Ferrate[Fe(Ⅵ)]has demonstrated its efficacy as a potent oxidizing agent in the treatment of wastewater,showcasing its potential for application in environmental remediation.The self-decomposition of Fe(Ⅵ)results in ...Ferrate[Fe(Ⅵ)]has demonstrated its efficacy as a potent oxidizing agent in the treatment of wastewater,showcasing its potential for application in environmental remediation.The self-decomposition of Fe(Ⅵ)results in the formation of Fe(Ⅳ)/Fe(V),which exhibits remarkable reactivity and selectivity towards the degradation of electron-rich micro-pollutants.Here we presented a comprehensive review on the removal of micro-pollutants in Fe(Ⅵ)/carbon materials(CMs)systems,encompassing an analysis of the oxidation mechanism and mutual activation,thereby providing guidance for the efficient elimination of recalcitrant micro-pollutants.The combnation of Fe(Ⅵ)and CMs can significantly enhanced the removal efficiency of various pollutants,with an increase ranges from 30%to 70%.The rate constants for pseudo-first order reactions were increased ranging from 3 to 14 times,while the total organic carbon(TOC)removal rate was effectively doubled.The presence of active species,including hydroxyl radicals,superoxide radical and Fe(Ⅳ)/Fe(V)generated by Fe(Ⅵ)and CMs,can significantly enhance the oxidation efficiency of micro-pollutants which are not easily degraded solely by Fe(Ⅵ)or CMs.Furthermore,Fe(Ⅵ)can enhance the surface area and void volume of CMs,thereby reinforcing the adsorption capacity towards micropollutants.展开更多
N-doped graphite carbon sphere coated cobalt nanoparticle catalyst(Co@C-N-900),prepared by solvothermal-calcination method,is applied to activate peroxymonosulfate(PMS)for bisphenol A(BPA)elimination.The outcomes demo...N-doped graphite carbon sphere coated cobalt nanoparticle catalyst(Co@C-N-900),prepared by solvothermal-calcination method,is applied to activate peroxymonosulfate(PMS)for bisphenol A(BPA)elimination.The outcomes demonstrate that the Co@C-N-900 could effectively activate PMS,thereby causing efficient removal of BPA in water.In addition,the Co@C-N-900/PMS system also has the advantages of low metal leaching,applicability in high salinity environments,good selectivity and stability.Further investigations using electron paramagnetic resonance,chronoamperometry,and quenching experiments demonstrated that the Co@C-N-900/PMS system is a typical non-radical route with singlet oxygen(^(1)O_(2))as the main reactive oxygen species(ROS).Density functional theory calculations(DFT)indicate that N-doping can effectively regulate the charge distribution on the catalyst surface,generating acidic/alkaline sites favorable for PMS adsorption and activation.Furthermore,it also can enhance the interaction and charge transfer capacity between the Co@C-N-900 and PMS.Lastly,LC-QTOF-MS/MS analysis revealed two possible BPA degradation pathways:(1)^(1)O_(2)attacked the isopropyl group in BPA between the two phenyl groups,causingβ-scission to occur.(2)Following the oxidation of the hydroxyl group in the aromatic ring of BPA,^(1)O_(2)could cause furtherβ-scission.The prepared Co@C-N-900 catalyst is a very promising catalyst,which would offer a workable remedy for treating water pollution.展开更多
The contamination of water resources by phenolic compounds(PCs)presents a significant environmental hazard,necessitating the development of novel materials and methodologies for effective mitigation.In this study,a me...The contamination of water resources by phenolic compounds(PCs)presents a significant environmental hazard,necessitating the development of novel materials and methodologies for effective mitigation.In this study,a metallic copper-doped zeolitic imidazolate framework was pyrolyzed and designated as CuNC-20 for the activation of peroxymonosulfate(PMS)to degrade phenol(PE).Cu-NC-20 could effectively address the issue of metal agglomeration while simultaneously diminishing copper dissolution during the activation of PMS reactions.The Cu-NC-20 catalyst exhibited a rapid degradation rate for PE across a broad pH range(3-9)and demonstrated high tolerance towards coexisting ions.According to scavenger experiments and electron paramagnetic resonance analysis,singlet oxygen(^(1)O_(2))and high-valent copperoxo(Cu(Ⅲ))were the predominant reactive oxygen species,indicating that the system was nonradicaldominated during the degradation process.The quantitative structure-activity relationship(QSAR)between the oxidation rate constants of various substituted phenols and Hammett constants was established.It indicated that the Cu-NC-20/PMS system had the optimal oxidation rate constant withσ^(-)correlation and exhibited a typical electrophilic reaction pattern.This study provides a comprehensive understanding of the heterogeneous activation process for the selective removal of phenolic compounds.展开更多
Among various advanced oxidation processes(AOPs),heterogeneous catalytic ozonation has garnered extensive attention in wastewater treatment owing to its broad pH range applicability and the elimination of the need for...Among various advanced oxidation processes(AOPs),heterogeneous catalytic ozonation has garnered extensive attention in wastewater treatment owing to its broad pH range applicability and the elimination of the need for additional energy input.Enhancing catalyst activity by introducing oxygen vacancies has been used extensively in heterogeneous catalytic ozonation.This paper reviews prevalent methods for the construction and characterization of oxygen vacancies.Based on a thorough examination of existing research,the role of oxygen vacancies is categorized according to their primary mechanisms of action in heterogeneous catalytic ozonation.For example,modulation of the catalyst electronic structure to enhance electron transfer;participation in the reaction as an active site to generate radicals and non-radicals;and exposure of more metal sites to enhance the reaction.Lastly,the paper delineates the limitations and future research directions concerning the role of oxygen vacancies in catalytic ozonation.This review addresses the gap in existing literature concerning the role of oxygen vacancies in catalytic ozone systems,establishes a comprehensive theoretical framework to aid in the design of efficient ozone catalysts,and delves into the functionality of oxygen vacancies in heterogeneous catalytic ozone reactions.展开更多
The carbon nanotubes(CNTs) as the emerging materials for organic pollutant removal have gradually become a burgeoning research field.Herein,a mini-review of CNTs-based materials curre ntly studies for organic pollutan...The carbon nanotubes(CNTs) as the emerging materials for organic pollutant removal have gradually become a burgeoning research field.Herein,a mini-review of CNTs-based materials curre ntly studies for organic pollutant elimination is presented.This review summarizes the preparation methods of CNTsbased materials.CNTs-based materials can be used as adsorbents to remove organic pollutants in wastewater.The adsorption mechanisms mainly include surface diffusio n,pore diffusion and adsorption reaction.Most importantly,an in-depth overview of CNTs-based materials currently available in advanced oxidation processes(AOPs) applications for wastewater treatment is proposed.CNTs-based materials can catalyze different oxidants(e.g.,hydrogen peroxide(H2 O2),persulfates(PMS/PDS),ozone(O3) and ferrate/permanganate(Fe(Ⅵ)/Mn(Ⅶ)) to generate more reactive oxygen species(ROS) for organic pollutant elimination.Moreover,the possible reaction mechanisms of removing organic pollutants by CNTs-based materials are summarized systematically and discussed in detail.Finally,application potential and future research directions of CNTs-based materials in the environmental remediation field are proposed.展开更多
Transition metal-based bimetallic oxides can effectively activate peroxymonosulfate(PMS) for the degradation of organic contaminants, which may be attributed to the enhanced electron transfer efficiency between transi...Transition metal-based bimetallic oxides can effectively activate peroxymonosulfate(PMS) for the degradation of organic contaminants, which may be attributed to the enhanced electron transfer efficiency between transition metals. Here, we investigated the high-efficiency catalytic activation reaction of PMS on a well-defined bimetallic Fe-Mn nanocomposite(BFMN) catalyst. The surface topography and chemical information of BFMN were simultaneously mapped with nanoscale resolution. Rhodamine B(Rh B, as a model pollutant) was used to evaluate the oxidation activity of PMS activation system. The maximum absorption peak of Rh B obviously blue shifted from 554 nm to 501 nm, and decreased sharply to disappear completely within 60 min. The removal performance is better than most of the reported single transition metal oxide. X-ray photoelectron spectroscopy(XPS) imaging of the BFMN electronic structure after catalytic activation confirmed that the accelerated internal electron transfer is mainly caused by the synergy effect of Mn and Fe sites at the catalysis boundary. The outstanding ability of BFMN for PMS chemical adsorption and activation may attribute to the enhanced covalency and reactivity of Mn-O. These results of this study can advance understandings on the origins of bimetallic oxides activity for PMS activation and developing the efficient metal oxide catalysts in real practice.展开更多
Studies widely acknowledge the enhancement of permanganate(Mn(Ⅶ))oxidation of organic contaminants by coexisting matrices in water.This study investigated the positive influence of Mn(Ⅱ),a common soluble metal ion,o...Studies widely acknowledge the enhancement of permanganate(Mn(Ⅶ))oxidation of organic contaminants by coexisting matrices in water.This study investigated the positive influence of Mn(Ⅱ),a common soluble metal ion,on the removal of trace organic pollutants by Mn(Ⅶ).Results showed that introducing 20μmol/L Mn(Ⅱ)at pH 5.0 accelerated trace organic pollutant removal by promoting colloidal MnO_(2)formation.UV-vis spectrum,quenching,and probe experiments confirmed role of MnO_(2)in sulfamethoxazole(SMX)oxidation,with Mn(Ⅲ)playing a predominant role.Meanwhile,in situ-generated MnO_(2)facilitated Mn(Ⅶ)*formation,enhancing oxidation performance,as indicated by Raman spectroscopy and electrochemical analysis.Eleven transformation products(TPs)of SMX in the Mn(Ⅶ)/Mn(Ⅱ)process were detected by UPLC-QTOF-MS/MS.Subsequently,the reaction pathways of SMX were elucidated through Fukui index analysis and the identification of TPs.Additionally,toxicity simulations with Toxicity Estimation Software Tool(T.E.S.T.)software revealed significantly lower cytotoxicity of TPs of SMX compared to the parent compound.This study unveils an effective strategy to enhance Mn(Ⅶ)-mediated degradation of organic pollutants in water,elucidating Mn(Ⅱ)-induced Mn(Ⅶ)activation mechanisms.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
To develop more efficient catalysts and discover new materials to work towards efficient solutions to the growing environmental problems,machine learning(ML)offers viable new ideas.Due to its ability to process large-...To develop more efficient catalysts and discover new materials to work towards efficient solutions to the growing environmental problems,machine learning(ML)offers viable new ideas.Due to its ability to process large-scale data and mine underlying patterns,ML has been widely used in the design and development of materials in recent years.The purpose of this manuscript is to summarize the research progress of ML to guide the development of materials in the environmental field and open new horizons for environmental pollution control.This manuscript firstly details the basic ML definitions and operational procedures.Secondly,it summarizes the main ways of applying ML in materials.Then it unfolds to introduce the specific application examples of ML in different materials.Finally,we summarize the shortcomings and research trends of ML in predicting material design.展开更多
Humic acid(HA) as a natural reducing ligand was employed to accelerate the Fenton and Fenton-like processes, however, the potential role of photosensitivity was overlooked. This research showed that HA exhibits more s...Humic acid(HA) as a natural reducing ligand was employed to accelerate the Fenton and Fenton-like processes, however, the potential role of photosensitivity was overlooked. This research showed that HA exhibits more significant promotion for levofloxacin(LVF) degradation under light conditions compared to darkness. The study also proposed a mechanism involving complexation and photosensitization interactions. A strong inhibitor of ethylenediaminetetraacetic acid confirmed that the formation of organic-iron complexes was crucial. Firstly, it was proposed that complexed iron has a lower redox potential than free iron, which may be responsible for accelerating electron transfer from iron to peroxydisulfate(PDS). The density functional theory(DFT) calculations confirmed that complexed iron has a lower reaction energy barrier for PDS activation. Additionally, the excited state substances(^(*)HA and ^(*)LVF) can transfer electrons to Fe(Ⅲ) and PDS, and the generation of HA/LVF-Fe(Ⅲ)-PDS can accelerate this process. These findings could offer fresh perspectives on the combined elimination of contaminants through natural organic compounds and light exposure.展开更多
In this study,batch experiments were conducted to investigate the performance of microscale Fe/Cu bimetallic particles-air-persulfate system(mFe/Cu-air-PS)for p-nitrophenol(PNP)treatment in aqueous solution.First,the ...In this study,batch experiments were conducted to investigate the performance of microscale Fe/Cu bimetallic particles-air-persulfate system(mFe/Cu-air-PS)for p-nitrophenol(PNP)treatment in aqueous solution.First,the optimal operating parameters(i.e.,aeration rate of 1.0 L/min,theoretical Cu mass loading(TMLCu)of 0.110 g Cu/g Fe,mFe/Cu dosage of 15 g/L,PS total dosage of 15 mmol/L,feeding times of PS of 5,initial pH 5.4)were obtained successively by single-factor experiments.Under the optimal conditions,high COD and TOC removal efficiencies(71.0%,65.8%)were obtained after 60 min treatment.Afterword,compared with control experiments(i.e.,mFe/Cu,air,PS,mFe/Cu-air,mFe/Cu–PS,air-PS and mFe-air-PS),mFe/Cu-air-PS system exerted superior performance for pollutants removal due to the synergistic effect between mFe/Cu,air and PS.In addition,the results of control experiments and radical quenching experiments indicate this reinforcement by feeding of PS was greater than by aeration in m Fe/Cu-air-PS system.Furthermore,the degradation intermediates of PNP in mFe/Cu-air-PS process were identified and measured by HPLC.Based on the detected intermediates,the degradation pathways of PNP were proposed comprehensively,which revealed that toxic and refractory PNP in aqueous solution could be decomposed effectively and transformed into lower toxicity intermediates.As a result,m Fe/Cu-air-PS system with the performance of oxidation combined reduction can be also a potential technology for the treatment of toxic and refractory PNP contained wastewater.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
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
Antibiotic re sistance genes(ARGs)in aquatic enviro nments,which seriously endanger human health and ecological safety,have become a worldwide concern due to their easy diffusion and proliferation.Wastewater treatment...Antibiotic re sistance genes(ARGs)in aquatic enviro nments,which seriously endanger human health and ecological safety,have become a worldwide concern due to their easy diffusion and proliferation.Wastewater treatment plants(WWTPs),which receive resistant bacteria and ARGs from a wide variety of sources(i.e.,livestock farms,hospitals,antibiotic manufactures,and households),are regarded as important emission sources of aquatic ARGs.This review presents a quantitative profile of the majority sources of ARGs in the influent of WWTPs and discusses the potential factors that affect the concentration distribution of ARGs.Specifically,a noteworthy existence of ARGs,which ranged from 1 E+05 to 1 E+11 copies/mL,was detected in livestock breeding wastewater,and household wastewater(caused by the unlimited utilization of antibiotics)was determined to be the predominant contributor of ARGs in WWTPs.We summarized the selective pressure on ARGs and determined the positive correlation of the concentration of ARGs and the existence of many containments,including antibiotics,heavy metals(Zn and Cu were frequently reported),quaternary ammonium compounds,etc.In the last section,physical,chemical,and biological treatments for the removal of ARGs and their effluent in WWTPs are discussed and prospective future studies are summarized.展开更多
Acetylene black(AB),as a kind of carbon material with large specific surface area,low density,strong electron transferability,is supposed to have great potential for application in advanced oxidation processes(AOPs).I...Acetylene black(AB),as a kind of carbon material with large specific surface area,low density,strong electron transferability,is supposed to have great potential for application in advanced oxidation processes(AOPs).In this study,AB was utilized as a peroxydisulfate(PDS)activator for the catalytic degradation of sulfamethoxazole(SMX)in aqueous media.Scanning electron microscopy(SEM),X-ray diffraction(XRD),Brunauer-Emmett-Teller(BET)techniques,zeta potential and Raman spectra were employed to characterize the features of AB.To verify the excellent performance of AB/PDS systems,a series of control experiments were carried out.Compared to graphite/PDS and biochar/PDS system,AB/PDS system could complete degradation of SMX within 15 min.Besides,the effects of key factors including AB dosage,PDS dosage,initial pH and SMX concentration on SMX degradation in AB/PDS system were elucidated systematically.Furthermore,through the radical quenching experiments,it was proved that singlet oxygen(1 O_(2))was dominantly responsible for the degradation of SMX.Finally,based on the experiment results and compre hensive analysis,a probable reaction mechanism of AB/PDS system for SMX degradation was proposed.This work suggests that AB has a good potential for tackling the hazardous pollutants in environmental remediation.展开更多
TiO_(2)/graphene oxide(GO)as photocatalyst in the photo-degradation of multitudinous pollutants has been extensively studied.But its low photocatalytic efficiency is attributed to the high band gap energy which lead t...TiO_(2)/graphene oxide(GO)as photocatalyst in the photo-degradation of multitudinous pollutants has been extensively studied.But its low photocatalytic efficiency is attributed to the high band gap energy which lead to low light utilization.Cu-TiO_(2)/GO was synthesized via the impregnation methods to enhance the catalytic performance.The Cu-TiO_(2)/GO reaction rate constant for photo-degradation of pollutants(tetracycline hydrochloride,TC)was about 1.4 times that of TiO_(2)/GO.In 90 min,the removal ratio of Cu-TiO_(2)/GO for TC was 98%,and the maximum degradation ratio occurred at p H 5.After five cycles,the removal ratio of Cu-Ti O_(2)/GO still exceeded 98%.UV-visible adsorption spectra of Cu-Ti O_(2)/GO showed that its band gap was narrower than TiO_(2)/GO.Electron paramagnetic resonance(EPR)spectra test illustrated the generation rate of·O_(2)^(-)and·OH was higher in Cu-TiO_(2)/GO system than TiO_(2)/GO and TiO_(2)system.The contribution sequence of oxidative species was·O_(2)^(-)>holes(h+)>·OH in both TiO_(2)/GO and Cu-Ti O_(2)/GO system.Interestingly,the contribution of·OH in Cu-TiO_(2)/GO was less than that in TiO_(2)/GO during the photo-degradation process.This phenomenon was attributed to the better adsorption performance of Cu-Ti O_(2)/GO which could reduce the accessibility of TC to·OH in liquid.The enhanced non-hydroxyl radical contribution could be attributed to that the more other active species or sites on(nearby)the surface of Cu-TiO_(2)/GO generated after doping Cu.These results provide a new perspective for the tradition metal-doped conventional catalysts to enhance the removal of organic pollutants in the environment.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
In this study,natural mackinawite (Fe S),a chalcophilic mineral,was utilized to prepare iron/copper bimetallic oxides (Cu^(O)@Fe_(x)O_(y)) by displacement plating and calcination process.Various characterization metho...In this study,natural mackinawite (Fe S),a chalcophilic mineral,was utilized to prepare iron/copper bimetallic oxides (Cu^(O)@Fe_(x)O_(y)) by displacement plating and calcination process.Various characterization methods prove that Cu;is successfully coated on the surface of Fe S,which were further oxidized to Cu^(O),Fe_(3)O_(4)and/or Fe_(2)O_(3)during calcination process,respectively.Cu^(O)@Fe_(x)O_(y)performed highly efficient capacity to activate PMS for the degradation of various emerging pollutants including sulfamethoxazole(SMX),carbamazepine (CBZ),bisphenol A (BPA),2,4-dichlorophenol (2,4-DCP) and diclofenac (DCF) in aqueous solution.Complete removal of the above pollutants was observed after 8 min of Cu^(O)@Fe_(x)O_(y)/PMS treatment.Taking SMX as an example,the key parameters including Cu^(O)@Fe_(x)O_(y)dosage,PMS dosage and initial p H were optimized.The results show that the catalytic system can be worked in a wide p H range (3.0-9.0).The quenching experiments and electron spin resonance (ESR) test demonstrated that the main reactive oxygen species in Cu^(O)@Fe_(x)O_(y)/PMS system were hydroxyl radicals (^(·)OH) and sulfate radicals(SO_(4)^(·ˉ)),and SO_(4)^(·ˉ)was the primary reactive species.Besides,the influence of coexisting anions (i.e.,Cl^(ˉ),NO_(3)^(ˉ),HCO_(3)^(ˉ)and H_(2)PO_(4)^(ˉ)) for the degradation of SMX was explored.Cu^(O)@Fe_(x)O_(y)/PMS system can maintain good catalytic activity and reusability in different water bodies and long-term running.This work provided a green strategy to fabricate the efficient catalyst in PMS-based advanced oxidation processes.展开更多
How to utilize inexhaustible solar light as a means of disinfection technology for its cheap and green remains a challenge.In this work,core-shell ZnO@ZIF-8 was synthesized and used for bacterial inactivation synergiz...How to utilize inexhaustible solar light as a means of disinfection technology for its cheap and green remains a challenge.In this work,core-shell ZnO@ZIF-8 was synthesized and used for bacterial inactivation synergizing with peroxymonosulfate(PMS)under visible light irradiation.It took 50 min to achieve thorough sterilization for 7.5-log Escherichia coli(E.coli)cells in vis/PMS/ZnO@ZIF-8 system,compared with that 4.5-log reduction completed in vis/PMS/ZnO system under the same conditions.The enhanced photocatalytic disinfection mechanisms of fabricated ZnO@ZIF-8 were investigated by UV-vis diffuse reflectance spectra,electrochemical impedance spectra and Mott-Schottky plots.The promoted bactericidal efficiency was attributed to higher charge-separation efficiency and stronger oxidation ability of photo-generated holes.Moreover,it was found that^(1)O_(2)and·OH induced bacterial cell lesion process,and the former was the main active species.The external reactive oxygen species(ROS)caused a series of cell wall damage,intercellular ROS up-regulation and genome DNA unwinding,finally resulted in irreversible bacterial death.A two-route mechanism in vis/PMS/ZnO@ZIF-8 system was proposed,in which the generation of^(1)O_(2)was supposed as the product of the oxygen oxidation of photo-generated holes and PMS dissociation.Our work is expected to provide advanced information about a low-cost water disinfection technology of visible light photocatalysis.展开更多
Microscale zero valent iron(mFe^(0))is one of the most potential water pollution remediation materials,but the effective utilization ability of electrons released by mFe^(0)in the reduction of hexavalent chromium(Cr(V...Microscale zero valent iron(mFe^(0))is one of the most potential water pollution remediation materials,but the effective utilization ability of electrons released by mFe^(0)in the reduction of hexavalent chromium(Cr(VI))is not satisfactory.Here,we find the microscale iron-copper(m Fe/Cu)bimetals coated with copper on the surface of mFe^(0)can significantly improve the effective utilization of electrons released by mFe^(0).Electrochemical analysis displays that copper plating on the surface of m Fe/Cu can promote the release the electrons from mFe^(0)and reduce the impedance of mFe^(0).Spin-polarized density functional theory(DFT)calculation reveals that Cu on the surface of m Fe/Cu bimetals promotes the release of electrons from mFe^(0)and reduces the adsorption energy of Fe to Cr.As the electron transporter,moreover,Cu can always attract Cr to the hollow position near itself of the Fe surface,which could promote the effective utilization of electrons released by Fe.Effective utilization ability of electrons in m Fe/Cu system is 12.5 times higher than that in mFe^(0)system.Our findings provide another basis for the efficient reduction of Cr(VI)by m Fe/Cu bimetals,which could promote the application and popularization of m Fe/Cu bimetals.展开更多
基金supported by the National Natural Science Foundation of China(Nos.52170044 and 52070133)。
文摘Ferrate[Fe(Ⅵ)]has demonstrated its efficacy as a potent oxidizing agent in the treatment of wastewater,showcasing its potential for application in environmental remediation.The self-decomposition of Fe(Ⅵ)results in the formation of Fe(Ⅳ)/Fe(V),which exhibits remarkable reactivity and selectivity towards the degradation of electron-rich micro-pollutants.Here we presented a comprehensive review on the removal of micro-pollutants in Fe(Ⅵ)/carbon materials(CMs)systems,encompassing an analysis of the oxidation mechanism and mutual activation,thereby providing guidance for the efficient elimination of recalcitrant micro-pollutants.The combnation of Fe(Ⅵ)and CMs can significantly enhanced the removal efficiency of various pollutants,with an increase ranges from 30%to 70%.The rate constants for pseudo-first order reactions were increased ranging from 3 to 14 times,while the total organic carbon(TOC)removal rate was effectively doubled.The presence of active species,including hydroxyl radicals,superoxide radical and Fe(Ⅳ)/Fe(V)generated by Fe(Ⅵ)and CMs,can significantly enhance the oxidation efficiency of micro-pollutants which are not easily degraded solely by Fe(Ⅵ)or CMs.Furthermore,Fe(Ⅵ)can enhance the surface area and void volume of CMs,thereby reinforcing the adsorption capacity towards micropollutants.
基金the financial support from Sichuan Science and Technology Program(No.2023NSFSC0847)Scientific Research and Innovation Team Program of Sichuan University of Science and Technology(No.SUSE652A003)+3 种基金Talent Introduction Project of Sichuan University of Science and Engineering(No.2021RC03)Talent Introduction Project of Sichuan University of Science and Engineering(No.2021RC05)the Undergraduate Training Program for Innovation and Entrepreneurship(No.CX2024042)The Innovation Fund of Postgraduate,Sichuan University of Science&Engineering(No.Y2024094)。
文摘N-doped graphite carbon sphere coated cobalt nanoparticle catalyst(Co@C-N-900),prepared by solvothermal-calcination method,is applied to activate peroxymonosulfate(PMS)for bisphenol A(BPA)elimination.The outcomes demonstrate that the Co@C-N-900 could effectively activate PMS,thereby causing efficient removal of BPA in water.In addition,the Co@C-N-900/PMS system also has the advantages of low metal leaching,applicability in high salinity environments,good selectivity and stability.Further investigations using electron paramagnetic resonance,chronoamperometry,and quenching experiments demonstrated that the Co@C-N-900/PMS system is a typical non-radical route with singlet oxygen(^(1)O_(2))as the main reactive oxygen species(ROS).Density functional theory calculations(DFT)indicate that N-doping can effectively regulate the charge distribution on the catalyst surface,generating acidic/alkaline sites favorable for PMS adsorption and activation.Furthermore,it also can enhance the interaction and charge transfer capacity between the Co@C-N-900 and PMS.Lastly,LC-QTOF-MS/MS analysis revealed two possible BPA degradation pathways:(1)^(1)O_(2)attacked the isopropyl group in BPA between the two phenyl groups,causingβ-scission to occur.(2)Following the oxidation of the hydroxyl group in the aromatic ring of BPA,^(1)O_(2)could cause furtherβ-scission.The prepared Co@C-N-900 catalyst is a very promising catalyst,which would offer a workable remedy for treating water pollution.
基金the financial support from Sichuan Program of Science and Technology(No.2021ZDZX0012)the National Natural Science Foundation of China(No.52200105)。
文摘The contamination of water resources by phenolic compounds(PCs)presents a significant environmental hazard,necessitating the development of novel materials and methodologies for effective mitigation.In this study,a metallic copper-doped zeolitic imidazolate framework was pyrolyzed and designated as CuNC-20 for the activation of peroxymonosulfate(PMS)to degrade phenol(PE).Cu-NC-20 could effectively address the issue of metal agglomeration while simultaneously diminishing copper dissolution during the activation of PMS reactions.The Cu-NC-20 catalyst exhibited a rapid degradation rate for PE across a broad pH range(3-9)and demonstrated high tolerance towards coexisting ions.According to scavenger experiments and electron paramagnetic resonance analysis,singlet oxygen(^(1)O_(2))and high-valent copperoxo(Cu(Ⅲ))were the predominant reactive oxygen species,indicating that the system was nonradicaldominated during the degradation process.The quantitative structure-activity relationship(QSAR)between the oxidation rate constants of various substituted phenols and Hammett constants was established.It indicated that the Cu-NC-20/PMS system had the optimal oxidation rate constant withσ^(-)correlation and exhibited a typical electrophilic reaction pattern.This study provides a comprehensive understanding of the heterogeneous activation process for the selective removal of phenolic compounds.
基金support from the Key R&D Program of Zhejiang province(No.2024C03136).
文摘Among various advanced oxidation processes(AOPs),heterogeneous catalytic ozonation has garnered extensive attention in wastewater treatment owing to its broad pH range applicability and the elimination of the need for additional energy input.Enhancing catalyst activity by introducing oxygen vacancies has been used extensively in heterogeneous catalytic ozonation.This paper reviews prevalent methods for the construction and characterization of oxygen vacancies.Based on a thorough examination of existing research,the role of oxygen vacancies is categorized according to their primary mechanisms of action in heterogeneous catalytic ozonation.For example,modulation of the catalyst electronic structure to enhance electron transfer;participation in the reaction as an active site to generate radicals and non-radicals;and exposure of more metal sites to enhance the reaction.Lastly,the paper delineates the limitations and future research directions concerning the role of oxygen vacancies in catalytic ozonation.This review addresses the gap in existing literature concerning the role of oxygen vacancies in catalytic ozone systems,establishes a comprehensive theoretical framework to aid in the design of efficient ozone catalysts,and delves into the functionality of oxygen vacancies in heterogeneous catalytic ozone reactions.
基金The authors would like to acknowledge the financial support from the National Natural Science Foundation of China(No.51878423)Fundamental Research Funds for the Central Universities(No.2018SCUH0071)Excellent Youth Foundation of Sichuan Scientific Committee(No.2019JDJQ0005).
文摘The carbon nanotubes(CNTs) as the emerging materials for organic pollutant removal have gradually become a burgeoning research field.Herein,a mini-review of CNTs-based materials curre ntly studies for organic pollutant elimination is presented.This review summarizes the preparation methods of CNTsbased materials.CNTs-based materials can be used as adsorbents to remove organic pollutants in wastewater.The adsorption mechanisms mainly include surface diffusio n,pore diffusion and adsorption reaction.Most importantly,an in-depth overview of CNTs-based materials currently available in advanced oxidation processes(AOPs) applications for wastewater treatment is proposed.CNTs-based materials can catalyze different oxidants(e.g.,hydrogen peroxide(H2 O2),persulfates(PMS/PDS),ozone(O3) and ferrate/permanganate(Fe(Ⅵ)/Mn(Ⅶ)) to generate more reactive oxygen species(ROS) for organic pollutant elimination.Moreover,the possible reaction mechanisms of removing organic pollutants by CNTs-based materials are summarized systematically and discussed in detail.Finally,application potential and future research directions of CNTs-based materials in the environmental remediation field are proposed.
基金supported by the National Key Research and Development Program of China (No. 2020YFC1808300)National Natural Science Foundation of China (Nos. 42077185, 41772264)the Research Fund of State Key Laboratory of Geohazard Prevention and Geoenvironment Protection (No. SKLGP2020Z002)。
文摘Transition metal-based bimetallic oxides can effectively activate peroxymonosulfate(PMS) for the degradation of organic contaminants, which may be attributed to the enhanced electron transfer efficiency between transition metals. Here, we investigated the high-efficiency catalytic activation reaction of PMS on a well-defined bimetallic Fe-Mn nanocomposite(BFMN) catalyst. The surface topography and chemical information of BFMN were simultaneously mapped with nanoscale resolution. Rhodamine B(Rh B, as a model pollutant) was used to evaluate the oxidation activity of PMS activation system. The maximum absorption peak of Rh B obviously blue shifted from 554 nm to 501 nm, and decreased sharply to disappear completely within 60 min. The removal performance is better than most of the reported single transition metal oxide. X-ray photoelectron spectroscopy(XPS) imaging of the BFMN electronic structure after catalytic activation confirmed that the accelerated internal electron transfer is mainly caused by the synergy effect of Mn and Fe sites at the catalysis boundary. The outstanding ability of BFMN for PMS chemical adsorption and activation may attribute to the enhanced covalency and reactivity of Mn-O. These results of this study can advance understandings on the origins of bimetallic oxides activity for PMS activation and developing the efficient metal oxide catalysts in real practice.
基金support from the National Natural Science Foundation of China(Nos.52300102,523B2094)the Key Laboratory of Jiangxi Province for Persistent Pollutants Prevention Control and Resource Reuse(No.2023SSY02061)+1 种基金the Natural Science Foundation of Sichuan Province(No.2024NSFSC0130)Miaozi Project in Science and Technology Innovation Program of Sichuan Province(No.MZGC20230098)。
文摘Studies widely acknowledge the enhancement of permanganate(Mn(Ⅶ))oxidation of organic contaminants by coexisting matrices in water.This study investigated the positive influence of Mn(Ⅱ),a common soluble metal ion,on the removal of trace organic pollutants by Mn(Ⅶ).Results showed that introducing 20μmol/L Mn(Ⅱ)at pH 5.0 accelerated trace organic pollutant removal by promoting colloidal MnO_(2)formation.UV-vis spectrum,quenching,and probe experiments confirmed role of MnO_(2)in sulfamethoxazole(SMX)oxidation,with Mn(Ⅲ)playing a predominant role.Meanwhile,in situ-generated MnO_(2)facilitated Mn(Ⅶ)*formation,enhancing oxidation performance,as indicated by Raman spectroscopy and electrochemical analysis.Eleven transformation products(TPs)of SMX in the Mn(Ⅶ)/Mn(Ⅱ)process were detected by UPLC-QTOF-MS/MS.Subsequently,the reaction pathways of SMX were elucidated through Fukui index analysis and the identification of TPs.Additionally,toxicity simulations with Toxicity Estimation Software Tool(T.E.S.T.)software revealed significantly lower cytotoxicity of TPs of SMX compared to the parent compound.This study unveils an effective strategy to enhance Mn(Ⅶ)-mediated degradation of organic pollutants in water,elucidating Mn(Ⅱ)-induced Mn(Ⅶ)activation mechanisms.
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the National Natural Science Foundation of China(Nos.52370083 and 52170088)Sichuan Science and Technology Program(No.2024NSFTD0014)Key R&D Program of Heilongjiang Province(No.2023ZX02C01)for financial support。
文摘To develop more efficient catalysts and discover new materials to work towards efficient solutions to the growing environmental problems,machine learning(ML)offers viable new ideas.Due to its ability to process large-scale data and mine underlying patterns,ML has been widely used in the design and development of materials in recent years.The purpose of this manuscript is to summarize the research progress of ML to guide the development of materials in the environmental field and open new horizons for environmental pollution control.This manuscript firstly details the basic ML definitions and operational procedures.Secondly,it summarizes the main ways of applying ML in materials.Then it unfolds to introduce the specific application examples of ML in different materials.Finally,we summarize the shortcomings and research trends of ML in predicting material design.
基金supported by the Natural Science Foundation of China (No. 42107073)Central Guidance for Local Science and Technology Development Fund Projects (No. 2024ZYD0030)+1 种基金Natural Science Foundation of Sichuan Province (No. 2024NSFSC0130)the Sichuan Science and Technology Program (No. 2024NSFTD0014)。
文摘Humic acid(HA) as a natural reducing ligand was employed to accelerate the Fenton and Fenton-like processes, however, the potential role of photosensitivity was overlooked. This research showed that HA exhibits more significant promotion for levofloxacin(LVF) degradation under light conditions compared to darkness. The study also proposed a mechanism involving complexation and photosensitization interactions. A strong inhibitor of ethylenediaminetetraacetic acid confirmed that the formation of organic-iron complexes was crucial. Firstly, it was proposed that complexed iron has a lower redox potential than free iron, which may be responsible for accelerating electron transfer from iron to peroxydisulfate(PDS). The density functional theory(DFT) calculations confirmed that complexed iron has a lower reaction energy barrier for PDS activation. Additionally, the excited state substances(^(*)HA and ^(*)LVF) can transfer electrons to Fe(Ⅲ) and PDS, and the generation of HA/LVF-Fe(Ⅲ)-PDS can accelerate this process. These findings could offer fresh perspectives on the combined elimination of contaminants through natural organic compounds and light exposure.
基金the financial support from the National Natural Science Foundation of China(No.51878423)China Postdoctoral Science Foundation(No.2018M631077)
文摘In this study,batch experiments were conducted to investigate the performance of microscale Fe/Cu bimetallic particles-air-persulfate system(mFe/Cu-air-PS)for p-nitrophenol(PNP)treatment in aqueous solution.First,the optimal operating parameters(i.e.,aeration rate of 1.0 L/min,theoretical Cu mass loading(TMLCu)of 0.110 g Cu/g Fe,mFe/Cu dosage of 15 g/L,PS total dosage of 15 mmol/L,feeding times of PS of 5,initial pH 5.4)were obtained successively by single-factor experiments.Under the optimal conditions,high COD and TOC removal efficiencies(71.0%,65.8%)were obtained after 60 min treatment.Afterword,compared with control experiments(i.e.,mFe/Cu,air,PS,mFe/Cu-air,mFe/Cu–PS,air-PS and mFe-air-PS),mFe/Cu-air-PS system exerted superior performance for pollutants removal due to the synergistic effect between mFe/Cu,air and PS.In addition,the results of control experiments and radical quenching experiments indicate this reinforcement by feeding of PS was greater than by aeration in m Fe/Cu-air-PS system.Furthermore,the degradation intermediates of PNP in mFe/Cu-air-PS process were identified and measured by HPLC.Based on the detected intermediates,the degradation pathways of PNP were proposed comprehensively,which revealed that toxic and refractory PNP in aqueous solution could be decomposed effectively and transformed into lower toxicity intermediates.As a result,m Fe/Cu-air-PS system with the performance of oxidation combined reduction can be also a potential technology for the treatment of toxic and refractory PNP contained wastewater.
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(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HIT Environment and Ecology Innovation Special Funds(No.HSCJ201611)The funding from the National Nature Science Foundation of China(No.51878213)the funding by State Key Laboratory of Urban Water Resource and Environment(No.2020TS01)。
文摘Antibiotic re sistance genes(ARGs)in aquatic enviro nments,which seriously endanger human health and ecological safety,have become a worldwide concern due to their easy diffusion and proliferation.Wastewater treatment plants(WWTPs),which receive resistant bacteria and ARGs from a wide variety of sources(i.e.,livestock farms,hospitals,antibiotic manufactures,and households),are regarded as important emission sources of aquatic ARGs.This review presents a quantitative profile of the majority sources of ARGs in the influent of WWTPs and discusses the potential factors that affect the concentration distribution of ARGs.Specifically,a noteworthy existence of ARGs,which ranged from 1 E+05 to 1 E+11 copies/mL,was detected in livestock breeding wastewater,and household wastewater(caused by the unlimited utilization of antibiotics)was determined to be the predominant contributor of ARGs in WWTPs.We summarized the selective pressure on ARGs and determined the positive correlation of the concentration of ARGs and the existence of many containments,including antibiotics,heavy metals(Zn and Cu were frequently reported),quaternary ammonium compounds,etc.In the last section,physical,chemical,and biological treatments for the removal of ARGs and their effluent in WWTPs are discussed and prospective future studies are summarized.
基金the financial support from National Natural Science Foundation of China(No.51878423)Sichuan Science and Technology ProgramKey Research and Development Program(Nos.2019YFG0314,2017SZ0180,2019YFG0324)the Major Scientific and Technological Special Program of Sichuan Province,China(2018SZDZX0027)。
文摘Acetylene black(AB),as a kind of carbon material with large specific surface area,low density,strong electron transferability,is supposed to have great potential for application in advanced oxidation processes(AOPs).In this study,AB was utilized as a peroxydisulfate(PDS)activator for the catalytic degradation of sulfamethoxazole(SMX)in aqueous media.Scanning electron microscopy(SEM),X-ray diffraction(XRD),Brunauer-Emmett-Teller(BET)techniques,zeta potential and Raman spectra were employed to characterize the features of AB.To verify the excellent performance of AB/PDS systems,a series of control experiments were carried out.Compared to graphite/PDS and biochar/PDS system,AB/PDS system could complete degradation of SMX within 15 min.Besides,the effects of key factors including AB dosage,PDS dosage,initial pH and SMX concentration on SMX degradation in AB/PDS system were elucidated systematically.Furthermore,through the radical quenching experiments,it was proved that singlet oxygen(1 O_(2))was dominantly responsible for the degradation of SMX.Finally,based on the experiment results and compre hensive analysis,a probable reaction mechanism of AB/PDS system for SMX degradation was proposed.This work suggests that AB has a good potential for tackling the hazardous pollutants in environmental remediation.
基金the National Natural Science Foundation of China(No.41772264)the Applied Basic Research Programs of Science and Technology Foundation of Sichuan Province(No.18YYJC1745)the Research Fund of State Key Laboratory of Geohazard Prevention and Geoenvironment Protection(No.SKLGP2018Z001)。
文摘TiO_(2)/graphene oxide(GO)as photocatalyst in the photo-degradation of multitudinous pollutants has been extensively studied.But its low photocatalytic efficiency is attributed to the high band gap energy which lead to low light utilization.Cu-TiO_(2)/GO was synthesized via the impregnation methods to enhance the catalytic performance.The Cu-TiO_(2)/GO reaction rate constant for photo-degradation of pollutants(tetracycline hydrochloride,TC)was about 1.4 times that of TiO_(2)/GO.In 90 min,the removal ratio of Cu-TiO_(2)/GO for TC was 98%,and the maximum degradation ratio occurred at p H 5.After five cycles,the removal ratio of Cu-Ti O_(2)/GO still exceeded 98%.UV-visible adsorption spectra of Cu-Ti O_(2)/GO showed that its band gap was narrower than TiO_(2)/GO.Electron paramagnetic resonance(EPR)spectra test illustrated the generation rate of·O_(2)^(-)and·OH was higher in Cu-TiO_(2)/GO system than TiO_(2)/GO and TiO_(2)system.The contribution sequence of oxidative species was·O_(2)^(-)>holes(h+)>·OH in both TiO_(2)/GO and Cu-Ti O_(2)/GO system.Interestingly,the contribution of·OH in Cu-TiO_(2)/GO was less than that in TiO_(2)/GO during the photo-degradation process.This phenomenon was attributed to the better adsorption performance of Cu-Ti O_(2)/GO which could reduce the accessibility of TC to·OH in liquid.The enhanced non-hydroxyl radical contribution could be attributed to that the more other active species or sites on(nearby)the surface of Cu-TiO_(2)/GO generated after doping Cu.These results provide a new perspective for the tradition metal-doped conventional catalysts to enhance the removal of organic pollutants in the environment.
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financial support from National Natural Science Foundation of China (No.51878423)China Postdoctoral Science Foundation (No.2019T120843)Sichuan Science and Technology Program (No.2019YJ0091)。
文摘In this study,natural mackinawite (Fe S),a chalcophilic mineral,was utilized to prepare iron/copper bimetallic oxides (Cu^(O)@Fe_(x)O_(y)) by displacement plating and calcination process.Various characterization methods prove that Cu;is successfully coated on the surface of Fe S,which were further oxidized to Cu^(O),Fe_(3)O_(4)and/or Fe_(2)O_(3)during calcination process,respectively.Cu^(O)@Fe_(x)O_(y)performed highly efficient capacity to activate PMS for the degradation of various emerging pollutants including sulfamethoxazole(SMX),carbamazepine (CBZ),bisphenol A (BPA),2,4-dichlorophenol (2,4-DCP) and diclofenac (DCF) in aqueous solution.Complete removal of the above pollutants was observed after 8 min of Cu^(O)@Fe_(x)O_(y)/PMS treatment.Taking SMX as an example,the key parameters including Cu^(O)@Fe_(x)O_(y)dosage,PMS dosage and initial p H were optimized.The results show that the catalytic system can be worked in a wide p H range (3.0-9.0).The quenching experiments and electron spin resonance (ESR) test demonstrated that the main reactive oxygen species in Cu^(O)@Fe_(x)O_(y)/PMS system were hydroxyl radicals (^(·)OH) and sulfate radicals(SO_(4)^(·ˉ)),and SO_(4)^(·ˉ)was the primary reactive species.Besides,the influence of coexisting anions (i.e.,Cl^(ˉ),NO_(3)^(ˉ),HCO_(3)^(ˉ)and H_(2)PO_(4)^(ˉ)) for the degradation of SMX was explored.Cu^(O)@Fe_(x)O_(y)/PMS system can maintain good catalytic activity and reusability in different water bodies and long-term running.This work provided a green strategy to fabricate the efficient catalyst in PMS-based advanced oxidation processes.
基金the financial support from National Natural Science Foundation of China(No.52070133)Sichuan Science and Technology Program:Key Research and Development Program(Nos.2019YFG0314,2017SZ0180,2019YFG0324)。
文摘How to utilize inexhaustible solar light as a means of disinfection technology for its cheap and green remains a challenge.In this work,core-shell ZnO@ZIF-8 was synthesized and used for bacterial inactivation synergizing with peroxymonosulfate(PMS)under visible light irradiation.It took 50 min to achieve thorough sterilization for 7.5-log Escherichia coli(E.coli)cells in vis/PMS/ZnO@ZIF-8 system,compared with that 4.5-log reduction completed in vis/PMS/ZnO system under the same conditions.The enhanced photocatalytic disinfection mechanisms of fabricated ZnO@ZIF-8 were investigated by UV-vis diffuse reflectance spectra,electrochemical impedance spectra and Mott-Schottky plots.The promoted bactericidal efficiency was attributed to higher charge-separation efficiency and stronger oxidation ability of photo-generated holes.Moreover,it was found that^(1)O_(2)and·OH induced bacterial cell lesion process,and the former was the main active species.The external reactive oxygen species(ROS)caused a series of cell wall damage,intercellular ROS up-regulation and genome DNA unwinding,finally resulted in irreversible bacterial death.A two-route mechanism in vis/PMS/ZnO@ZIF-8 system was proposed,in which the generation of^(1)O_(2)was supposed as the product of the oxygen oxidation of photo-generated holes and PMS dissociation.Our work is expected to provide advanced information about a low-cost water disinfection technology of visible light photocatalysis.
基金the financial support from Fundamental Research Funds for the Central Universities(Southwest Minzu University,No.U2021124)the Startup Foundation of Chengdu University of Information Technology(No.KYTZ202013)+1 种基金National Natural Science Foundation of China(No.21808146)China Postdoctoral Science Foundation(No.2018M643479)。
文摘Microscale zero valent iron(mFe^(0))is one of the most potential water pollution remediation materials,but the effective utilization ability of electrons released by mFe^(0)in the reduction of hexavalent chromium(Cr(VI))is not satisfactory.Here,we find the microscale iron-copper(m Fe/Cu)bimetals coated with copper on the surface of mFe^(0)can significantly improve the effective utilization of electrons released by mFe^(0).Electrochemical analysis displays that copper plating on the surface of m Fe/Cu can promote the release the electrons from mFe^(0)and reduce the impedance of mFe^(0).Spin-polarized density functional theory(DFT)calculation reveals that Cu on the surface of m Fe/Cu bimetals promotes the release of electrons from mFe^(0)and reduces the adsorption energy of Fe to Cr.As the electron transporter,moreover,Cu can always attract Cr to the hollow position near itself of the Fe surface,which could promote the effective utilization of electrons released by Fe.Effective utilization ability of electrons in m Fe/Cu system is 12.5 times higher than that in mFe^(0)system.Our findings provide another basis for the efficient reduction of Cr(VI)by m Fe/Cu bimetals,which could promote the application and popularization of m Fe/Cu bimetals.
