Realizing fast and continuous generation of reactive oxygen species(ROSs)via iron-based advanced oxidation processes(AOPs)is significant in the environmental and biological fields.However,current AOPs assisted by co-c...Realizing fast and continuous generation of reactive oxygen species(ROSs)via iron-based advanced oxidation processes(AOPs)is significant in the environmental and biological fields.However,current AOPs assisted by co-catalysts still suffer from the poor mass/electron transfer and non-durable promotion effect,giving rise to the sluggish Fe^(2+)/Fe^(3+)cycle and low dynamic concentration of Fe^(2+)for ROS production.Herein,we present a three-dimensional(3D)macroscale co-catalyst functionalized with molybdenum disulfide(MoS_(2))to achieve ultra-efficient Fe^(2+)regeneration(equilibrium Fe^(2+)ratio of 82.4%)and remarkable stability(more than 20 cycles)via a circulating flow-through process.Unlike the conventional batch-type reactor,experiments and computational fluid dynamics simulations demonstrate that the optimal utilization of the 3D active area under the flow-through mode,initiated by the convectionenhanced mass/charge transfer for Fe^(2+)reduction and then strengthened by MoS_(2)-induced flow rotation for sufficient reactant mixing,is crucial for oxidant activation and subsequent ROS generation.Strikingly,the flow-through co-catalytic system with superwetting capabilities can even tackle the intricate oily wastewater stabilized by different surfactants without the loss of pollutant degradation efficiency.Our findings highlight an innovative co-catalyst system design to expand the applicability of AOPs based technology,especially in large-scale complex wastewater treatment.展开更多
Antibiotic resistant bacteria(ARB)with antibiotic resistance genes(ARGs)can reduce or eliminate the effectiveness of antibiotics and thus threaten human health.The United Nations Environment Programme considers antibi...Antibiotic resistant bacteria(ARB)with antibiotic resistance genes(ARGs)can reduce or eliminate the effectiveness of antibiotics and thus threaten human health.The United Nations Environment Programme considers antibiotic resistance the first of six emerging issues of concern.Advanced oxidation processes(AOPs)that combine ultraviolet(UV)irradiation and chemical oxidation(primarily chlorine,hydrogen peroxide,and persulfate)have attracted increasing interest as advanced water and wastewater treatment technologies.These integrated technologies have been reported to significantly elevate the efficiencies of ARB inactivation and ARG degradation compared with direct UV irradiation or chemical oxidation alone due to the generation of multiple reactive species.In this study,the performance and underlying mechanisms of UV/chlorine,UV/hydrogen peroxide,and UV/persulfate processes for controlling ARB and ARGs were reviewed based on recent studies.Factors affecting the process-specific efficiency in controlling ARB and ARGs were discussed,including biotic factors,oxidant dose,UV fluence,pH,and water matrix properties.In addition,the cost-effectiveness of the UV-based AOPs was evaluated using the concept of electrical energy per order.The UV/chlorine process exhibited a higher efficiency with lower energy consumption than other UV-based AOPs in the wastewater matrix,indicating its potential for ARB inactivation and ARG degradation in wastewater treatment.Further studies are required to address the trade-off between toxic byproduct formation and the energy efficiency of the UV/chlorine process in real wastewater to facilitate its optimization and application in the control of ARB and ARGs.展开更多
Investigation that protein oxidation to the formation of advanced glycation end products(AGEs)after chicken myofibrillar protein glycation is limited.Models of protein oxidation induced by different concentrations of ...Investigation that protein oxidation to the formation of advanced glycation end products(AGEs)after chicken myofibrillar protein glycation is limited.Models of protein oxidation induced by different concentrations of hydroxyl radicals(·OH)were developed after the chicken myofibrillar protein mild glycation(MPG).Results exhibited that levels of AGEs and surface hydrophobicity(H_(0))steadily increased with the a ddition of h ydrogen peroxide(H_(2)O_(2))concentration.However,levels of s ulfhydryl group,free amino group,and particle size gradually decreased with the H_(2)O_(2)concentration.The protein carbonyl value increased in H_(2)O_(2)concentration until 10 mmol/L.Pearson's correlation indicated that MPG structure modification(unfolding and degradation)induced by protein oxidation were significantly positively correlated with AGEs concentration(P<0.05).Finally,a mechanism was proposed to hypothesize t he effect of protein oxidation on the formation of AGEs under MPG conditions.展开更多
This article, for the first time, provides a novel advanced oxidation process based on sulfate radical (SO^4·-) to degrade organic pollutants in wastewater: microwave (MW)-activated persulfate oxidation (AP...This article, for the first time, provides a novel advanced oxidation process based on sulfate radical (SO^4·-) to degrade organic pollutants in wastewater: microwave (MW)-activated persulfate oxidation (APO) with or without active carbon (AC). Azo dye acid Orange 7 (AO7) is used as a model compound to investigate the high reactivity of MW-APO. It is found that AO7 (up to 1000 mg/L) is completely decolorized within 5-7 min under an 800 W MW furnace assisted-APO. In the presence of chloride ion (up to 0.50 mol/L), the decolorization is still 100% completed, though delayed for about 1-2 min. Experiments are made to examine the enhancement by AC. It is exciting to find that the 100% decolorization of AO7 (500 mg/L) is achieved within 3 min by MW-APO using 1.0 g/L AC as catalyst, while the degradation efficiency maintains at 50% by MW energy without persulfate after about 5 min. Besides the destruction of visible light chromophore band of AO7 (484 nm), during MW-APO, two bands in the ultraviolet region (228 nm and 310 nm) are rapidly broken down. The removal of COD is about 83%-95% for 500 mg/L AO7. SO^4·- is identified with quenching studies using specific alcohols. Both SO^4·- and ·OH could degrade AO7, but SO^4·- plays the dominant role. In a word, MW-APO AC is a new catalytic combustion technology for destruction of organic contamination even for high concentration.展开更多
The degradation capacity of advanced oxidants generated from oxygen reduction was investigated in model effluent containing chlorobenzene, aniline and benzene through the advanced oxidation processes(AOPs). Intermedia...The degradation capacity of advanced oxidants generated from oxygen reduction was investigated in model effluent containing chlorobenzene, aniline and benzene through the advanced oxidation processes(AOPs). Intermediate products of the degradation process were determined by GC–MS, and they contributed to specify the degradation pathways of monoaromatic compounds. The study particularly focused on the influence of the dosage of the oxidant, pH and the initial concentration of organic compounds on the degradation effectiveness.When the dosage of oxidant was 4 wt% and the pH was 7, the maximum degradation rates of 74.83% chlorobenzene, 70.32% aniline and 37.69% benzene were achieved. Furthermore, microwave was applied to intensify the oxidation process under optimal operation conditions, and the degradation rates were increased to 87.85% chlorobenzene, 89.11% aniline and 39.03% benzene, respectively.展开更多
In this study,advanced oxidation processes(AOPs) such as anodic oxidation(AO),UV/H_2O_2 and Fenton processes(FP) were investigated for the degradation of salicylic acid(SA) in lab-scale experiments.Boron-doped diamond...In this study,advanced oxidation processes(AOPs) such as anodic oxidation(AO),UV/H_2O_2 and Fenton processes(FP) were investigated for the degradation of salicylic acid(SA) in lab-scale experiments.Boron-doped diamond(BDD) film electrodes using Ta as substrates were employed for AO of SA.In the case of FP and UV/H_2O_2,most favorable experimental conditions were determined for each process and these were used for comparing with AO process.The study showed that the FP was the most effective process under aci...展开更多
The removal of the natural organic matter present in coffee processing wastewater through chemical coagulation-flocculation and advanced oxidation processes (AOP) had been studied. The effectiveness of the removal o...The removal of the natural organic matter present in coffee processing wastewater through chemical coagulation-flocculation and advanced oxidation processes (AOP) had been studied. The effectiveness of the removal of natural organic matter using commercial flocculants and UV/H202, UV/O3 and UV/H2O2/O3 processes was determined under acidic conditions. For each of these processes, different operational conditions were explored to optimize the treatment efficiency of the coffee wastewater. Coffee wastewater is characterized by a high chemical oxygen demand (COD) and low total suspended solids. The outcomes of coffee wastewater treatment using coagulation-flocculation and photodegradation processes were assessed in terms of reduction of COD, color, and turbidity. It was found that a reduction in COD of 67% could be realized when the coffee wastewater was treated by chemical coagulation-flocculation with lime and coagulant T-1. When coffee wastewater was treated by coagulation-flocculation in combination with UV/H2O2, a COD reduction of 86% was achieved, although only after prolonged UV irradiation. Of the three advanced oxidation processes considered, UV/H2O2, UV/O3 and UV/H2O2/O3, we found that the treatment with UV/H2O2/O3 was the most effective, with an efficiency of color, turbidity and further COD removal of 87%, when applied to the flocculated coffee wastewater.展开更多
2,4-Dinitroanisole(DNAN)is an important component of insensitive munitions that is anticipated to replace 2,4,6-trinitrotoluene(TNT)in munitions formulations.Photocatalyzed hydrogen peroxide(H2O2)oxidation experiments...2,4-Dinitroanisole(DNAN)is an important component of insensitive munitions that is anticipated to replace 2,4,6-trinitrotoluene(TNT)in munitions formulations.Photocatalyzed hydrogen peroxide(H2O2)oxidation experiments and chemical analyses were conducted to study the effect of initial pH and H2O2 dosage on the kinetics of DNAN decomposition and the reaction pathways.The results show that DNAN degradation followed zero-order kinetics when a 250 ppm DNAN solution was treated with ultraviolet(UV)light and 1500–4500 ppm H2O2 in an initial pH range of 4–7.However,when the H2O2 concentration was 750 ppm,DNAN degradation followed pseudo-first-order kinetics.The results indicate that DNAN can easily be oxidized by UV/H2O2 treatment.When the H2O2 dosage was 1500 ppm and the initial pH was 7,DNAN was reduced from 250 ppm to less than 1 ppm in 3 h.However,the total organic carbon(TOC)and total carbon(TC)concentrations were reduced slowly from 100 to less than 70 ppm carbon(C)in 3 h,and decreased to about 5 ppm after 9 h of treatment,suggesting the formation of other organic compounds.Those reaction intermediates were oxidized to carbon dioxide(CO2)at a slower rate than the oxidation of DNAN.CO2 was emitted from the solution because the solution pH decreased rapidly to about 3 during the UV/H2O2 oxidation.Most of the nitrogen in DNAN was converted to nitrate by UV/H2O2 oxidation after 9 h of treatment.The research results indicate that UV/H2O2 oxidation is a promising technique for the treatment of DNAN in wastewater.展开更多
A kinetic model has been developed for the degradation of organic pollutants concerning with hydroperoxide ion as the initial step for generation of hydroxyl radical and its subsequent reaction mechanisms. Rate equati...A kinetic model has been developed for the degradation of organic pollutants concerning with hydroperoxide ion as the initial step for generation of hydroxyl radical and its subsequent reaction mechanisms. Rate equations were derived for depletion of ozone and pollutants in the peroxone oxidation process using ozone and hydrogen peroxide as combined oxidants. Kinetic data obtained experimentally from the hydrogen peroxide-ozone reaction and peroxone oxidation of nitrobenzene were analyzed by using the proposed rate equations.展开更多
Sweet and sour cherries contain several polyphenols that possess antioxidant and anti-inflammatory properties. Aim of this study was to investigate the effect of the maturity stage on phenol content and biological pro...Sweet and sour cherries contain several polyphenols that possess antioxidant and anti-inflammatory properties. Aim of this study was to investigate the effect of the maturity stage on phenol content and biological properties of extract of a local Morello-type of sour cherry (Prunus cerasus?L.), “visciola”. The study of total phenol content and total antioxidant potential was associated with the evaluation of the antioxidant property of extracts using a copper catalyzed human low density lipoproteins (LDL) oxidation as experimental model. Moreover, using albumin glycated by methylglyoxal, we evaluated the anti-glycation effect of fruit extract. The results demonstrated that fully ripened fruits exert higher antioxidant and anti-glycation properties when compared with partially ripened fruits. Information about the health-promoting components of “visciola” could lead to a better understanding and an increased consumption of these, including its use as functional food.展开更多
Due to an increasing environmental pollution, a search for the cost effective treatment and disposal of the dyes from the textile effluents is getting more and more importance. Oxidation and reduction processes play i...Due to an increasing environmental pollution, a search for the cost effective treatment and disposal of the dyes from the textile effluents is getting more and more importance. Oxidation and reduction processes play important roles in the degradation treatments of the azo dyes. The latter process is more effective and in consequence its mechanism is also better understood. The mechanism of the oxidation processes, the intermediates involved in these reactions and their role in the effectiveness of the oxidative degradation of the azo dyes, viz, phenyl azo b-naphthol (PAN), Sudan I. On exposure to sunlight at 2 1/2 hours for various samples in different concentrations of PAN mixed with Fenton reagent, when the reactive intermediate?reacted with the colour, the pH vs. absorbance generally showed significant degradation in between pH 5 and 6. The results were compared with the same samples on exposure to uv-light of 254 nm and irradiated at 20 minutes. The degradation occurred in samples of relatively high concentrations, viz, 10-3 and 5 × 10-4 mol· dm-3 at near neutral pH 6 whereas. Low concentration samples such as 10-4 and 5 × 10-5 mol·dm-3 showed degradation towards more acidic range of pH 2 to 4. In advanced oxidation process (AOP), generally reactive, strongly oxidizing ·OH radicals play a main role in destruction of the dye molecules. The proposed mechanisms and the rate coefficients for the reactions of ·OH intermediates with the dye molecules and with model compounds are summarized.展开更多
The radiation-induced degradation of 4-nitrophenol(4-NP) was performed in combination with a Fenton reagent, H_2O_2, and Ti O_2 nanoparticles to investigate the synergetic effects of radiolytical degradation combined ...The radiation-induced degradation of 4-nitrophenol(4-NP) was performed in combination with a Fenton reagent, H_2O_2, and Ti O_2 nanoparticles to investigate the synergetic effects of radiolytical degradation combined with other advanced oxidation processes. The experimental results indicated that the degradation efficiency of 4-NP was 87.5, 57.4, and 41.0 % at a dose of 20 k Gy when its initial concentration was 100, 200, and 350 mg/L, respectively. Radiation combined with H_2O_2, the Fenton method,and Ti O_2 remarkably increased the degradation efficiency of 4-NP, showing the synergetic effects. Radiation may enhance the biodegradability of 4-NP, suggesting that it has the potential to be used as a pretreatment method in combination with the biological method for the treatment of industrial wastewater containing toxic organic pollutants. Major intermediates during the 4-NP degradation process were identified and a possible degradation pathway was tentatively proposed.展开更多
A modified advanced oxidation process(AOP) utilizing a UV/electrochemically-generated peroxide system was used to fabricate titania films on chemically polished NiTi shape memory alloy(SMA). The microstructure and bio...A modified advanced oxidation process(AOP) utilizing a UV/electrochemically-generated peroxide system was used to fabricate titania films on chemically polished NiTi shape memory alloy(SMA). The microstructure and biomedical properties of the film were characterized by scanning electron microscopy(SEM), X-ray photoelectron spectroscopy(XPS), inductively-coupled plasma mass spectrometry(ICPMS), hemolysis analysis, and blood platelet adhesion test. It is found that the modified AOP has a high processing effectiveness and can result in the formation of a dense titania film with a Ni-free zone near its top surface. In comparison, Ni can still be detected on the outer NiTi surface by the conventional AOP using the UV/H2O2 system. The depth profiles of O, Ni, Ti show that the film possesses a smooth graded interface structure next to the NiTi substrate and this structure enhances the mechanical stability of titania film. The titania film can dramatically reduce toxic Ni ion release and also improve the hemolysis resistance and thromboresistance of biomedical NiTi SMA.展开更多
The degradation of the anti-inflammatory ibuprofen(IBP)was evaluated by several advanced oxidation processes.IBP was treated by single ozonation and oxidation with hydrogen peroxide(H_(2)O_(2)),as well as a combinatio...The degradation of the anti-inflammatory ibuprofen(IBP)was evaluated by several advanced oxidation processes.IBP was treated by single ozonation and oxidation with hydrogen peroxide(H_(2)O_(2)),as well as a combination of these treatments.In order to improve the efficiency,the presence of catalysts such as original carbon nanotubes,labelled as CNT,and iron oxide supported on carbon nanotubes,named as Fe/CNT sample,was considered.The evolution of IBP degradation,mineralization and toxicity of the solutions was assessed.The formation of intermediates was also monitored.In the non-catalytic processes,IBP was faster removed by single ozonation,whereas no significant total organic carbon(TOC)removal was achieved.Oxidation with H_(2)O_(2) did not present satisfactory results.When ozone and H_(2)O_(2) were combined,a higher mineralization was attained(70%after 180 min of reaction).On the other hand,in the catalytic processes,this combined process allowed the fastest IBP degradation.In terms of mineralization degree,the presence of Fe/CNT increases the removal rate in the first hour of reaction,achieving a TOC removal of 85%.Four compounds were detected as by-products.All treated solutions presented lower toxicity than the initial solution,suggesting that the released intermediates during applied processes are less toxic.展开更多
A model was developed to generate the complex degradation pathway of contaminants initiated by hydroxyl radical in the advanced oxidation processes. The model abstracts chemical structures into mathematic graphs. The ...A model was developed to generate the complex degradation pathway of contaminants initiated by hydroxyl radical in the advanced oxidation processes. The model abstracts chemical structures into mathematic graphs. The manipulation of the graphs enumerates the reactions among the large number of molecules, radicals, and other intermediates in the advanced oxidation processes. Using Canonical Simplified Molecular Input Line Entry Specification (Canonical SMILE) representation, the algorithm was able to simulate the reaction of contaminants containing both chain and ring structures. The input chemicals, reaction pattern, and the reaction rules could be specified by users through a graphical user interface. The degradation pathway of Atrazine was used as an example to demonstrate the capability of the algorithm. The generated reaction pathways were compared with those reported in literatures.展开更多
The experimental degradation of a water soluble dye, potassium indigo tetrasulfonate salt, has been studied using stand-alone ozonation and photocatalytic oxidation process. Progress of the dye oxidation was followed ...The experimental degradation of a water soluble dye, potassium indigo tetrasulfonate salt, has been studied using stand-alone ozonation and photocatalytic oxidation process. Progress of the dye oxidation was followed by UV-VIS spectrophotometric measurements at controlled operating conditions. The organic content of reaction samples was measured to verify the process efficiency in dye mineralization. According to current results, almost complete color removal was obtained for ozonation within about 1 h reaction time. The reduction of the organic load was almost 80% from its original while initial sulphur content decreased to 32.5%. Dye conversion of 100% was obtained by means of a photocatalytic process using TiO2 as catalyst at 294 nm irradiated UV light. This complete color removal for the catalytic process was observed within 7 min of reaction time. The calculated initial rate of reaction of photocatalysis treatment was 8 times faster than that of ozonolysis. However, the remaining organic load of photocatalysis was almost 88% from its original while the final sulphur content was 27.3%. This contrasting behavior of the performance of the type of oxidation process stressed importance of physicochemical phenomena and intermediates molecules present during dye degradation. An insightful and mechanistic aspect of the dye oxidation was developed by performing quantumchemical calculations.展开更多
We studied the decomposition of two haloacetic acids (HAAs),dichloroacetic acid (DCAA) and trichloroacetic acid (TCAA),in water by single oxidants ozone (O3) and ultraviolet radiation (UV) and the advanced oxidation p...We studied the decomposition of two haloacetic acids (HAAs),dichloroacetic acid (DCAA) and trichloroacetic acid (TCAA),in water by single oxidants ozone (O3) and ultraviolet radiation (UV) and the advanced oxidation processes (AOPs) constituted by the combinations of O3/UV,H2O2/UV,O3 /H2O2,and O3/H2O2/UV. The concentrations of HAAs were analyzed at specified time intervals to track their decomposition. Except for O3 and UV,the four combined oxidation processes remarkably enhance the decomposition of DCAA and TCAA owing to the generated very reactive hydroxyl radicals. The fastest decomposition process is O3/H2O2/UV,closely followed by O3/UV. DCAA is much easier to decompose than TCAA. The kinetics of HAA decomposition by O3/UV can be described well by a pseudo first-order reaction model under a constant initial dissolved O3 concentration and fixed UV radiation. Humic acids and HCO3-in the reaction system both decrease the decomposition rate constants for DCAA and TCAA. The amount of H2O2 accumulates in the presence of humic acids in the O3/UV process.展开更多
Advanced glycation end products(AGE) are potential harmful substances formed in the advanced Maillard reaction and increasingly investigated in muscle foods. However, the contribution of oxidation to the AGE formation...Advanced glycation end products(AGE) are potential harmful substances formed in the advanced Maillard reaction and increasingly investigated in muscle foods. However, the contribution of oxidation to the AGE formation is controversial. Moreover, reports on glyoxal(GO) induced AGE formation in chicken meat emulsion(CME) are limited. Thus, the effects of GO on emulsifying properties, rheological behavior and AGE formation in CME were investigated. Our findings exhibited that levels of Nε-carboxymethyllysine(CML) and Nε-carboxyethyllysine(CEL) were associated with lipid oxidation but not significantly(P > 0.05). Levels of AGE peaked when GO concentration ranged from 5 mmol/L(CML) to 10 mmol/L(CEL). The droplets’ aggregation associated with the disulfide bond when the concentration of GO was at 0.5–30 mmol/L while non-disulfide bond association occurred at 30–50 mmol/L GO concentration. In conclusion, compared to the effect of oxidation, GO exhibited the main role in the AGE formation of CME. This study will provide theoretical significance for further understanding and controlling the formation of AGE in CME.展开更多
Treatment to crystallization mother liquor containing high concentration of organic and inorganic substances is a challenge in zero liquid discharge of industrial wastewater.Acid precipitation coupled membrane-dispers...Treatment to crystallization mother liquor containing high concentration of organic and inorganic substances is a challenge in zero liquid discharge of industrial wastewater.Acid precipitation coupled membrane-dispersion advanced oxidation process(MAOP)was proposed for organics degradation before salt crystallization by evaporation.With acid-MAOP treatment CODCrin mother liquor of pulping wastewater was eliminated by 55.2%from ultrahigh initial concentration up to 12,500 mg·L^-1.The decolorization rate was 96.5%.Recovered salt was mainly NaCl(83.3 wt%)having whiteness 50 brighter than industrial baysalt of whiteness 45.The oxidation conditions were optimized as CO3=0.11 g·L^-1 and CH2O2=2.0 g·L^-1 with dispersing rate 0.53 ml·min^-1 for 100 min reaction toward acidified liquor of p H=2.Acidification has notably improved evaporation efficiency during crystallization.Addition of H2O2 made through membrane dispersion has eliminated hydroxyl radical"quench effect"and enhanced the degradation capacity,in particular,the breakage of carbon-chloride bonds(of both aliphatic and aromatic).As a result,the proposed coupling method has improved organic pollutant reduction so as the purity of salt from the wastewater mixture which can facilitate water and salt recycling in industry.展开更多
Studies to decompose persistent organic pollutants in wastewater from chemical factories by using Advanced Oxidation Processes (AOPs) have recently been performed. Oxidation reactions involving ozone and •OH ...Studies to decompose persistent organic pollutants in wastewater from chemical factories by using Advanced Oxidation Processes (AOPs) have recently been performed. Oxidation reactions involving ozone and •OH radicals and cleavage caused by UV are the main decomposition reactions that occur in AOPs using ozone and UV. The mechanisms through which organic compounds are decomposed in AOPs are complicated and difficult to understand because various decomposition reactions occur simultaneously. The Total Organic Carbon (TOC) removal efficiencies achieved in several different AOPs were evaluated in this study. The TOC removal efficiencies were different for organic compounds with different chemical structures. The TOC was more effectively removed when aromatic compounds were treated using the O<sub>3</sub>-UV-TiO<sub>2</sub> process than when using the other AOPs, and the TOC was removed more effectively by the O<sub>3</sub>-UV process than by the UV-TiO<sub>2</sub> process. However, the TOC was removed more effectively when open-chain compounds were treated using the UV-TiO<sub>2</sub> process than using the O<sub>3</sub>-UV process, and the UV-TiO<sub>2</sub> and O<sub>3</sub>-UV-TiO<sub>2</sub> processes resulted in similar TOC removal efficiencies. Therefore, it is necessary to use the O<sub>3</sub>-UV-TiO<sub>2</sub> process to decompose aromatic compounds as quickly as possible. On the other hand, the UV-TiO<sub>2</sub> process degraded the open-chain compounds most effectively, and the O<sub>3</sub>-UV-TiO<sub>2</sub> process did not need to decompose open-chain compounds. Moreover, the TOC of aromatic compounds was removed more slowly than that of open-chain compounds. The TOC removal efficiency increased with decreasing the number of carbon atoms in the molecule. The TOC removal efficiencies increased in order of the organic compounds containing methyl groups, aldehyde groups and carboxyl groups. The removal of the TOC when organic compounds were treated using the O<sub>3</sub>-UV-TiO<sub>2</sub> process followed pseudo-zero-order kinetics.展开更多
基金supported by National Natural Science Foundation of China(52003240)Zhejiang Provincial Natural Science Foundation of China(LQ21B070007)China Postdoctoral Science Foundation(2022M722818).
文摘Realizing fast and continuous generation of reactive oxygen species(ROSs)via iron-based advanced oxidation processes(AOPs)is significant in the environmental and biological fields.However,current AOPs assisted by co-catalysts still suffer from the poor mass/electron transfer and non-durable promotion effect,giving rise to the sluggish Fe^(2+)/Fe^(3+)cycle and low dynamic concentration of Fe^(2+)for ROS production.Herein,we present a three-dimensional(3D)macroscale co-catalyst functionalized with molybdenum disulfide(MoS_(2))to achieve ultra-efficient Fe^(2+)regeneration(equilibrium Fe^(2+)ratio of 82.4%)and remarkable stability(more than 20 cycles)via a circulating flow-through process.Unlike the conventional batch-type reactor,experiments and computational fluid dynamics simulations demonstrate that the optimal utilization of the 3D active area under the flow-through mode,initiated by the convectionenhanced mass/charge transfer for Fe^(2+)reduction and then strengthened by MoS_(2)-induced flow rotation for sufficient reactant mixing,is crucial for oxidant activation and subsequent ROS generation.Strikingly,the flow-through co-catalytic system with superwetting capabilities can even tackle the intricate oily wastewater stabilized by different surfactants without the loss of pollutant degradation efficiency.Our findings highlight an innovative co-catalyst system design to expand the applicability of AOPs based technology,especially in large-scale complex wastewater treatment.
基金supported by grants from the Research Grants Council of the Hong Kong SAR,China(T21-705/20-N and 16210221).
文摘Antibiotic resistant bacteria(ARB)with antibiotic resistance genes(ARGs)can reduce or eliminate the effectiveness of antibiotics and thus threaten human health.The United Nations Environment Programme considers antibiotic resistance the first of six emerging issues of concern.Advanced oxidation processes(AOPs)that combine ultraviolet(UV)irradiation and chemical oxidation(primarily chlorine,hydrogen peroxide,and persulfate)have attracted increasing interest as advanced water and wastewater treatment technologies.These integrated technologies have been reported to significantly elevate the efficiencies of ARB inactivation and ARG degradation compared with direct UV irradiation or chemical oxidation alone due to the generation of multiple reactive species.In this study,the performance and underlying mechanisms of UV/chlorine,UV/hydrogen peroxide,and UV/persulfate processes for controlling ARB and ARGs were reviewed based on recent studies.Factors affecting the process-specific efficiency in controlling ARB and ARGs were discussed,including biotic factors,oxidant dose,UV fluence,pH,and water matrix properties.In addition,the cost-effectiveness of the UV-based AOPs was evaluated using the concept of electrical energy per order.The UV/chlorine process exhibited a higher efficiency with lower energy consumption than other UV-based AOPs in the wastewater matrix,indicating its potential for ARB inactivation and ARG degradation in wastewater treatment.Further studies are required to address the trade-off between toxic byproduct formation and the energy efficiency of the UV/chlorine process in real wastewater to facilitate its optimization and application in the control of ARB and ARGs.
基金supported by National Key R&D Program of China(2021YFD2100104)griculture Research System of China(CARS-41-Z)+2 种基金Science and Technology Project of Nanjing City(202002040)Jiangsu Province Policy Guidance Program(BX2020008)Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX21_0579),China。
文摘Investigation that protein oxidation to the formation of advanced glycation end products(AGEs)after chicken myofibrillar protein glycation is limited.Models of protein oxidation induced by different concentrations of hydroxyl radicals(·OH)were developed after the chicken myofibrillar protein mild glycation(MPG).Results exhibited that levels of AGEs and surface hydrophobicity(H_(0))steadily increased with the a ddition of h ydrogen peroxide(H_(2)O_(2))concentration.However,levels of s ulfhydryl group,free amino group,and particle size gradually decreased with the H_(2)O_(2)concentration.The protein carbonyl value increased in H_(2)O_(2)concentration until 10 mmol/L.Pearson's correlation indicated that MPG structure modification(unfolding and degradation)induced by protein oxidation were significantly positively correlated with AGEs concentration(P<0.05).Finally,a mechanism was proposed to hypothesize t he effect of protein oxidation on the formation of AGEs under MPG conditions.
文摘This article, for the first time, provides a novel advanced oxidation process based on sulfate radical (SO^4·-) to degrade organic pollutants in wastewater: microwave (MW)-activated persulfate oxidation (APO) with or without active carbon (AC). Azo dye acid Orange 7 (AO7) is used as a model compound to investigate the high reactivity of MW-APO. It is found that AO7 (up to 1000 mg/L) is completely decolorized within 5-7 min under an 800 W MW furnace assisted-APO. In the presence of chloride ion (up to 0.50 mol/L), the decolorization is still 100% completed, though delayed for about 1-2 min. Experiments are made to examine the enhancement by AC. It is exciting to find that the 100% decolorization of AO7 (500 mg/L) is achieved within 3 min by MW-APO using 1.0 g/L AC as catalyst, while the degradation efficiency maintains at 50% by MW energy without persulfate after about 5 min. Besides the destruction of visible light chromophore band of AO7 (484 nm), during MW-APO, two bands in the ultraviolet region (228 nm and 310 nm) are rapidly broken down. The removal of COD is about 83%-95% for 500 mg/L AO7. SO^4·- is identified with quenching studies using specific alcohols. Both SO^4·- and ·OH could degrade AO7, but SO^4·- plays the dominant role. In a word, MW-APO AC is a new catalytic combustion technology for destruction of organic contamination even for high concentration.
基金Supported by the Key Technologies R&D Program of China(2011BAE111300)
文摘The degradation capacity of advanced oxidants generated from oxygen reduction was investigated in model effluent containing chlorobenzene, aniline and benzene through the advanced oxidation processes(AOPs). Intermediate products of the degradation process were determined by GC–MS, and they contributed to specify the degradation pathways of monoaromatic compounds. The study particularly focused on the influence of the dosage of the oxidant, pH and the initial concentration of organic compounds on the degradation effectiveness.When the dosage of oxidant was 4 wt% and the pH was 7, the maximum degradation rates of 74.83% chlorobenzene, 70.32% aniline and 37.69% benzene were achieved. Furthermore, microwave was applied to intensify the oxidation process under optimal operation conditions, and the degradation rates were increased to 87.85% chlorobenzene, 89.11% aniline and 39.03% benzene, respectively.
文摘In this study,advanced oxidation processes(AOPs) such as anodic oxidation(AO),UV/H_2O_2 and Fenton processes(FP) were investigated for the degradation of salicylic acid(SA) in lab-scale experiments.Boron-doped diamond(BDD) film electrodes using Ta as substrates were employed for AO of SA.In the case of FP and UV/H_2O_2,most favorable experimental conditions were determined for each process and these were used for comparing with AO process.The study showed that the FP was the most effective process under aci...
文摘The removal of the natural organic matter present in coffee processing wastewater through chemical coagulation-flocculation and advanced oxidation processes (AOP) had been studied. The effectiveness of the removal of natural organic matter using commercial flocculants and UV/H202, UV/O3 and UV/H2O2/O3 processes was determined under acidic conditions. For each of these processes, different operational conditions were explored to optimize the treatment efficiency of the coffee wastewater. Coffee wastewater is characterized by a high chemical oxygen demand (COD) and low total suspended solids. The outcomes of coffee wastewater treatment using coagulation-flocculation and photodegradation processes were assessed in terms of reduction of COD, color, and turbidity. It was found that a reduction in COD of 67% could be realized when the coffee wastewater was treated by chemical coagulation-flocculation with lime and coagulant T-1. When coffee wastewater was treated by coagulation-flocculation in combination with UV/H2O2, a COD reduction of 86% was achieved, although only after prolonged UV irradiation. Of the three advanced oxidation processes considered, UV/H2O2, UV/O3 and UV/H2O2/O3, we found that the treatment with UV/H2O2/O3 was the most effective, with an efficiency of color, turbidity and further COD removal of 87%, when applied to the flocculated coffee wastewater.
文摘2,4-Dinitroanisole(DNAN)is an important component of insensitive munitions that is anticipated to replace 2,4,6-trinitrotoluene(TNT)in munitions formulations.Photocatalyzed hydrogen peroxide(H2O2)oxidation experiments and chemical analyses were conducted to study the effect of initial pH and H2O2 dosage on the kinetics of DNAN decomposition and the reaction pathways.The results show that DNAN degradation followed zero-order kinetics when a 250 ppm DNAN solution was treated with ultraviolet(UV)light and 1500–4500 ppm H2O2 in an initial pH range of 4–7.However,when the H2O2 concentration was 750 ppm,DNAN degradation followed pseudo-first-order kinetics.The results indicate that DNAN can easily be oxidized by UV/H2O2 treatment.When the H2O2 dosage was 1500 ppm and the initial pH was 7,DNAN was reduced from 250 ppm to less than 1 ppm in 3 h.However,the total organic carbon(TOC)and total carbon(TC)concentrations were reduced slowly from 100 to less than 70 ppm carbon(C)in 3 h,and decreased to about 5 ppm after 9 h of treatment,suggesting the formation of other organic compounds.Those reaction intermediates were oxidized to carbon dioxide(CO2)at a slower rate than the oxidation of DNAN.CO2 was emitted from the solution because the solution pH decreased rapidly to about 3 during the UV/H2O2 oxidation.Most of the nitrogen in DNAN was converted to nitrate by UV/H2O2 oxidation after 9 h of treatment.The research results indicate that UV/H2O2 oxidation is a promising technique for the treatment of DNAN in wastewater.
基金Supported by Guangdong Province Natural Scientific Foundation(No.970457).
文摘A kinetic model has been developed for the degradation of organic pollutants concerning with hydroperoxide ion as the initial step for generation of hydroxyl radical and its subsequent reaction mechanisms. Rate equations were derived for depletion of ozone and pollutants in the peroxone oxidation process using ozone and hydrogen peroxide as combined oxidants. Kinetic data obtained experimentally from the hydrogen peroxide-ozone reaction and peroxone oxidation of nitrobenzene were analyzed by using the proposed rate equations.
文摘Sweet and sour cherries contain several polyphenols that possess antioxidant and anti-inflammatory properties. Aim of this study was to investigate the effect of the maturity stage on phenol content and biological properties of extract of a local Morello-type of sour cherry (Prunus cerasus?L.), “visciola”. The study of total phenol content and total antioxidant potential was associated with the evaluation of the antioxidant property of extracts using a copper catalyzed human low density lipoproteins (LDL) oxidation as experimental model. Moreover, using albumin glycated by methylglyoxal, we evaluated the anti-glycation effect of fruit extract. The results demonstrated that fully ripened fruits exert higher antioxidant and anti-glycation properties when compared with partially ripened fruits. Information about the health-promoting components of “visciola” could lead to a better understanding and an increased consumption of these, including its use as functional food.
文摘Due to an increasing environmental pollution, a search for the cost effective treatment and disposal of the dyes from the textile effluents is getting more and more importance. Oxidation and reduction processes play important roles in the degradation treatments of the azo dyes. The latter process is more effective and in consequence its mechanism is also better understood. The mechanism of the oxidation processes, the intermediates involved in these reactions and their role in the effectiveness of the oxidative degradation of the azo dyes, viz, phenyl azo b-naphthol (PAN), Sudan I. On exposure to sunlight at 2 1/2 hours for various samples in different concentrations of PAN mixed with Fenton reagent, when the reactive intermediate?reacted with the colour, the pH vs. absorbance generally showed significant degradation in between pH 5 and 6. The results were compared with the same samples on exposure to uv-light of 254 nm and irradiated at 20 minutes. The degradation occurred in samples of relatively high concentrations, viz, 10-3 and 5 × 10-4 mol· dm-3 at near neutral pH 6 whereas. Low concentration samples such as 10-4 and 5 × 10-5 mol·dm-3 showed degradation towards more acidic range of pH 2 to 4. In advanced oxidation process (AOP), generally reactive, strongly oxidizing ·OH radicals play a main role in destruction of the dye molecules. The proposed mechanisms and the rate coefficients for the reactions of ·OH intermediates with the dye molecules and with model compounds are summarized.
基金supported by the Program for Changjiang Scholars and Innovative Research Team in University (No. IRT-13026)the National High Technology Research and Development Program (No. 2009AA063905)+1 种基金the International S&T Cooperation Program (ISTCP) of China (No. 2009DFB90600)the National Natural Science Foundation of China (No. 51338005)
文摘The radiation-induced degradation of 4-nitrophenol(4-NP) was performed in combination with a Fenton reagent, H_2O_2, and Ti O_2 nanoparticles to investigate the synergetic effects of radiolytical degradation combined with other advanced oxidation processes. The experimental results indicated that the degradation efficiency of 4-NP was 87.5, 57.4, and 41.0 % at a dose of 20 k Gy when its initial concentration was 100, 200, and 350 mg/L, respectively. Radiation combined with H_2O_2, the Fenton method,and Ti O_2 remarkably increased the degradation efficiency of 4-NP, showing the synergetic effects. Radiation may enhance the biodegradability of 4-NP, suggesting that it has the potential to be used as a pretreatment method in combination with the biological method for the treatment of industrial wastewater containing toxic organic pollutants. Major intermediates during the 4-NP degradation process were identified and a possible degradation pathway was tentatively proposed.
基金Project(NCET-06-0464) supported by the Program for New Century Excellent Talents in University of Ministry of Education of ChinaProject(BK2007515) supported by the Natural Science Foundation of Jiangsu Province, China+2 种基金Project(2006AA03Z445) supported by the National High-tech Research and Development Program of ChinaProject supported by Nippon Sheet Glass Foundation for Materials Science and Engineering (NSG Foundation)Project(7001999) supported by SRG Grant from the Research Committee of the CityU of HK
文摘A modified advanced oxidation process(AOP) utilizing a UV/electrochemically-generated peroxide system was used to fabricate titania films on chemically polished NiTi shape memory alloy(SMA). The microstructure and biomedical properties of the film were characterized by scanning electron microscopy(SEM), X-ray photoelectron spectroscopy(XPS), inductively-coupled plasma mass spectrometry(ICPMS), hemolysis analysis, and blood platelet adhesion test. It is found that the modified AOP has a high processing effectiveness and can result in the formation of a dense titania film with a Ni-free zone near its top surface. In comparison, Ni can still be detected on the outer NiTi surface by the conventional AOP using the UV/H2O2 system. The depth profiles of O, Ni, Ti show that the film possesses a smooth graded interface structure next to the NiTi substrate and this structure enhances the mechanical stability of titania film. The titania film can dramatically reduce toxic Ni ion release and also improve the hemolysis resistance and thromboresistance of biomedical NiTi SMA.
基金financially supported by Base Funding–UIDB/50020/2020 of the Associate Laboratory LSRE-LCM–funded by national funds through FCT/MCTES(PIDDAC)Project PTDC/EAM-AMB/31337/2017–POCI-01-0145-FEDER-031337–funded by FEDER funds through COMPETE2020–Programa Operacional Competitividade e Internacionalização(POCI)+4 种基金with financial support of FCT/MCTES through national funds(PIDDAC)by NORTE-01-0247-FEDER-069836co-funded by the European Regional Development Fund(ERDF),through the North Portugal Regional Operational Programme(NORTE2020),under the PORTUGAL 2020 Partnership AgreementFCT funding under DL57/2016 Transitory Norm ProgrammeFCT funding under the Scientific Employment Stimulus–Institutional Call CEECINST/00049/2018
文摘The degradation of the anti-inflammatory ibuprofen(IBP)was evaluated by several advanced oxidation processes.IBP was treated by single ozonation and oxidation with hydrogen peroxide(H_(2)O_(2)),as well as a combination of these treatments.In order to improve the efficiency,the presence of catalysts such as original carbon nanotubes,labelled as CNT,and iron oxide supported on carbon nanotubes,named as Fe/CNT sample,was considered.The evolution of IBP degradation,mineralization and toxicity of the solutions was assessed.The formation of intermediates was also monitored.In the non-catalytic processes,IBP was faster removed by single ozonation,whereas no significant total organic carbon(TOC)removal was achieved.Oxidation with H_(2)O_(2) did not present satisfactory results.When ozone and H_(2)O_(2) were combined,a higher mineralization was attained(70%after 180 min of reaction).On the other hand,in the catalytic processes,this combined process allowed the fastest IBP degradation.In terms of mineralization degree,the presence of Fe/CNT increases the removal rate in the first hour of reaction,achieving a TOC removal of 85%.Four compounds were detected as by-products.All treated solutions presented lower toxicity than the initial solution,suggesting that the released intermediates during applied processes are less toxic.
文摘A model was developed to generate the complex degradation pathway of contaminants initiated by hydroxyl radical in the advanced oxidation processes. The model abstracts chemical structures into mathematic graphs. The manipulation of the graphs enumerates the reactions among the large number of molecules, radicals, and other intermediates in the advanced oxidation processes. Using Canonical Simplified Molecular Input Line Entry Specification (Canonical SMILE) representation, the algorithm was able to simulate the reaction of contaminants containing both chain and ring structures. The input chemicals, reaction pattern, and the reaction rules could be specified by users through a graphical user interface. The degradation pathway of Atrazine was used as an example to demonstrate the capability of the algorithm. The generated reaction pathways were compared with those reported in literatures.
文摘The experimental degradation of a water soluble dye, potassium indigo tetrasulfonate salt, has been studied using stand-alone ozonation and photocatalytic oxidation process. Progress of the dye oxidation was followed by UV-VIS spectrophotometric measurements at controlled operating conditions. The organic content of reaction samples was measured to verify the process efficiency in dye mineralization. According to current results, almost complete color removal was obtained for ozonation within about 1 h reaction time. The reduction of the organic load was almost 80% from its original while initial sulphur content decreased to 32.5%. Dye conversion of 100% was obtained by means of a photocatalytic process using TiO2 as catalyst at 294 nm irradiated UV light. This complete color removal for the catalytic process was observed within 7 min of reaction time. The calculated initial rate of reaction of photocatalysis treatment was 8 times faster than that of ozonolysis. However, the remaining organic load of photocatalysis was almost 88% from its original while the final sulphur content was 27.3%. This contrasting behavior of the performance of the type of oxidation process stressed importance of physicochemical phenomena and intermediates molecules present during dye degradation. An insightful and mechanistic aspect of the dye oxidation was developed by performing quantumchemical calculations.
基金Natural Science Foundation of Chongqing under Grant No. CSTC2008BB7299.
文摘We studied the decomposition of two haloacetic acids (HAAs),dichloroacetic acid (DCAA) and trichloroacetic acid (TCAA),in water by single oxidants ozone (O3) and ultraviolet radiation (UV) and the advanced oxidation processes (AOPs) constituted by the combinations of O3/UV,H2O2/UV,O3 /H2O2,and O3/H2O2/UV. The concentrations of HAAs were analyzed at specified time intervals to track their decomposition. Except for O3 and UV,the four combined oxidation processes remarkably enhance the decomposition of DCAA and TCAA owing to the generated very reactive hydroxyl radicals. The fastest decomposition process is O3/H2O2/UV,closely followed by O3/UV. DCAA is much easier to decompose than TCAA. The kinetics of HAA decomposition by O3/UV can be described well by a pseudo first-order reaction model under a constant initial dissolved O3 concentration and fixed UV radiation. Humic acids and HCO3-in the reaction system both decrease the decomposition rate constants for DCAA and TCAA. The amount of H2O2 accumulates in the presence of humic acids in the O3/UV process.
基金supported by Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX21_0579)the China Scholarship Council(No.202006850022)+1 种基金supported by Agriculture Research System of China(CARS-41-Z)Science and Technology Project of Nanjing City(No.202002040)。
文摘Advanced glycation end products(AGE) are potential harmful substances formed in the advanced Maillard reaction and increasingly investigated in muscle foods. However, the contribution of oxidation to the AGE formation is controversial. Moreover, reports on glyoxal(GO) induced AGE formation in chicken meat emulsion(CME) are limited. Thus, the effects of GO on emulsifying properties, rheological behavior and AGE formation in CME were investigated. Our findings exhibited that levels of Nε-carboxymethyllysine(CML) and Nε-carboxyethyllysine(CEL) were associated with lipid oxidation but not significantly(P > 0.05). Levels of AGE peaked when GO concentration ranged from 5 mmol/L(CML) to 10 mmol/L(CEL). The droplets’ aggregation associated with the disulfide bond when the concentration of GO was at 0.5–30 mmol/L while non-disulfide bond association occurred at 30–50 mmol/L GO concentration. In conclusion, compared to the effect of oxidation, GO exhibited the main role in the AGE formation of CME. This study will provide theoretical significance for further understanding and controlling the formation of AGE in CME.
基金Financial supports from the Prospective Joint Research Project of Jiangsu Province(BY2014005-06)National Natural Science Foundation of China(U1510202)the Jiangsu National Synergistic Innovation Center for Advanced Materials(SICAM)。
文摘Treatment to crystallization mother liquor containing high concentration of organic and inorganic substances is a challenge in zero liquid discharge of industrial wastewater.Acid precipitation coupled membrane-dispersion advanced oxidation process(MAOP)was proposed for organics degradation before salt crystallization by evaporation.With acid-MAOP treatment CODCrin mother liquor of pulping wastewater was eliminated by 55.2%from ultrahigh initial concentration up to 12,500 mg·L^-1.The decolorization rate was 96.5%.Recovered salt was mainly NaCl(83.3 wt%)having whiteness 50 brighter than industrial baysalt of whiteness 45.The oxidation conditions were optimized as CO3=0.11 g·L^-1 and CH2O2=2.0 g·L^-1 with dispersing rate 0.53 ml·min^-1 for 100 min reaction toward acidified liquor of p H=2.Acidification has notably improved evaporation efficiency during crystallization.Addition of H2O2 made through membrane dispersion has eliminated hydroxyl radical"quench effect"and enhanced the degradation capacity,in particular,the breakage of carbon-chloride bonds(of both aliphatic and aromatic).As a result,the proposed coupling method has improved organic pollutant reduction so as the purity of salt from the wastewater mixture which can facilitate water and salt recycling in industry.
文摘Studies to decompose persistent organic pollutants in wastewater from chemical factories by using Advanced Oxidation Processes (AOPs) have recently been performed. Oxidation reactions involving ozone and •OH radicals and cleavage caused by UV are the main decomposition reactions that occur in AOPs using ozone and UV. The mechanisms through which organic compounds are decomposed in AOPs are complicated and difficult to understand because various decomposition reactions occur simultaneously. The Total Organic Carbon (TOC) removal efficiencies achieved in several different AOPs were evaluated in this study. The TOC removal efficiencies were different for organic compounds with different chemical structures. The TOC was more effectively removed when aromatic compounds were treated using the O<sub>3</sub>-UV-TiO<sub>2</sub> process than when using the other AOPs, and the TOC was removed more effectively by the O<sub>3</sub>-UV process than by the UV-TiO<sub>2</sub> process. However, the TOC was removed more effectively when open-chain compounds were treated using the UV-TiO<sub>2</sub> process than using the O<sub>3</sub>-UV process, and the UV-TiO<sub>2</sub> and O<sub>3</sub>-UV-TiO<sub>2</sub> processes resulted in similar TOC removal efficiencies. Therefore, it is necessary to use the O<sub>3</sub>-UV-TiO<sub>2</sub> process to decompose aromatic compounds as quickly as possible. On the other hand, the UV-TiO<sub>2</sub> process degraded the open-chain compounds most effectively, and the O<sub>3</sub>-UV-TiO<sub>2</sub> process did not need to decompose open-chain compounds. Moreover, the TOC of aromatic compounds was removed more slowly than that of open-chain compounds. The TOC removal efficiency increased with decreasing the number of carbon atoms in the molecule. The TOC removal efficiencies increased in order of the organic compounds containing methyl groups, aldehyde groups and carboxyl groups. The removal of the TOC when organic compounds were treated using the O<sub>3</sub>-UV-TiO<sub>2</sub> process followed pseudo-zero-order kinetics.