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
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
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
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
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
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
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
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
This paper,reports the performance of a wastewater treatment scale-pilot plant to treat 2 GPM(Gallons per Minute)discharges with 5,205 mg/L of pollutants expressed in COD(Chemical Oxygen Demand),from“Lomas de la Maes...This paper,reports the performance of a wastewater treatment scale-pilot plant to treat 2 GPM(Gallons per Minute)discharges with 5,205 mg/L of pollutants expressed in COD(Chemical Oxygen Demand),from“Lomas de la Maestransa”a small community in Morelia City,Michoacan,Mexico.The scale-pilot plant is a train with(1)pretreatment with a triturated pump for floating solid,(2)primary treatment with“in line”coagulation,and rapid filtration to retain suspended colloids and dissolved solids higher of 5μm diameter,(3)double advanced oxidation as secondary treatment with ozone and heterogeneous photo catalysis to oxidize volatile solids,and(4)tertiary treatment with activated carbon to retain refractory compounds.Plant performance was analyzed by a certified laboratory that belongs to Potable Water,Sewage and Sanitation Department from Morelia City Government.Results show that treated water effluent complied with the Mexican Official Standard NOM-001-SEMARNAT-1996 for discharges into national waters,with exception of fecal coliforms,since the raw water contains an average of 64,228,351 MNP/100 mL of fecal coliforms,and in spite that we obtained a 99.998%efficiency,the maximum level allowable 2,000 MPN/100 mL standard,was exceeded by 400 MPN/100 mL.After this experience,the wastewater treatment plant is equipped with a residual chlorine tank to keep a 1.5 ppm chlorine residual concentration to keep the treated water clean.This project was possible because we had the support of the Morelia Sanitation Department.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
Hospital sewage contains various harmful pharmaceutical contaminants(e.g.,antibiotics,anti-inflammatory agents,and painkillers)and pathogens(e.g.,bacteria,viruses,and parasites),whose direct discharge into the environ...Hospital sewage contains various harmful pharmaceutical contaminants(e.g.,antibiotics,anti-inflammatory agents,and painkillers)and pathogens(e.g.,bacteria,viruses,and parasites),whose direct discharge into the environment will induce diseases and pose a powerful threat to human health and safety,and environmental ecology.In recent years,advanced oxidation processes(AOPs),particularly photocatalysis,electrocatalysis,and ozone catalysis have been developed as widespread and effective techniques for hospital sewage treatments.However,there is a lack of systematic comparison and review of the prior studies on hospital sewage treatment using AOPs systems.This review elaborates on the mechanisms,removal efficiencies,and advantages/disadvantages of these AOPs systems for hospital wastewater decontamination and disinfection.Meanwhile,some novel and potential technologies such as photo-electrocatalysis,electro-peroxone,Fenton/Fenton-like,and piezoelectric catalysis are also included and summarized.Moreover,we further summarize and compare the capacity of these AOPs to treat the actual hospital wastewater under the impact of the water matrix and pH,and estimate the economic cost of these technologies for practical application.Finally,the future development directions of AOPs for hospital wastewater decontamination and disinfection have been prospected.Overall,this study provides a comparison and overview of these AOP systems in an attempt to raise extensive concerns about hospital wastewater decontamination and disinfection technologies and guide researchers to discover the future directions of technologies optimization,which would be a crucial step forward in the field of hospital sewage treatment.展开更多
Maximizing the sustainable recycling of spent lithium-ion batteries(LIBs)shows economic and environmental significance.This study recovered lithium cobaltate(LiCoO_(2),LCO)from spent LIBs cathode powder.The recovered ...Maximizing the sustainable recycling of spent lithium-ion batteries(LIBs)shows economic and environmental significance.This study recovered lithium cobaltate(LiCoO_(2),LCO)from spent LIBs cathode powder.The recovered LCO was then combined with NaHSO_(3)to remove refractory organic pollutants of carbamazepine(CBZ)in water.The degradation of CBZ reached 80.0%within 60 min,by 1O_(2),SO_(4),OH and O_(2)^(-)generated in the LCO/NaHSO_(3)reaction.The electron transfer between Co(III)and Co(II)was beneficial to the generation of free radicals.The LCO/NaHSO_(3)degraded CBZ effectively in both secondary outlet water and tap water.However,high concentrations of inorganic ions(Cl^(−),HCO_(3)^(-),HPO_(4)^(2-),SO_(2)−4,NO_(3)^(-))and natural organic matter(humic acid,HA)could inhibit the degradation of CBZ.After three cycles,the stability of the LCO/NaHSO_(3)system was demonstrated by the maintained high efficiency in the degradation of CBZ.The obtained data indicate that the LCO/NaHSO_(3)system holds great application potential in the field of advanced oxidation degradation of pollutants.展开更多
Manganese oxides(MNO_(x)),as low-toxicity and high-abundance catalysts,have been demonstrated to hold great promise for application in advanced oxidation processes(AOPs).However,further application of this material is...Manganese oxides(MNO_(x)),as low-toxicity and high-abundance catalysts,have been demonstrated to hold great promise for application in advanced oxidation processes(AOPs).However,further application of this material is restricted due to its unsatisfactory oxidant activation efficiency.Fortunately,recently remarkable research on deep activation mechanisms and modification of MNO_(x)have been undertaken to improve its reactivity.Herein,modification enhancement mechanisms of MNO_(x)to efficiently degrade various organic contaminants were discussed and highlighted,including metal doping,coupling with other metal oxides,composite with carbonaceous material,and compounding with other support.The activation mechanisms of different MNO_(x)and derivative-modified material(such as doped MNO_(x),metal oxide-MNO_(x)hybrids,and MNO_(x)-carbonaceous material hybrids)were summarized in great details,which was specifically categorized into both radical and non-radical pathways.The effects of pH,inorganic ions,and natural organic matter on degradation reactions are also discussed.Finally,future research directions and perspectives are presented to provide a clear interpretation on the MNO_(x)initiated AOPs.展开更多
In some industrial wastewater,heavy metals combine with organic complexing agents to form heavy metal complexes(HMCs).These HMCs can be difficult to decompose and remove through conventional techniques due to their hi...In some industrial wastewater,heavy metals combine with organic complexing agents to form heavy metal complexes(HMCs).These HMCs can be difficult to decompose and remove through conventional techniques due to their higher stability than free heavy metal ions.In recent years,persulfate based advanced oxidation processes(PS-based AOPs)have been recognized as a viable technique for HMCs degradation.Nevertheless,a comprehensive and in-depth understanding of the relevant HMCs decomplexation mechanisms in PS-based AOPs is still lacking.This review delineates the current progress of HMCs decomplexation in PS-based AOPs.We discuss the distinctions between the two widely used oxidant types in PS-based AOPs techniques.Moreover,we summarize and highlight the decomplexation mechanisms based on electron and energy transfer,and degradation pathways of HMCs.We also emphasize the effects of environmental water constituents,namely p H,inorganic ions,and natural organic matter(NOM),on HMCs decomplexation.Ultimately,we identify the existing challenges and perspectives that will steer the direction of advancing PS-based AOPs to remove HMCs.展开更多
As important emerging contaminants, antibiotics have caused potential hazards to the ecological environment and human health due to their extensive production and consumption. Among various techniques for removing ant...As important emerging contaminants, antibiotics have caused potential hazards to the ecological environment and human health due to their extensive production and consumption. Among various techniques for removing antibiotics from wastewater, H_(2)O_(2)-based advanced oxidation processes(AOPs) have received increasing attention due to their fast reaction rate and strong oxidation capability. Hence this review critically discusses:(i) Recent research progress of AOPs with the addition of H_(2)O_(2) for antibiotics removal through different methods of H_(2)O_(2) activation;(ii) recent advances in AOPs that can in-situ generate and activate H_(2)O_(2) for antibiotics removal;(iii) H_(2)O_(2)-based AOPs as a combination with other techniques for the degradation and mineralization of antibiotics in wastewater. Future perspectives about H_(2)O_(2)-based AOPs are also presented to grasp the future research trend in the area.展开更多
The degradation of metoprolol(MTP)by the UV/sulfite with oxygen as an advanced reduction process(ARP)and that without oxygen as an advanced oxidation process(AOP)was comparatively studied herein.The degradation of MTP...The degradation of metoprolol(MTP)by the UV/sulfite with oxygen as an advanced reduction process(ARP)and that without oxygen as an advanced oxidation process(AOP)was comparatively studied herein.The degradation of MTP by both processes followed the first-order rate law with comparable reaction rate constants of 1.50×10^(-3)sec^(−1)and 1.20×10^(-3)sec^(−1),respectively.Scavenging experiments demonstrated that both e^(−)_(aq)and H·played a crucial role in MTP degradation by the UV/sulfite as an ARP,while SO_(4)^(·−)was the dominant oxidant in the UV/sulfite AOP.The degradation kinetics of MTP by the UV/sulfite as an ARP and AOP shared a similar pH dependence with a minimum rate obtained around pH 8.The results could be well explained by the pH impacts on the MTP speciation and sulfite species.Totally six transformation products(TPs)were identified from MTP degradation by the UV/sulfite ARP,and two additional ones were detected in the UV/sulfite AOP.The benzene ring and ether groups of MTP were proposed as the major reactive sites for both processes based on molecular orbital calculations by density functional theory(DFT).The similar degradation products of MTP by the UV/sulfite process as an ARP and AOP indicated that e^(−)_(aq)/H·and SO_(4)^(·−)might share similar reaction mechanisms,primarily including hydroxylation,dealkylation,and H abstraction.The toxicity of MTP solution treated by the UV/sulfite AOP was calculated to be higher than that in the ARP by the Ecological Struc-ture Activity Relationships(ECOSAR)software,due to the accumulation of TPs with higher toxicity.展开更多
This study explored the catalytic mechanism and performance impacted by the materials ratio of Fe_(3)O_(4)-GO_(x) composites in three typical advanced oxidation processes(AOPs)of O_(3),peroxodisulfate(PDS)and photo-Fe...This study explored the catalytic mechanism and performance impacted by the materials ratio of Fe_(3)O_(4)-GO_(x) composites in three typical advanced oxidation processes(AOPs)of O_(3),peroxodisulfate(PDS)and photo-Fenton processes for tetracycline hydrochloride(TCH)degradation.The ratio of GO in the Fe_(3)O_(4)-GO_(x) composites exhibited different trends of degradation capacity in each AOPs based on different mechanisms.Fe_(3)O_(4)-rGO_(20wt%) exhibited the optimum catalytic performance which enhanced the ozone decomposition efficiency from 33.48%(ozone alone)to 51.83%with the major reactive oxygen species(ROS)of O_(2)·-.In PDS and photo-Fenton processes,Fe_(3)O_(4)-rGO_(5wt%) had the highest catalytic performance in PDS and H_(2)O_(2) decomposition for SO_(4)·–,and·OH generation,respectively.Compared with using PDS alone,PDS decomposition rate and TCH degradation rate could be increased by 5.97 and 1.73 times under Fe_(3)O_(4)-rGO_(5wt%) catalysis.In the photo-Fenton system,Fe_(3)O_(4)-rGO_(5wt%) with the best catalyst performance in H_(2)O_(2) decomposition,and TCH degradation rate increased by 2.02 times compared with blank group.Meantime,the catalytic mechanisms in those systems of that the ROS produced by conversion between Fe^(2+)/Fe^(3+)were also analyzed.展开更多
This study examined the effectiveness for degradation of hydrophobic (HPO),transphilic(TPI) and hydrophilic (HPI) fractions of natural organic matter (NOM) during UV/H_(2)O_(2),UV/TiO_(2)and UV/K2S2O8(UV/PS) advanced ...This study examined the effectiveness for degradation of hydrophobic (HPO),transphilic(TPI) and hydrophilic (HPI) fractions of natural organic matter (NOM) during UV/H_(2)O_(2),UV/TiO_(2)and UV/K2S2O8(UV/PS) advanced oxidation processes (AOPs).The changing characteristics of NOM were evaluated by dissolved organic carbon (DOC),the specific UV absorbance (SUVA),trihalomethanes formation potential (THMFP),organic halogen adsorbable on activated carbon formation potential (AOXFP) and parallel factor analysis of excitation–emission matrices (PARAFAC-EEMs).In the three UV-based AOPs,HPI fraction with low molecular weight and aromaticity was more likely to degradate than HPO and TPI,and the removal efficiency of SUVA for HPO was much higher than TPI and HPI fraction.In terms of the specific THMFP of HPO,TPI and HPI,a reduction was achieved in the UV/H_(2)O_(2)process,and the higest removal rate even reached to 83%.UV/TiO_(2)and UV/PS processes can only decrease the specific THMFP of HPI.The specific AOXFP of HPO,TPI and HPI fractions were all able to be degraded by the three UV-based AOPs,and HPO content is more susceptible to decompose than TPI and HPI content.UV/H_(2)O_(2)was found to be the most effective treatment for the removal of THMFP and AOXFP under given conditions.C1 (microbial or marine derived humic-like substances),C_(2) (terrestrially derived humic-like substances)and C_(3) (tryptophan-like proteins) fluorescent components of HPO fraction were fairly labile across the UV-based AOPs treatment.C_(3) of each fraction of NOM was the most resistant to degrade upon the UV-based AOPs.Results from this study may provide the prediction about the consequence of UV-based AOPs for the degradation of different fractions of NOM with varied characteristics.展开更多
In this study, we proposed a novel method to investigate the advanced oxidation process of neonicotinoids(NNIs) from the perspective of concomitant chemiluminescence(CL) reaction. It was found that in the presence of ...In this study, we proposed a novel method to investigate the advanced oxidation process of neonicotinoids(NNIs) from the perspective of concomitant chemiluminescence(CL) reaction. It was found that in the presence of cobalt ions with cyanoimino NNIs, acetamiprid(ACE) and thiacloprid(THI), could promote peroxymonosulfate and Ru(bpy)_(3)^(2+) to produce strong CL, but no CL occurred with nitro-involved NNIs as alternatives. Experimental dada from UV absorption spectra and chemiluminescence spectra suggested that new cyclic compounds might be formed during the reaction. Based on the results of free radical scavenging experiment and mass spectra, a new degradation and reaction mechanism of cyanoiminocontaining NNIs was proposed. ACE or THI were first attacked by SO_(4)^(·-) to form benzyl radicals, which in turn reacted with the carbon atoms of cyano group through electrophilic addition reaction in the formation of intramolecular ring. Then a redox reaction between Ru(bpy)_(3)^(3+) and imino group immediately took place with CL emission(610 nm). The new mechanistic knowledge would be meaningful for other contaminants for their interactions with PMS.展开更多
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 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.
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.
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.
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.
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.
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.
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.
文摘This paper,reports the performance of a wastewater treatment scale-pilot plant to treat 2 GPM(Gallons per Minute)discharges with 5,205 mg/L of pollutants expressed in COD(Chemical Oxygen Demand),from“Lomas de la Maestransa”a small community in Morelia City,Michoacan,Mexico.The scale-pilot plant is a train with(1)pretreatment with a triturated pump for floating solid,(2)primary treatment with“in line”coagulation,and rapid filtration to retain suspended colloids and dissolved solids higher of 5μm diameter,(3)double advanced oxidation as secondary treatment with ozone and heterogeneous photo catalysis to oxidize volatile solids,and(4)tertiary treatment with activated carbon to retain refractory compounds.Plant performance was analyzed by a certified laboratory that belongs to Potable Water,Sewage and Sanitation Department from Morelia City Government.Results show that treated water effluent complied with the Mexican Official Standard NOM-001-SEMARNAT-1996 for discharges into national waters,with exception of fecal coliforms,since the raw water contains an average of 64,228,351 MNP/100 mL of fecal coliforms,and in spite that we obtained a 99.998%efficiency,the maximum level allowable 2,000 MPN/100 mL standard,was exceeded by 400 MPN/100 mL.After this experience,the wastewater treatment plant is equipped with a residual chlorine tank to keep a 1.5 ppm chlorine residual concentration to keep the treated water clean.This project was possible because we had the support of the Morelia Sanitation Department.
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.
基金the National Natural Science Foundation of China(Nos.52170088 and 52070133)China Postdoctoral Science Foundation(No.2021M690844)Sichuan Science and Technology Program(No.2021JDRC0027)for financially supporting this study.
文摘Hospital sewage contains various harmful pharmaceutical contaminants(e.g.,antibiotics,anti-inflammatory agents,and painkillers)and pathogens(e.g.,bacteria,viruses,and parasites),whose direct discharge into the environment will induce diseases and pose a powerful threat to human health and safety,and environmental ecology.In recent years,advanced oxidation processes(AOPs),particularly photocatalysis,electrocatalysis,and ozone catalysis have been developed as widespread and effective techniques for hospital sewage treatments.However,there is a lack of systematic comparison and review of the prior studies on hospital sewage treatment using AOPs systems.This review elaborates on the mechanisms,removal efficiencies,and advantages/disadvantages of these AOPs systems for hospital wastewater decontamination and disinfection.Meanwhile,some novel and potential technologies such as photo-electrocatalysis,electro-peroxone,Fenton/Fenton-like,and piezoelectric catalysis are also included and summarized.Moreover,we further summarize and compare the capacity of these AOPs to treat the actual hospital wastewater under the impact of the water matrix and pH,and estimate the economic cost of these technologies for practical application.Finally,the future development directions of AOPs for hospital wastewater decontamination and disinfection have been prospected.Overall,this study provides a comparison and overview of these AOP systems in an attempt to raise extensive concerns about hospital wastewater decontamination and disinfection technologies and guide researchers to discover the future directions of technologies optimization,which would be a crucial step forward in the field of hospital sewage treatment.
基金the National Natural Science Foundation of China(Nos.42067057,42367060)the Science and Technology Plan Project of Yunnan Provincial Science and Technology Department,China(No.202101AT070087)the High-level Scientific Research Foundation for Talent Introduction of Kunming University of Science and Technology,China(No.10978172).
文摘Maximizing the sustainable recycling of spent lithium-ion batteries(LIBs)shows economic and environmental significance.This study recovered lithium cobaltate(LiCoO_(2),LCO)from spent LIBs cathode powder.The recovered LCO was then combined with NaHSO_(3)to remove refractory organic pollutants of carbamazepine(CBZ)in water.The degradation of CBZ reached 80.0%within 60 min,by 1O_(2),SO_(4),OH and O_(2)^(-)generated in the LCO/NaHSO_(3)reaction.The electron transfer between Co(III)and Co(II)was beneficial to the generation of free radicals.The LCO/NaHSO_(3)degraded CBZ effectively in both secondary outlet water and tap water.However,high concentrations of inorganic ions(Cl^(−),HCO_(3)^(-),HPO_(4)^(2-),SO_(2)−4,NO_(3)^(-))and natural organic matter(humic acid,HA)could inhibit the degradation of CBZ.After three cycles,the stability of the LCO/NaHSO_(3)system was demonstrated by the maintained high efficiency in the degradation of CBZ.The obtained data indicate that the LCO/NaHSO_(3)system holds great application potential in the field of advanced oxidation degradation of pollutants.
基金the National Natural Science Foundation of China(Nos.52170088 and 52070133)for financial support。
文摘Manganese oxides(MNO_(x)),as low-toxicity and high-abundance catalysts,have been demonstrated to hold great promise for application in advanced oxidation processes(AOPs).However,further application of this material is restricted due to its unsatisfactory oxidant activation efficiency.Fortunately,recently remarkable research on deep activation mechanisms and modification of MNO_(x)have been undertaken to improve its reactivity.Herein,modification enhancement mechanisms of MNO_(x)to efficiently degrade various organic contaminants were discussed and highlighted,including metal doping,coupling with other metal oxides,composite with carbonaceous material,and compounding with other support.The activation mechanisms of different MNO_(x)and derivative-modified material(such as doped MNO_(x),metal oxide-MNO_(x)hybrids,and MNO_(x)-carbonaceous material hybrids)were summarized in great details,which was specifically categorized into both radical and non-radical pathways.The effects of pH,inorganic ions,and natural organic matter on degradation reactions are also discussed.Finally,future research directions and perspectives are presented to provide a clear interpretation on the MNO_(x)initiated AOPs.
基金financially supported by National Natural Science Foundation of China(Nos.U22A20403,22006047)Natural Science Foundation of Hebei Province(Nos.E2021203140,B2021203016)Hebei Industrial Innovation and Entrepreneurship team(No.215A7608D)。
文摘In some industrial wastewater,heavy metals combine with organic complexing agents to form heavy metal complexes(HMCs).These HMCs can be difficult to decompose and remove through conventional techniques due to their higher stability than free heavy metal ions.In recent years,persulfate based advanced oxidation processes(PS-based AOPs)have been recognized as a viable technique for HMCs degradation.Nevertheless,a comprehensive and in-depth understanding of the relevant HMCs decomplexation mechanisms in PS-based AOPs is still lacking.This review delineates the current progress of HMCs decomplexation in PS-based AOPs.We discuss the distinctions between the two widely used oxidant types in PS-based AOPs techniques.Moreover,we summarize and highlight the decomplexation mechanisms based on electron and energy transfer,and degradation pathways of HMCs.We also emphasize the effects of environmental water constituents,namely p H,inorganic ions,and natural organic matter(NOM),on HMCs decomplexation.Ultimately,we identify the existing challenges and perspectives that will steer the direction of advancing PS-based AOPs to remove HMCs.
基金financially supported by National Natural Science Foundation of China(Nos.21976096,52170085 and 21773129)Tianjin Development Program for Innovation and Entrepreneurship+2 种基金Key Project of Natural Science Foundation of Tianjin(No.21JCZDJC00320)Tianjin Post-graduate Students Research and Innovation Project(No.2021YJSB013)Fundamental Research Funds for the Central Universities,Nankai University。
文摘As important emerging contaminants, antibiotics have caused potential hazards to the ecological environment and human health due to their extensive production and consumption. Among various techniques for removing antibiotics from wastewater, H_(2)O_(2)-based advanced oxidation processes(AOPs) have received increasing attention due to their fast reaction rate and strong oxidation capability. Hence this review critically discusses:(i) Recent research progress of AOPs with the addition of H_(2)O_(2) for antibiotics removal through different methods of H_(2)O_(2) activation;(ii) recent advances in AOPs that can in-situ generate and activate H_(2)O_(2) for antibiotics removal;(iii) H_(2)O_(2)-based AOPs as a combination with other techniques for the degradation and mineralization of antibiotics in wastewater. Future perspectives about H_(2)O_(2)-based AOPs are also presented to grasp the future research trend in the area.
基金This study was supported by the Guangdong introducing innovative and entrepreneurial teams(No.2019ZT08L213)the Key Special Project for Introduced Talents Team of Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou)(No.GML2019ZD0403)+2 种基金the National Natural Science Foundation of China(Nos.51979044 and 42177045)the Young Talent Project of Beijing Normal University at Zhuhai(No.310432101)We also thank the support received from China Scholarship Council(CSC)for providing a graduate fellowship to Y.C.(No.202006120356).
文摘The degradation of metoprolol(MTP)by the UV/sulfite with oxygen as an advanced reduction process(ARP)and that without oxygen as an advanced oxidation process(AOP)was comparatively studied herein.The degradation of MTP by both processes followed the first-order rate law with comparable reaction rate constants of 1.50×10^(-3)sec^(−1)and 1.20×10^(-3)sec^(−1),respectively.Scavenging experiments demonstrated that both e^(−)_(aq)and H·played a crucial role in MTP degradation by the UV/sulfite as an ARP,while SO_(4)^(·−)was the dominant oxidant in the UV/sulfite AOP.The degradation kinetics of MTP by the UV/sulfite as an ARP and AOP shared a similar pH dependence with a minimum rate obtained around pH 8.The results could be well explained by the pH impacts on the MTP speciation and sulfite species.Totally six transformation products(TPs)were identified from MTP degradation by the UV/sulfite ARP,and two additional ones were detected in the UV/sulfite AOP.The benzene ring and ether groups of MTP were proposed as the major reactive sites for both processes based on molecular orbital calculations by density functional theory(DFT).The similar degradation products of MTP by the UV/sulfite process as an ARP and AOP indicated that e^(−)_(aq)/H·and SO_(4)^(·−)might share similar reaction mechanisms,primarily including hydroxylation,dealkylation,and H abstraction.The toxicity of MTP solution treated by the UV/sulfite AOP was calculated to be higher than that in the ARP by the Ecological Struc-ture Activity Relationships(ECOSAR)software,due to the accumulation of TPs with higher toxicity.
基金supported by the National Natural Science Foundation of China(Nos.21906088,51902169,52170039)the National Science Foundation for Post-doctoral Scientists of China(No.2021T140165)+3 种基金the Natural Science Foundation of Heilongjiang Province,China(No.LH2020B023)Department of Education Heilongjiang Province(No.135309338)University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(Nos.UNPYSCT-2020068,UNPYSCT-2020067)the financial support by the Heilongjiang Provincial Key Laboratory of Surface Active Agent and Auxiliary(No.BMHXJKF009)。
文摘This study explored the catalytic mechanism and performance impacted by the materials ratio of Fe_(3)O_(4)-GO_(x) composites in three typical advanced oxidation processes(AOPs)of O_(3),peroxodisulfate(PDS)and photo-Fenton processes for tetracycline hydrochloride(TCH)degradation.The ratio of GO in the Fe_(3)O_(4)-GO_(x) composites exhibited different trends of degradation capacity in each AOPs based on different mechanisms.Fe_(3)O_(4)-rGO_(20wt%) exhibited the optimum catalytic performance which enhanced the ozone decomposition efficiency from 33.48%(ozone alone)to 51.83%with the major reactive oxygen species(ROS)of O_(2)·-.In PDS and photo-Fenton processes,Fe_(3)O_(4)-rGO_(5wt%) had the highest catalytic performance in PDS and H_(2)O_(2) decomposition for SO_(4)·–,and·OH generation,respectively.Compared with using PDS alone,PDS decomposition rate and TCH degradation rate could be increased by 5.97 and 1.73 times under Fe_(3)O_(4)-rGO_(5wt%) catalysis.In the photo-Fenton system,Fe_(3)O_(4)-rGO_(5wt%) with the best catalyst performance in H_(2)O_(2) decomposition,and TCH degradation rate increased by 2.02 times compared with blank group.Meantime,the catalytic mechanisms in those systems of that the ROS produced by conversion between Fe^(2+)/Fe^(3+)were also analyzed.
基金supported by the “Central leading local” Science and Technology Development Fund Project of Shandong Province (No.YDZX202037 00001642)the Key Research and Development Plan of Shandong Province(NO.2020CXGC011406),the Natural Science Foundation of Shandong Province (No.ZR2021ME166)the Special Project of Taishan Scholar Construction Engineering (No.ts201712084)。
文摘This study examined the effectiveness for degradation of hydrophobic (HPO),transphilic(TPI) and hydrophilic (HPI) fractions of natural organic matter (NOM) during UV/H_(2)O_(2),UV/TiO_(2)and UV/K2S2O8(UV/PS) advanced oxidation processes (AOPs).The changing characteristics of NOM were evaluated by dissolved organic carbon (DOC),the specific UV absorbance (SUVA),trihalomethanes formation potential (THMFP),organic halogen adsorbable on activated carbon formation potential (AOXFP) and parallel factor analysis of excitation–emission matrices (PARAFAC-EEMs).In the three UV-based AOPs,HPI fraction with low molecular weight and aromaticity was more likely to degradate than HPO and TPI,and the removal efficiency of SUVA for HPO was much higher than TPI and HPI fraction.In terms of the specific THMFP of HPO,TPI and HPI,a reduction was achieved in the UV/H_(2)O_(2)process,and the higest removal rate even reached to 83%.UV/TiO_(2)and UV/PS processes can only decrease the specific THMFP of HPI.The specific AOXFP of HPO,TPI and HPI fractions were all able to be degraded by the three UV-based AOPs,and HPO content is more susceptible to decompose than TPI and HPI content.UV/H_(2)O_(2)was found to be the most effective treatment for the removal of THMFP and AOXFP under given conditions.C1 (microbial or marine derived humic-like substances),C_(2) (terrestrially derived humic-like substances)and C_(3) (tryptophan-like proteins) fluorescent components of HPO fraction were fairly labile across the UV-based AOPs treatment.C_(3) of each fraction of NOM was the most resistant to degrade upon the UV-based AOPs.Results from this study may provide the prediction about the consequence of UV-based AOPs for the degradation of different fractions of NOM with varied characteristics.
基金financial supports from the National Natural Science Foundation of China(Nos.81960600and 81760601)the Natural Science Foundation of Jiangxi Province(Nos.20192BAB205089 and 20192BAB205091)。
文摘In this study, we proposed a novel method to investigate the advanced oxidation process of neonicotinoids(NNIs) from the perspective of concomitant chemiluminescence(CL) reaction. It was found that in the presence of cobalt ions with cyanoimino NNIs, acetamiprid(ACE) and thiacloprid(THI), could promote peroxymonosulfate and Ru(bpy)_(3)^(2+) to produce strong CL, but no CL occurred with nitro-involved NNIs as alternatives. Experimental dada from UV absorption spectra and chemiluminescence spectra suggested that new cyclic compounds might be formed during the reaction. Based on the results of free radical scavenging experiment and mass spectra, a new degradation and reaction mechanism of cyanoiminocontaining NNIs was proposed. ACE or THI were first attacked by SO_(4)^(·-) to form benzyl radicals, which in turn reacted with the carbon atoms of cyano group through electrophilic addition reaction in the formation of intramolecular ring. Then a redox reaction between Ru(bpy)_(3)^(3+) and imino group immediately took place with CL emission(610 nm). The new mechanistic knowledge would be meaningful for other contaminants for their interactions with PMS.