Current research on heterogeneous advanced oxidation processes(HAOPs)predominantly emphasizes catalyst iteration and innovation.Significant efforts have been made to regulate the electron structure and optimize the el...Current research on heterogeneous advanced oxidation processes(HAOPs)predominantly emphasizes catalyst iteration and innovation.Significant efforts have been made to regulate the electron structure and optimize the electron distribution,thereby increasing the catalytic activity.However,this focus often overshadows an equally essential aspect of HAOPs:the adsorption effect.Adsorption is a critical initiator for triggering the interaction of oxidants and contaminants with heterogeneous catalysts.The efficacy of these interactions is influenced by a variety of physicochemical properties,including surface chemistry and pore sizes,which determine the affinities between contaminants and material surfaces.This dispar ity in affinity is pivotal because it underpins the selective removal of contaminants,especially in complex waste streams containing diverse contaminants and competing matrices.Consequently,understanding and mastering these interfacial interactions is fundamentally indispensable not only for improving pro cess efficiency but also for enhancing the selectivity of contaminant removal.Herein,we highlight the importance of adsorption-driven interfacial interactions for fundamentally elucidating the catalytic mechanisms of HAOPs.Such interactions dictate the overall performance of the treatment processes by balancing the adsorption,reaction,and desorption rates on the catalyst surfaces.Elucidating the adsorption effect not only shifts the paradigm in understanding HAOPs but also improves their practical ity in water treatment and wastewater decontamination.Overall,we propose that revisiting adsorption driven interfacial interactions holds great promise for optimizing catalytic processes to develop effective HAOP strategies.展开更多
The global concern surrounding the advancement of methods for treating wastewater and polluted soil has markedly increased over time.While electrochemical advanced oxidation processes(EAOPs)and biotreatments are commo...The global concern surrounding the advancement of methods for treating wastewater and polluted soil has markedly increased over time.While electrochemical advanced oxidation processes(EAOPs)and biotreatments are commonly employed technologies for remediating wastewater and polluted soil,their widespread adoption is hindered by their limitations,which include high costs associated with EAOPs and prolonged remediation time of biotreatments.In the review,we provided an overviewof EAOP technology and biotreatment,emphasizing the critical aspects involved in building a combined system.This review systematically evaluates recent research that combines EAOPswith bioremediation for treating wastewater or contaminated soil as pretreatment or post-treatment process.Research findings suggest that the combined treatment method represents a promising and competitive technology that can overcome some of the limitations of individual treatments.Additionally,we discussed the potential applications of this technology in varying levels of wastewater and soil pollution,as well as the underlying combination mechanisms.展开更多
Enhancing the corrosion resistance of carriers within Fenton-like systems and inhibiting the migration and aggregation of single atoms in reaction environments are essential for maintaining both high activity and stab...Enhancing the corrosion resistance of carriers within Fenton-like systems and inhibiting the migration and aggregation of single atoms in reaction environments are essential for maintaining both high activity and stability at catalytic sites,thus meeting fundamental requirements for practical application.The Fenton-like process of activating various strong oxidants by silicon-based single atom catalysts(SACs)prepared based on silicon-based materials(mesoporous silica,silicon-based minerals,and organosilicon materials)has unique advantages such as structural stability(especially important under strong oxidation conditions)and environmental protection.In this paper,the preparation strategies for the silicon-based SACs were assessed first,and the structural characteristics of various silicon-based SACs are systematically discussed,their application process and mechanism in Fenton-like process to achieve water purification are investigated,and the progress of Fenton-like process in density functional theory(DFT)of siliconbased derived single atom catalysts is summarized.In this paper,the preparation strategies and applications of silicon-based derived SACs are analyzed in depth,and their oxidation activities and pathways to different pollutants in water are reviewed.In addition,this paper also summarizes the device design and application of silicon-based derived SACs,and prospects the future development of silicon-based SACs in Fenton-like applications.展开更多
Efficient and innovative nano-catalytic oxidation technologies offer a breakthrough in removing emerging contaminants(ECs)from water,surpassing the limitations of traditional methods.Environmental functional materials...Efficient and innovative nano-catalytic oxidation technologies offer a breakthrough in removing emerging contaminants(ECs)from water,surpassing the limitations of traditional methods.Environmental functional materials(EFMs),particularly high-end oxidation systems using eco-friendly nanomaterials,show promise for absorbing and degrading ECs.This literature review presents a comprehensive analysis of diverse traditional restoration techniques-biological,physical,and chemical-assessing their respective applications and limitations in pesticide-contaminated water purification.Through meticulous comparison,we unequivocally advocate for the imperative integration of environmentally benign nanomaterials,notably titanium-based variants,in forthcoming methodologies.Our in-depth exploration scrutinizes the catalytic efficacy,underlying mechanisms,and adaptability of pioneering titanium-based nanomaterials across a spectrum of environmental contexts.Additionally,strategic recommendations are furnished to surmount challenges and propel the frontiers of implementing eco-friendly nanomaterials in practical water treatment scenarios.展开更多
The widespread occurrence of antibiotics in wastewater aroused serious attention.UV-based advanced oxidation processes(UV-AOPs)are powerful technologies in removing antibiotics in wastewater,which include UV/catalyst,...The widespread occurrence of antibiotics in wastewater aroused serious attention.UV-based advanced oxidation processes(UV-AOPs)are powerful technologies in removing antibiotics in wastewater,which include UV/catalyst,UV/H_(2)O_(2),UV/Fenton,UV/persulfate,UV/chlorine,UV/ozone,and UV/peracetic acid.In this review,we collated recent advances in application of UV-AOPs for the abatement of fiuoroquinolones(FQs)as widely used class of antibiotics.Representative FQs of ciprofioxacin,norfioxacin,ofioxacin,and enrofioxacin were most extensively studied in the state-of-art studies.The evolvement of gas-state and solid-state UV light sources was presented and batch and continuous fiow UV reactors were compared towards practical applications in UV-AOPs.Generally,degradation of FQs followed the pseudo-first order kinetics in UV-AOPs and strongly affected by the operating factors and components of water matrix.Participation of reactive species and transformation mechanisms of FQs were compared among different UV-AOPs.Challenges and future prospects were pointed out for providing insights into the practical application of UV-AOPs for antibiotic remediation in wastewater.展开更多
Low-valent sulfur oxy-acid salts(LVSOs)represent a category of oxygen-containing salts characterized by their potent reducing capabilities.Notably,sulfite,dithionite,and thiosulfate are prevalent reducing agents that ...Low-valent sulfur oxy-acid salts(LVSOs)represent a category of oxygen-containing salts characterized by their potent reducing capabilities.Notably,sulfite,dithionite,and thiosulfate are prevalent reducing agents that are readily available,cost-effective,and exhibit minimal ecological toxicity.These LVSOs have the ability to generate or promote the generation of strong oxidants or reductants,which makes them widely used in advanced oxidation processes(AOPs)and advanced reduction processes(ARPs).This article provides a comprehensive review of the recent advancements in AOPs and ARPs involving LVSOs,alongside an examination of the fundamental principles governing the generation of active species within these processes.LVSOs fulfill three primary functions in AOPs:Serving as sources of reactive oxygen species(ROS),auxiliary agents,and activators.Particular attention is devoted to elucidating the reaction mechanisms through which LVSOs,in conjunction with metal ions,metal oxides,ultraviolet light(UV),and ozone,produce potent oxidizing agents in both homogeneous and heterogeneous systems.Regarding ARPs,this review delineates the mechanisms by which LVSOs generate strong reducing agents,including hydrated electrons,hydrogen radicals,and sulfite radicals,under UV irradiation,while also exploring the interactions between these reductants and pollutants.The review identifies existing gaps within the current framework and proposes future research avenues to address these challenges.展开更多
Addressing the growing challenge of water contamination,this study comparatively evaluated a persulfate(PDS)system activated by nonradical nitrogen-doped carbon nanotubes(N-CNTs)versus a PDS system activated by radica...Addressing the growing challenge of water contamination,this study comparatively evaluated a persulfate(PDS)system activated by nonradical nitrogen-doped carbon nanotubes(N-CNTs)versus a PDS system activated by radical-based iron(Fe^(2+)),both used for the degradation of bisphenol A(BPA).The N-CNTs/PDS system,driven by the electron transfer mechanism,achieved remarkable 90.9%BPA removal within 30 min at high BPA concentrations,significantly outperforming the Fe^(2+)/PDS system,which attained only 38.9%removal.The N-CNTs/PDS system maintained robust degradation efficiency across a wide range of BPA concentrations and exhibited a high degree of resilience in diverse water matrices.By directly abstracting electrons from BPA molecules,the N-CNTs/PDS system effectively minimised oxidant wastage and mitigated the risk of secondary pollution,ensuring efficient utilisation of active sites on N-CNTs and sustaining a high catalytic rate.The formation of the N-CNTs-PDS^(*)complex significantly enhanced BPA degradation and mineralisation,thereby optimising PDS consumption.These findings highlight the unparalleled advantages of the N-CNTs/PDS system in managing complex wastewater,offering a promising and innovative solution for treating complex industrial wastewater and advancing environmental remediation efforts.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 recent years,with the emergence of new pollutants,the effective treatment of wastewater has become very important.Persulfate-based advanced oxidation processes have been successfully applied to the treatment of was...In recent years,with the emergence of new pollutants,the effective treatment of wastewater has become very important.Persulfate-based advanced oxidation processes have been successfully applied to the treatment of wastewater,such as wastewater containing antibiotics,pharmaceuticals and personal care products,dyes,endocrine-disrupting chemicals,chlorinated organic pollutants,and phenolics,for the degradation of refractory organic contaminants.This paper summarizes the production of sulfate radicals,which can be generated by the activation of persulfate via conventional and emerging approaches.The existing problems of persulfate-based advanced oxidation processes were analyzed in detail,including residual sulfates,coexisting factors(coexisting inorganic anions and natural organic matter),and energy consumption.This paper proposes corresponding possible solutions to the problems mentioned above,and this paper could provide a reference for the application of persulfate-based advanced oxidation processes in actual wastewater treatment.展开更多
Heavy metal complexes with high mobility are widely distributed in wastewater from modern industries,which are mo re stable and refracto ry than free heavy metal ions.Their re movals from wastewater draw increasing at...Heavy metal complexes with high mobility are widely distributed in wastewater from modern industries,which are mo re stable and refracto ry than free heavy metal ions.Their re movals from wastewater draw increasing attentions and various technologies have been developed,among which advanced oxidation processes(AOPs)are more effectively and promising.Progresses on five representative types of AOPs,including Fenton(like)oxidation,electrochemical oxidation,photocatalytic oxidation,ozonation and discharge plasma oxidation for heavy metal complexe s degradation are summarized in this review.Their rationales,advantages,applications,challenges and prospects are introduced independently.Combinations among these AOPs,such as electrochemical Fenton oxidation and photoelectrocatalytic oxidation,are also comprehensively highlighted.Future efforts should be made to reduce acid requirement and scale up for practical applications of AOPs for heavy metal complex degradation efficiently and cost-effectively.展开更多
Refractory organic pollutants in water threaten human health and environmental safety,and advanced oxidation processes (AOPs) are effective for the degradation of these pollutants.Catalysts play vital role in AOPs,and...Refractory organic pollutants in water threaten human health and environmental safety,and advanced oxidation processes (AOPs) are effective for the degradation of these pollutants.Catalysts play vital role in AOPs,and Ce-based catalysts have exhibited excellent performance.Recently,the development and application of Ce-based catalysts in various AOPs have been reported.Our study conducts the first review in this rapid growing field.This paper clarifies the variety and properties of Ce-based catalysts.Their applications in different AOP systems (catalytic ozonation,photodegradation,Fenton-like reactions,sulfate radicalbased AOPs,and catalytic sonochemistry) are discussed.Different Ce-based catalysts suit different reaction systems and produce different active radicals.Finally,future research directions of Ce-based catalysts in AOP systems are suggested.展开更多
The electrochemical advanced oxidation processes(EAOPs) have been extensively applied in the treatment of organic pollutants degradation.Herein,the mini review provides the coupling systems about EAOPs and different o...The electrochemical advanced oxidation processes(EAOPs) have been extensively applied in the treatment of organic pollutants degradation.Herein,the mini review provides the coupling systems about EAOPs and different oxidants(e.g.,persulfate(PS),peroxymonosulfate(PMS),and ozone(O3)),including EAOPs-PS systems,EAOPs-PMS systems,EAOPs-peroxone systems,and photoelectro-oxidants systems,for the organic compounds degradation.The coupling system of EAOPs with oxidants is an effective way to improve the generated free radicals(e.g.,HO^·and SO4^·-) concentration and to accelerate pollutant degradation.In this review,we make a summary of the homogeneous and heterogeneous EAOPs-oxidant processes.The reaction mechanisms of EAOPs combined with different oxidants are elucidated in detail,as well as the synergistic effect for improving the degradation and mineralization efficiency.展开更多
Herein,we prepa red novel three-dimensional(3D)gear-s haped Co3O4@C(Co3O4 modified by amorphous carbon)and sheet-like SnO2/CC(SnO2 grow on the carbon cloth)as anode and cathode to achieve efficient removal of 4-nitrop...Herein,we prepa red novel three-dimensional(3D)gear-s haped Co3O4@C(Co3O4 modified by amorphous carbon)and sheet-like SnO2/CC(SnO2 grow on the carbon cloth)as anode and cathode to achieve efficient removal of 4-nitrophenol(4-NP)in the presence of peroxymonosulfate(PMS)and simultaneous electrocatalytic reduction of CO2,respectively.In this process,4-NP was mineralized into CO2 by the Co3O4@C,and the generated CO2 was reduced into HCOOH by the sheet-like SnO2/CC cathode.Compared with the pure Co0.5(Co3O4 was prepared using 0.5 g urea)with PMS(30 mg,0.5 g/L),the degradation efficiency of 4-NP(60 mL,10 mg/L)increased from 74.5%-85.1%in 60 min using the Co0.5 modified by amorphous carbon(Co0.5@C).Furthermore,when the voltage of 1.0 V was added in the anodic system of Co0.5@C with PMS(30 mg,0.5 g/L),the degradation efficiency of 4-NP increased from 85.1%-99.1%when Pt was used as cathode.In the experiments of 4-NP degradation coupled with simultaneous electrocatalytic CO2 reduction,the degradation efficiency of 4-NP was 99.0%in the anodic system of Co0.5@C with addition of PMS(30 mg,0.5 g/L),while the Faraday efficiency(FE)of HCOOH was 24.1%at voltage of-1.3 V using the SnO2/CC as cathode.The results showed that the anode of Co3O4 modified by amorphous carbon can markedly improve the degradation efficiency of 4-NP,while the cathode of SnO2/CC can greatly improve the FE and selectivity of CO2 reduction to HCOOH and the stability of cathode.Finally,the promotion mechanism was proposed to explain the degradation of organic pollutants and reduction of CO2 into HCOOH in the process of electrocatalysis coupled with advanced oxidation processes(AOPs)and simultaneous CO2 reduction.展开更多
Due to the formation of disinfection by-products and high concentrations of Al residue in drinking water purification, humic substances are a major component of organic matter in natural waters and have therefore rece...Due to the formation of disinfection by-products and high concentrations of Al residue in drinking water purification, humic substances are a major component of organic matter in natural waters and have therefore received a great deal of attention in recent years. We investigated the effects of advanced oxidation pretreatment methods usually applied for removing dissolved organic matters on residual Al control. Results showed that the presence of humic acid increased residual Al concentration notably. With 15 mg/L of humic acid in raw water, the concentrations of soluble aluminum and total aluminum in the treated water were close to the quantity of Al addition. After increasing coagulant dosage from 12 to 120 mg/L, the total-Al in the treated water was controlled to below 0.2 mg/L. Purification systems with ozonation, chlorination, or potassium permanganate oxidation pretreatment units had little effects on residual Al control; while UV radiation decreased Al concentration notably. Combined with ozonation, the effects of UV radiation were enhanced. Optimal dosages were 0.5 mg O 3 /mg C and 3 hr for raw water with 15 mg/L of humic acid. Under UV light radiation, the combined forces or bonds that existed among humic acid molecules were destroyed; adsorption sites increased positively with radiation time, which promoted adsorption of humic acid onto polymeric aluminum and Al（OH） 3 （s）. This work provides a new solution for humic acid coagulation and residual Al control for raw water with humic acid purification.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
In the field of advanced oxidation processes(AOPs) of wastewater, many materials can be used as heterogeneous catalysts. The role of these catalysts is to activate oxidants and generate reactive oxygen species(ROS) to...In the field of advanced oxidation processes(AOPs) of wastewater, many materials can be used as heterogeneous catalysts. The role of these catalysts is to activate oxidants and generate reactive oxygen species(ROS) to decompose refractory pollutants. Perovskite oxide, an emerging catalyst in the field of AOPs, has been extensively studied in wastewater treatment. Nevertheless, the application of perovskite in AOP systems still faces some problems, such as leaching of metal ions, a small surface area, a low number of active sites, etc. Herein, this critical review comparatively examines the activation mechanisms of peroxymonosulfate, hydrogen peroxide, and peroxydisulfate. Furthermore, the formation pathways of oxidizing species based on recent advances in experimental and theoretical studies were evaluated. In addition, the impacts of water parameters and constituents such as initial p H, oxidant concentration, catalyst dosage,natural organic matter, halide, phosphate, and carbonate were discussed. Finally, a critical discussion and prospects of mechanism exploration and possible materials development are proposed to confront the existing challenges in the application of perovskite oxides in AOPs.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
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
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
Metal-organic frameworks(MOFs)materials with highly ordered and porous crystalline structure,have excellent performance in advanced oxidation progresses(AOPs)for organic contaminants degradation in water treatment.Thi...Metal-organic frameworks(MOFs)materials with highly ordered and porous crystalline structure,have excellent performance in advanced oxidation progresses(AOPs)for organic contaminants degradation in water treatment.This review intends to summarize the timely references and insights for the recent advances in MOFs that are used in AOPs.Starting with the preparation methodologies,including conventional hydrothermal method,electrochemical method,sol-gel method,and emerging microwave and ultrasound assisted synthesis methods.Application and mechanism for MOFs using in various AOPs of Fenton-like,photocatalysis,catalytic ozonation,persulfate catalysis and other emerging oxidation methods are emphatically discussed.We hope this review can comprehensively summarize the research and application progress of MOFs in AOPs,deepen the understanding of the catalytic mechanisms.展开更多
基金supported by the National Key Research and Development Program of China(2022YFC3205300)the National Natural Science Foundation of China(22176124).
文摘Current research on heterogeneous advanced oxidation processes(HAOPs)predominantly emphasizes catalyst iteration and innovation.Significant efforts have been made to regulate the electron structure and optimize the electron distribution,thereby increasing the catalytic activity.However,this focus often overshadows an equally essential aspect of HAOPs:the adsorption effect.Adsorption is a critical initiator for triggering the interaction of oxidants and contaminants with heterogeneous catalysts.The efficacy of these interactions is influenced by a variety of physicochemical properties,including surface chemistry and pore sizes,which determine the affinities between contaminants and material surfaces.This dispar ity in affinity is pivotal because it underpins the selective removal of contaminants,especially in complex waste streams containing diverse contaminants and competing matrices.Consequently,understanding and mastering these interfacial interactions is fundamentally indispensable not only for improving pro cess efficiency but also for enhancing the selectivity of contaminant removal.Herein,we highlight the importance of adsorption-driven interfacial interactions for fundamentally elucidating the catalytic mechanisms of HAOPs.Such interactions dictate the overall performance of the treatment processes by balancing the adsorption,reaction,and desorption rates on the catalyst surfaces.Elucidating the adsorption effect not only shifts the paradigm in understanding HAOPs but also improves their practical ity in water treatment and wastewater decontamination.Overall,we propose that revisiting adsorption driven interfacial interactions holds great promise for optimizing catalytic processes to develop effective HAOP strategies.
基金supported by the National Natural Science Foundation of China(No.51709103)the Natural Science Foundation of Hunan Province,China(Nos.2018JJ3242 and 2021JJ30362)the Science and Technology Innovation Leading Plan of High Tech Industry in Hunan Province(No.2021GK4055).
文摘The global concern surrounding the advancement of methods for treating wastewater and polluted soil has markedly increased over time.While electrochemical advanced oxidation processes(EAOPs)and biotreatments are commonly employed technologies for remediating wastewater and polluted soil,their widespread adoption is hindered by their limitations,which include high costs associated with EAOPs and prolonged remediation time of biotreatments.In the review,we provided an overviewof EAOP technology and biotreatment,emphasizing the critical aspects involved in building a combined system.This review systematically evaluates recent research that combines EAOPswith bioremediation for treating wastewater or contaminated soil as pretreatment or post-treatment process.Research findings suggest that the combined treatment method represents a promising and competitive technology that can overcome some of the limitations of individual treatments.Additionally,we discussed the potential applications of this technology in varying levels of wastewater and soil pollution,as well as the underlying combination mechanisms.
基金supported by National Natural Science Foundation of China(No.52170086)Natural Science Foundation of Shandong Province(No.ZR2021ME013)+1 种基金Natural science Foundation of Shaanxi province(No.2024JC-YBQN-0252)Special Scientific Research Project of Hanzhong City-Shaanxi University of Technology Co-construction State Key Laboratory(No.SXJ2106)。
文摘Enhancing the corrosion resistance of carriers within Fenton-like systems and inhibiting the migration and aggregation of single atoms in reaction environments are essential for maintaining both high activity and stability at catalytic sites,thus meeting fundamental requirements for practical application.The Fenton-like process of activating various strong oxidants by silicon-based single atom catalysts(SACs)prepared based on silicon-based materials(mesoporous silica,silicon-based minerals,and organosilicon materials)has unique advantages such as structural stability(especially important under strong oxidation conditions)and environmental protection.In this paper,the preparation strategies for the silicon-based SACs were assessed first,and the structural characteristics of various silicon-based SACs are systematically discussed,their application process and mechanism in Fenton-like process to achieve water purification are investigated,and the progress of Fenton-like process in density functional theory(DFT)of siliconbased derived single atom catalysts is summarized.In this paper,the preparation strategies and applications of silicon-based derived SACs are analyzed in depth,and their oxidation activities and pathways to different pollutants in water are reviewed.In addition,this paper also summarizes the device design and application of silicon-based derived SACs,and prospects the future development of silicon-based SACs in Fenton-like applications.
基金supported by the Research Platform Open Fund Project of Zhejiang Industry and Trade Vocation College(No.Kf202203)the Scientific Research Project of CCCC First Harbor Engineering Company Ltd.(No.2022-7-2)+3 种基金the National Natural Science Foundation of China(No.22406142)the Fellowship of China National Postdoctoral Program for Innovative Talents(No.BX20230262)the Fellowship of China Postdoctoral Science Foundation(No.2023M732636)the Shanghai Post-doctoral Excellence Program(No.2023755).
文摘Efficient and innovative nano-catalytic oxidation technologies offer a breakthrough in removing emerging contaminants(ECs)from water,surpassing the limitations of traditional methods.Environmental functional materials(EFMs),particularly high-end oxidation systems using eco-friendly nanomaterials,show promise for absorbing and degrading ECs.This literature review presents a comprehensive analysis of diverse traditional restoration techniques-biological,physical,and chemical-assessing their respective applications and limitations in pesticide-contaminated water purification.Through meticulous comparison,we unequivocally advocate for the imperative integration of environmentally benign nanomaterials,notably titanium-based variants,in forthcoming methodologies.Our in-depth exploration scrutinizes the catalytic efficacy,underlying mechanisms,and adaptability of pioneering titanium-based nanomaterials across a spectrum of environmental contexts.Additionally,strategic recommendations are furnished to surmount challenges and propel the frontiers of implementing eco-friendly nanomaterials in practical water treatment scenarios.
基金the financial support from National Natural Science Foundation of China(Nos.52100204 and 52330005)Beijing Outstanding Young Scientist Program(No.BJJWZYJH01201910004016)。
文摘The widespread occurrence of antibiotics in wastewater aroused serious attention.UV-based advanced oxidation processes(UV-AOPs)are powerful technologies in removing antibiotics in wastewater,which include UV/catalyst,UV/H_(2)O_(2),UV/Fenton,UV/persulfate,UV/chlorine,UV/ozone,and UV/peracetic acid.In this review,we collated recent advances in application of UV-AOPs for the abatement of fiuoroquinolones(FQs)as widely used class of antibiotics.Representative FQs of ciprofioxacin,norfioxacin,ofioxacin,and enrofioxacin were most extensively studied in the state-of-art studies.The evolvement of gas-state and solid-state UV light sources was presented and batch and continuous fiow UV reactors were compared towards practical applications in UV-AOPs.Generally,degradation of FQs followed the pseudo-first order kinetics in UV-AOPs and strongly affected by the operating factors and components of water matrix.Participation of reactive species and transformation mechanisms of FQs were compared among different UV-AOPs.Challenges and future prospects were pointed out for providing insights into the practical application of UV-AOPs for antibiotic remediation in wastewater.
基金supported by Natural Science Foundation of China(Nos.52070133,42107073,42477075)Natural Science Foundation of Sichuan Province(No.2024NSFSC0130)+2 种基金the Sichuan Science and Technology Program(No.2024NSFTD0014)Key Laboratory of Jiangxi Province for Persistent Pollutants Prevention Control and Resource Reuse(No.2023SSY02061)Key R&D Program of Heilongjiang Province(No.2023ZX02C01)。
文摘Low-valent sulfur oxy-acid salts(LVSOs)represent a category of oxygen-containing salts characterized by their potent reducing capabilities.Notably,sulfite,dithionite,and thiosulfate are prevalent reducing agents that are readily available,cost-effective,and exhibit minimal ecological toxicity.These LVSOs have the ability to generate or promote the generation of strong oxidants or reductants,which makes them widely used in advanced oxidation processes(AOPs)and advanced reduction processes(ARPs).This article provides a comprehensive review of the recent advancements in AOPs and ARPs involving LVSOs,alongside an examination of the fundamental principles governing the generation of active species within these processes.LVSOs fulfill three primary functions in AOPs:Serving as sources of reactive oxygen species(ROS),auxiliary agents,and activators.Particular attention is devoted to elucidating the reaction mechanisms through which LVSOs,in conjunction with metal ions,metal oxides,ultraviolet light(UV),and ozone,produce potent oxidizing agents in both homogeneous and heterogeneous systems.Regarding ARPs,this review delineates the mechanisms by which LVSOs generate strong reducing agents,including hydrated electrons,hydrogen radicals,and sulfite radicals,under UV irradiation,while also exploring the interactions between these reductants and pollutants.The review identifies existing gaps within the current framework and proposes future research avenues to address these challenges.
基金supported by the Natural Science Foundation of Inner Mongolia Autonomous Region of China(Grant No.2024LHMS05048).
文摘Addressing the growing challenge of water contamination,this study comparatively evaluated a persulfate(PDS)system activated by nonradical nitrogen-doped carbon nanotubes(N-CNTs)versus a PDS system activated by radical-based iron(Fe^(2+)),both used for the degradation of bisphenol A(BPA).The N-CNTs/PDS system,driven by the electron transfer mechanism,achieved remarkable 90.9%BPA removal within 30 min at high BPA concentrations,significantly outperforming the Fe^(2+)/PDS system,which attained only 38.9%removal.The N-CNTs/PDS system maintained robust degradation efficiency across a wide range of BPA concentrations and exhibited a high degree of resilience in diverse water matrices.By directly abstracting electrons from BPA molecules,the N-CNTs/PDS system effectively minimised oxidant wastage and mitigated the risk of secondary pollution,ensuring efficient utilisation of active sites on N-CNTs and sustaining a high catalytic rate.The formation of the N-CNTs-PDS^(*)complex significantly enhanced BPA degradation and mineralisation,thereby optimising PDS consumption.These findings highlight the unparalleled advantages of the N-CNTs/PDS system in managing complex wastewater,offering a promising and innovative solution for treating complex industrial wastewater and advancing environmental remediation efforts.
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the National Natural Science Foundation of China(No.51678185)Talents of High Level Scientific Research Foundation of Qingdao Agricultural University(No.6651120004).
文摘In recent years,with the emergence of new pollutants,the effective treatment of wastewater has become very important.Persulfate-based advanced oxidation processes have been successfully applied to the treatment of wastewater,such as wastewater containing antibiotics,pharmaceuticals and personal care products,dyes,endocrine-disrupting chemicals,chlorinated organic pollutants,and phenolics,for the degradation of refractory organic contaminants.This paper summarizes the production of sulfate radicals,which can be generated by the activation of persulfate via conventional and emerging approaches.The existing problems of persulfate-based advanced oxidation processes were analyzed in detail,including residual sulfates,coexisting factors(coexisting inorganic anions and natural organic matter),and energy consumption.This paper proposes corresponding possible solutions to the problems mentioned above,and this paper could provide a reference for the application of persulfate-based advanced oxidation processes in actual wastewater treatment.
基金the National Natural Science Foundation of China(NSFC)(No.41672237)the Beijing Natural Science Foundation(No.8192040)。
文摘Heavy metal complexes with high mobility are widely distributed in wastewater from modern industries,which are mo re stable and refracto ry than free heavy metal ions.Their re movals from wastewater draw increasing attentions and various technologies have been developed,among which advanced oxidation processes(AOPs)are more effectively and promising.Progresses on five representative types of AOPs,including Fenton(like)oxidation,electrochemical oxidation,photocatalytic oxidation,ozonation and discharge plasma oxidation for heavy metal complexe s degradation are summarized in this review.Their rationales,advantages,applications,challenges and prospects are introduced independently.Combinations among these AOPs,such as electrochemical Fenton oxidation and photoelectrocatalytic oxidation,are also comprehensively highlighted.Future efforts should be made to reduce acid requirement and scale up for practical applications of AOPs for heavy metal complex degradation efficiently and cost-effectively.
基金supported by National Water Pollution Control and Treatment Science and Technology Major Project (No.2018ZX07110003)the National Natural Science Foundation of China (No.51779068)。
文摘Refractory organic pollutants in water threaten human health and environmental safety,and advanced oxidation processes (AOPs) are effective for the degradation of these pollutants.Catalysts play vital role in AOPs,and Ce-based catalysts have exhibited excellent performance.Recently,the development and application of Ce-based catalysts in various AOPs have been reported.Our study conducts the first review in this rapid growing field.This paper clarifies the variety and properties of Ce-based catalysts.Their applications in different AOP systems (catalytic ozonation,photodegradation,Fenton-like reactions,sulfate radicalbased AOPs,and catalytic sonochemistry) are discussed.Different Ce-based catalysts suit different reaction systems and produce different active radicals.Finally,future research directions of Ce-based catalysts in AOP systems are suggested.
基金the financial support from the National Natural Science Foundation of China(No. 51878423)Graduate Student’s Research and Innovation Fund of Sichuan University(No.2018YJSY075)
文摘The electrochemical advanced oxidation processes(EAOPs) have been extensively applied in the treatment of organic pollutants degradation.Herein,the mini review provides the coupling systems about EAOPs and different oxidants(e.g.,persulfate(PS),peroxymonosulfate(PMS),and ozone(O3)),including EAOPs-PS systems,EAOPs-PMS systems,EAOPs-peroxone systems,and photoelectro-oxidants systems,for the organic compounds degradation.The coupling system of EAOPs with oxidants is an effective way to improve the generated free radicals(e.g.,HO^·and SO4^·-) concentration and to accelerate pollutant degradation.In this review,we make a summary of the homogeneous and heterogeneous EAOPs-oxidant processes.The reaction mechanisms of EAOPs combined with different oxidants are elucidated in detail,as well as the synergistic effect for improving the degradation and mineralization efficiency.
基金the National Natural Science Foundation of China(Nos.51878325,51868050,51622806,51378246 and 51720105001)the Natural Science Foundation of Jiangxi Province(Nos.20162BCB22017,20165BCB18008,20171ACB20017,20133ACB21001 and 20171BAB206049)the Graduate Innovation Fund of Jiangxi Province(No.YC2018-S360)。
文摘Herein,we prepa red novel three-dimensional(3D)gear-s haped Co3O4@C(Co3O4 modified by amorphous carbon)and sheet-like SnO2/CC(SnO2 grow on the carbon cloth)as anode and cathode to achieve efficient removal of 4-nitrophenol(4-NP)in the presence of peroxymonosulfate(PMS)and simultaneous electrocatalytic reduction of CO2,respectively.In this process,4-NP was mineralized into CO2 by the Co3O4@C,and the generated CO2 was reduced into HCOOH by the sheet-like SnO2/CC cathode.Compared with the pure Co0.5(Co3O4 was prepared using 0.5 g urea)with PMS(30 mg,0.5 g/L),the degradation efficiency of 4-NP(60 mL,10 mg/L)increased from 74.5%-85.1%in 60 min using the Co0.5 modified by amorphous carbon(Co0.5@C).Furthermore,when the voltage of 1.0 V was added in the anodic system of Co0.5@C with PMS(30 mg,0.5 g/L),the degradation efficiency of 4-NP increased from 85.1%-99.1%when Pt was used as cathode.In the experiments of 4-NP degradation coupled with simultaneous electrocatalytic CO2 reduction,the degradation efficiency of 4-NP was 99.0%in the anodic system of Co0.5@C with addition of PMS(30 mg,0.5 g/L),while the Faraday efficiency(FE)of HCOOH was 24.1%at voltage of-1.3 V using the SnO2/CC as cathode.The results showed that the anode of Co3O4 modified by amorphous carbon can markedly improve the degradation efficiency of 4-NP,while the cathode of SnO2/CC can greatly improve the FE and selectivity of CO2 reduction to HCOOH and the stability of cathode.Finally,the promotion mechanism was proposed to explain the degradation of organic pollutants and reduction of CO2 into HCOOH in the process of electrocatalysis coupled with advanced oxidation processes(AOPs)and simultaneous CO2 reduction.
基金supported by the National Natural Science Foundation of China (No. 21007050)the Changjiang Scholars and Innovative Research Team in University (PC-SIRT) (No. IRT0853)the Natural Science Foundation of Shaanxi (No. 2009JQ7001)
文摘Due to the formation of disinfection by-products and high concentrations of Al residue in drinking water purification, humic substances are a major component of organic matter in natural waters and have therefore received a great deal of attention in recent years. We investigated the effects of advanced oxidation pretreatment methods usually applied for removing dissolved organic matters on residual Al control. Results showed that the presence of humic acid increased residual Al concentration notably. With 15 mg/L of humic acid in raw water, the concentrations of soluble aluminum and total aluminum in the treated water were close to the quantity of Al addition. After increasing coagulant dosage from 12 to 120 mg/L, the total-Al in the treated water was controlled to below 0.2 mg/L. Purification systems with ozonation, chlorination, or potassium permanganate oxidation pretreatment units had little effects on residual Al control; while UV radiation decreased Al concentration notably. Combined with ozonation, the effects of UV radiation were enhanced. Optimal dosages were 0.5 mg O 3 /mg C and 3 hr for raw water with 15 mg/L of humic acid. Under UV light radiation, the combined forces or bonds that existed among humic acid molecules were destroyed; adsorption sites increased positively with radiation time, which promoted adsorption of humic acid onto polymeric aluminum and Al（OH） 3 （s）. This work provides a new solution for humic acid coagulation and residual Al control for raw water with humic acid purification.
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...
基金financial support from National Key R&D Program of China (No.2019YFD1100200)National Natural Science Foundation of China (Nos.51878431,51961145106)+2 种基金Shanghai Rising-Star Program (No.20QC1401200)Shanghai Science and Technology Committee (No.19DZ1208400)State Key Laboratory of Pollution Control and Resource Reuse Foundation,(No.PCRRE20002)。
文摘In the field of advanced oxidation processes(AOPs) of wastewater, many materials can be used as heterogeneous catalysts. The role of these catalysts is to activate oxidants and generate reactive oxygen species(ROS) to decompose refractory pollutants. Perovskite oxide, an emerging catalyst in the field of AOPs, has been extensively studied in wastewater treatment. Nevertheless, the application of perovskite in AOP systems still faces some problems, such as leaching of metal ions, a small surface area, a low number of active sites, etc. Herein, this critical review comparatively examines the activation mechanisms of peroxymonosulfate, hydrogen peroxide, and peroxydisulfate. Furthermore, the formation pathways of oxidizing species based on recent advances in experimental and theoretical studies were evaluated. In addition, the impacts of water parameters and constituents such as initial p H, oxidant concentration, catalyst dosage,natural organic matter, halide, phosphate, and carbonate were discussed. Finally, a critical discussion and prospects of mechanism exploration and possible materials development are proposed to confront the existing challenges in the application of perovskite oxides in AOPs.
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)+2 种基金the Heilongjiang Provincial Natural Science Foundation of China(No.LH2020B023)Department of Education Heilongjiang Province(Nos.135309338,135309351)University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(Nos.UNPYSCT-2020068,UNPYSCT-2020067).
文摘Metal-organic frameworks(MOFs)materials with highly ordered and porous crystalline structure,have excellent performance in advanced oxidation progresses(AOPs)for organic contaminants degradation in water treatment.This review intends to summarize the timely references and insights for the recent advances in MOFs that are used in AOPs.Starting with the preparation methodologies,including conventional hydrothermal method,electrochemical method,sol-gel method,and emerging microwave and ultrasound assisted synthesis methods.Application and mechanism for MOFs using in various AOPs of Fenton-like,photocatalysis,catalytic ozonation,persulfate catalysis and other emerging oxidation methods are emphatically discussed.We hope this review can comprehensively summarize the research and application progress of MOFs in AOPs,deepen the understanding of the catalytic mechanisms.
