005,2012ZX07202-002,2014 ZX07216001-2)
摘要The removal of four dissolved organic matter(DOM) fractions, non-acid hydrophobics,hydrophobic acids, hydrophilics and transphilics, was achieved by coagulation-UV/H_2O_2 oxidation in post-pharmaceutical wastewater(PhW W). Coagulation with Polyferric chloride(PFC), Polymeric ferric sulfate(PFS) and Polymeric aluminum ferric chloride(PAFC) was studied separately to evaluate the effects of the initial pH and coagulant dosage. The coagulation-UV/H_2O_2 oxidation method resulted in much higher reduction rates for dissolved organic carbon(DOC)(by 75%) and UV254(by 92%) than coagulation or UV/H_2O_2 oxidation alone. The proportion of non-acid hydrophobics, hydrophobic acids, transphilics and hydrophilics removed by coagulation was 54%, 49%, 27% and 12 %, while the combined treatment removed 92%, 87%,70% and 39%, respectively. Parallel factor analysis(PARAFAC) of fluorescence measurements revealed that the humic-like fluorescent component C4 showed the highest removal(by 44%)during the coagulation stage. After coagulation-UV/H_2O_2 treatment, the humic-like fluorescent component C3 had the highest removal(by 72%), whereas xenobiotic organic fluorescent components C1 and C4 remained recalcitrant to decomposition. Significant correlations(R2> 0.8)between C1 and the hydrophobic acids and non-acid hydrophobics suggested the possibility of using fluorescence spectroscopy as an effective tool to assess variations in DOM fraction treatment efficacy in coagulation-UV/H_2O_2 systems. After the combined treatment, toxic inhibition of cellular activity by post PhW W decreased from 88% to 47% and biodegradability increased from 0.1 to 0.52.
基金Funding for this work was provided by the National Natural Science Foundation of China(Grant Nos.42122037,42105016,41975047).
摘要Excessive exposure to ultraviolet(UV)radiation harms humans and ecosystems.The level of surface UV radiation had increased due to declines in stratospheric ozone in the late 1970s in response to emissions of chlorofluorocarbons.Following the implementation of the Montreal Protocol,the stratospheric loading of chlorine/bromine peaked in the late 1990s and then decreased;subsequently,stratospheric ozone and surface UV radiation would be expected to recover and decrease,respectively.Here,we show,based on multiple data sources,that the May–September surface UV radiation in the tropics and Northern Hemisphere mid-latitudes has undergone a statistically significant increasing trend[about 60.0 J m–2(10 yr)–1]at the 2σlevel for the period 2010–20,due to the onset of total column ozone(TCO)depletion[about−3.5 DU(10 yr)–1].Further analysis shows that the declines in stratospheric ozone after 2010 could be related to an increase in stratospheric nitrogen oxides due to increasing emissions of the source gas nitrous oxide(N2O).
基金supported by the National Key Technologies Supporting Program of China during the 11th Five-Year Plan Period (No. 2006BAJ08B06)the National Major Project of Science & Technology Ministry of China (No. 2008ZX07421-002)the Shanghai Science & Technology Commission Key Scientific & Technological Project (No. 072312001), China
摘要The degradation of Microcystin-LR (MC-LR) in water by hydrogen peroxide assisted ultraviolet (UV/H2O2) process was investigated in this paper. The UV/H2O2 process appeared to be effective in removal of the MC-LR. MC-LR decomposition was primarily ascribed to production of strong and nonselective oxidant-hydroxyl radicals within the system. The intensity of UV radiation, initial concentration of MC-LR, MC-LR purity, dosages of H2O2, the initial solution pH, and anions present in water, to some extent, influenced the degradation rate of MC-LR. A modified pseudo-first-order kinetic model was developed to predict the removal efficiency under different experimental conditions.
摘要The experiments were performed to investigate the degradation of microcystins in order to assess the effectiveness and feasibility of UV/H2O2 system for the disinfection of water polluted by microcystins. The influence factors such as H2O2, pH and UV light intensities were investigated respectively. Degradation of microcystin-RR (MC-RR) could be fitted by either the pseudo-first-order or second-order rate equations. This homogenous system could significantly enhance the degradation rate due to the synergetic effect between UV and H2O2. The degradation mainly followed the mechanism of direct photolysis and .OH oxidation reactions. Experimental results showed that 94.83% of MC-RR was removed under optimal experimental conditions and the UV/H2O2 system provided an alternative to promote the removal of microcystins in drinking water supplies.
基金Sponsored by the Key Project of National Science Foundation of China (Grant NO.50638020)the National High Technology Research and Development Program of China (Grant No.2007AA06A411)the State Key Laboratory of Urban Water Resource & Environment (Grant No.2009TS04)
摘要The batch photodegradation reactor was used to investigate the influence of the common coexisting substances in wastewater,such as H+,anions (HCO3-,Cl-and NO3-) and organic compounds (methanol and bisphenol A),on the photodegradation behaviors of EE2 in the UV/H2O2 process.The results indicated that the addition of coexisting substances can influence the photodegradation behaviors of EE2 and it also follows the first-order kinetics.The acidic (pH 2-4) and alkaline (pH 10-12) medium benefit the photodegradation of EE2,but the photodegradation rate constant of EE2 keeps almost constant in the pH value of 4-10.The addition of anions,such as HCO3-,Cl-and NO3-,can inhibit the photodegradation of EE2,and the rate constant has a negative linear relationship with the concentration of the anions.However,the reduction degrees vary with the anions kinds,and the inhibition effect of the three anions is in the order of HCO3->NO3->Cl-.Addition of 5 mg/L methanol and bisphenol A can reduce the photodegradation rate constant of EE2by 84.31% and 72%,respectively.By comparison,the retardant effect of methanol is much more evident.In the studied concentrations range,the photodegradation rate constant of EE2 is the unary quadratic function of the organic compounds concentrations.
基金Project supported by the Science Project of Harbin City(No. H2001-12)the Youth Foundation of School of Municipal and Environmental Engineering in Harbin Institute of Technology(No. 01306914).
摘要The degradation of formaldehyde gas was studied using UV/TiO2/O3 process under the condition of continuous flow mode. The effects of humidity, initial formaldehyde concentration, residence time and ozone adding amount on degradation of formaldehyde gas were investigated. The experimental results indicated that the combination of ozonation with photocatalytic oxidation on the degradation of formaldehyde showed a synergetic action, e.g,, it could considerably increase decomposing of formaldehyde. The degradation efficiency of formaldehyde was between 73.6% and 79.4% while the initial concentration in the range of 1.84--24 mg/m^3 by O3/TiO2flJV process. The optimal humidity was about 50% in UV/TiO2/O3 processs and degradation of formaldehyde increases from 39.0% to 94.1% when the ozone content increased from 0 to 141 mg/m^3. Furthermore, the kinetics of formaldehyde degradation reaction could be described by Langmuir-Hinshelwood model. The rate constant k of 46.72 mg/(m^3.min) and Langmuir adsorption coefficient K of 0.0268 m^3/mg were obtained.
基金Supported by the Social Development Scientific and Technolgical Project[GKHS-2007-1007]The Special Funds for Top Talents [GSZH-2007-108]The Special Project for Improving Researeh Conditionsof Guizhou [TZJF-2007-15]
摘要[Objective] The paper aimed to study on the effects of photocatalytic degradation of microcystins MC-RR and MC-LR by UV/Fenton/TiO2 in depth lake water.[Method] With Fenton-TiO2 as photocatalyst,the influences of different reaction time,initial pH value,H2O2 concentration,Fe2+ concentration,TiO2 dosage,light intensity,initial concentration of microcystin on UV/Fenton/TiO2 heterogeneous photocatalytic degradation of microcystin were investigated,and removal effects of microcystin between heterogeneous photocatalytic degradation and UV photolysis were compared at the same time.[Result] Under the conditions that the initial concentration of H2O2 was 0.1 mmol/L,[H2O2]/[FeSO4] was 15:1,pH value was 4.0,the distance between the reaction solution and UV lamp tube was 1 cm,TiO2 dosage was 0.05 g/L,reaction temperature was (16±2) ℃,the removal rate of MC-RR with concentration of 0.35 mg/L and MC-LR with concentration of 0.29 mg/L could reach 91.5% and 90.2% after 3 minutes reacting.[Conclusion] UV/Fenton/TiO2 photocatalytic oxidation was proved to be effective in degradating microcystins.
摘要Photodegradation of nitrobenzene and nitrophenols in aqueous solutions by means of UV/H2 O2 process was studied in the Rayox batch reactors. Three nitrophenol isomers were identified as main photoproducts in the irradiated NB aqueous solutions. The distribution of nitrophenol isomers follows the order p-〉 m-〉 o-nitrophenol. Other intermediates detected include nitrohydroquinone, nitrocatechol, catechol, benzoquinone, phenol, nitrateitrite ions, formic acid, glyoxylic acid, maleic acid, oxalic acid and some aliphatic ketones and aldehydes. The degradation of nitrobenzene and nitrophenols at initial stages follows the first-order kinetics and the decay rate constants for nitrobenzene(NB) are around l0^-3-10^-2 s^-1 and for nitrophenols are around 10^-2 s^-1. The decomposition of H2 O2 in the presence of NB and each nitrophenol isomers follows zero-order kinetics. The quantum yields at initial stages for NB decay were estimated around 0.30 to 0.36, and for NPs decay is around 0.31-0.54.
基金Project(2011CB201505)supported by the National Key Basic Research Program of ChinaProject(BA2011031)supported by the Special Fund of Transformation of Scientific and Technological Achievements of Jiangsu Province,China
摘要Nitric oxide(NO) from flue gas is hard to remove because of low solubility and reactivity. A new technology for photocatalytic oxidation of NO using ultraviolet(UV)/TiO2/H2O2 process is studied in an efficient laboratory-scale reactor. Effects of several key operational parameters on NO removal efficiency are studied, including TiO2 content, H2O2 initial concentration, UV lamp power, NO initial content, oxygen volume fraction and TiO2/H2O2 solution volume. The results illustrate that the NO removal efficiency increases with the increasing of H2O2 initial concentration or UV lamp power. Meanwhile, a lower NO initial content or a higher TiO2/H2O2 solution volume will result in higher NO removal efficiency. In addition, oxygen volume fraction has a little effect.The highest NO removal efficiency is achieved at the TiO2 content of 0.75 g/L, H2O2 initial concentration of 2.5 mol/L, UV lamp power of 36 W, NO initial content of 206×10-6 and TiO2/H2O2 solution volume of 600 m L. It is beneficial for the development and application of NO removal from coal-fired flue gas with UV/TiO2/H2O2 process.
摘要The comparison of degradation of Acid Yellow 61 as a model dye compound in both oxidation processes of H 2O 2/UV and O 3 has been studied. When the decolorization rate of Acid Yellow 61 in both reactions presented similar, it was found there are some differences from the results of AOX removal and production of inorganic ions and organic acids. The results reveal that the H 2O 2/UV has beneficial effect on mineralization than O 3 only for degradation of Acid Yellow 61 solution and it is possible for enhancement of method efficiency by taking longer reaction time and addition of high concentration of oxidants.
摘要Three types of simulated commercial reactive dye wastewater, separately prepared with FN-2BL red, C-R blue and C-2R yellow, were oxidized with UV/ferrioxalate/H2O2 system, especially by the introduction of Fe2+ ion. The experimental results show that the optimized experimental conditions are pH=3.5, [Fe2+]=1mM, H2O2782mg/L for FN-2BL red and C-R blue and H2O2646mg/L for C-2R yellow, t=4h and T=80℃ when the concentration of dye is 400mg/L. Under such conditions, the observed COD and color removal efficiencies are above 94% and 99%, respectively for all the cases. This investigation has provided fundamental information for the treatment of wastewater containing reactive dyes using UV/ferrioxalate/H2O2.
基金supported by the National Natural Science Foundation of China(No.51908536)the Ministry of Science and Technology of China(No.2018YFE0204103)。
摘要The degradation of atrazine(ATZ),sulfamethoxazole(SMX)and metoprolol(MET)in flowthrough VUV/UV/H2O2reactors was investigated with a focus on the effects of H2O2dosage and reactor internal diameter(ID).Results showed that the micropollutants were degraded efficiently in the flow-through VUV/UV/H2O2reactors following the pseudo first-order kinetics(R2>0.92).However,the steady-state assumption(SSA)kinetic model being vital in batch reactors was found invalid in flow-through reactors where fluid mixing was less sufficient.With the increase of H2O2dosage,the ATZ removal efficiency remained almost constant while the SMX and MET removal was enhanced to different extents,which could be explained by the different reactivities of the pollutants towards HO·.A larger reactor ID resulted in lower degradation rate constants for all the three pollutants on account of the lower average fluence rate,but the change in energy efficiency was much more complicated.In reality,the electrical energy per order(EEO)of the investigated VUV/UV/H2O2treatments ranged between 0.14–0.20,0.07–0.14 and 0.09–0.26 k Wh/m3/order for ATZ,SMX and MET,respectively,with the lowest EEOfor each pollutant obtained under varied H2O2dosages and reactor IDs.This study has demonstrated the efficiency of VUV/UV/H2O2process for micropollutant removal and the inadequacy of the SSA model in flow-through reactors,and elaborated the influential mechanisms of H2O2dosage and reactor ID on the reactor performances.
基金supported by the National Nature Science Foundation of China (No. 21777067)the Primary Research&Development Plan of Jiangsu Province (No. BE2019679)+1 种基金Open Fund of National Key Laboratory of Collaborative Control and Remediation of Soil and Water Pollution for Environmental Protection (No. GHBK-001)the Open Fund of the State Environmental Protection Key Laboratory of Wetland Ecology and Vegetation Restoration,Northeast Normal University (No. 130028903)。
摘要Tri(2-chloroethyl) phosphate(TCEP) with the initial concentration of 5 mg/L was degraded by UV/H2O2 oxidation process. The removal rate of TCEP in the UV/H2O2 system was 89.1% with the production of Cl-and PO4^3- of 0.23 and 0.64 mg/L. The removal rate of total organic carbon of the reaction was 48.8% and the pH reached 3.3 after the reaction. The oxidative degradation process of TCEP in the UV/H2O2 system obeyed the first order kinetic reaction with the apparent rate constant of 0.0025 min^-1( R^2 = 0.9788). The intermediate products were isolated and identified by gas chromatography-mass spectrometer. The addition reaction of HO · and H2O and the oxidation reaction with H2O2 were found during the degradation pathway of 5 mg/L TCEP in the UV/H2O2 system. For the first time, environment risk was estimated via the "ecological structure activity relationships" program and acute and chronic toxicity changes of intermediate products were pointed out. The luminescence inhibition rate of photobacterium was used to evaluate the acute toxicity of intermediate products. The results showed that the toxicity of the intermediate products increased with the increase of reaction time, which may be due to the production of chlorine compounds. Some measures should be introduced to the UV/H2O2 system to remove the highly toxic Cl-containing compounds, such as a nanofiltration or reverse osmosis unit.