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Highly efficient degradation of emerging contaminants by magnetic CuO@Fe_(x)O_(y) derived from natural mackinawite(FeS) in the presence of peroxymonosulfate

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Chinese Chemical Letters 2022年第2期33卷 948-952页

作者： Ruohan Zhang Maolian Chen Zhaokun Xiong Yong Guo Bo Lai State Key Laboratory of Hydraulics and Mountain River Engineering College of Architecture and EnvironmentSichuan University-Pittsburgh InstituteSichuan UniversityChengdu 610207China Department of Process Equipment and Safety Engineering School of Chemical EngineeringSichuan UniversityChengdu 610065China Sino-German Centre for Water and Health Research Sichuan UniversityChengdu 610065China

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.

关键词： Emerging organic contaminants Mackinawite Peroxymonosulfate CuO@Fe_(x)O_(y) Reactive oxygen species

The electrochemical advanced oxidation processes coupling of oxidants for organic pollutants degradation: A mini-review

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Chinese Chemical Letters 2019年第12期30卷 2139-2146页

作者： Jun Li Yangju Li Zhaokun Xiong Gang Yao Bo Lai State Key Laboratory of Hydraulics and Mountain River Engineering College of Architecture and EnvironmentSichuan UniversityChengdu 610065China Sino-German Centre for Water and Health Research Sichuan UniversityChengdu 610065China Institute of Environmental Engineering RWTH Aachen UniversityAachen 52072Germany

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.

关键词： Electrochemical advanced oxidation processes Organic compounds Oxidants Free radicals Reaction mechanism

Degradation of p-nitrophenol(PNP) in aqueous solution by mFe/Cu-air-PS system

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Chinese Chemical Letters 2019年第5期30卷 1129-1132页

作者： Heng Zhang Qingqing Ji Leiduo Lai Gang Yao Bo Lai State Key Laboratory of Hydraulics and Mountain River Engineering College of Architecture and EnvironmentSichuan UniversityChengdu 610065China Sino-German Centre for Water and Health Research Sichuan UniversityChengdu 610065China Institute of Environmental Engineering RWTH Aachen UniversityAachenGermany

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.

关键词： p-Nitrophenol(PNP) Microscale Fe/Cu bimetallic particles(mFe/Cu) Persulfate(PS) Air aeration mFe/Cu-air-PS system

Efficient degradation of sulfamethoxazole by acetylene black activated peroxydisulfate

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Chinese Chemical Letters 2020年第10期31卷 2657-2660页

作者： Silang Nimai Heng Zhang Zelin Wu Naiwen Li Bo Lai State Key Laboratory of Hydraulics and Mountain River Engineering College of Architecture and EnvironmentSichuan UniversityChengdu 610065China College of Hydraulic and Hydroelectric Engineering Sichuan UniversityChengdu 610065China Sino-German Centre for Water and Health Research Sichuan UniversityChengdu 610065China

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.

关键词： Sulfamethoxazole(SMX) Acetylene black(AB) Peroxydisulfate(PDS) Reaction mechanism

Effective E.coli inactivation of core-shell ZnO@ZIF-8 photocatalysis under visible light synergize with peroxymonosulfate:Efficiency and mechanism

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Chinese Chemical Letters 2022年第1期33卷 415-423页

作者： Yanni Jiang Zhaokun Xiong Jianbo Huang Feng Yan Gang Yao Bo Lai State Key Laboratory of Hydraulics and Mountain River Engineering College of Architecture and EnvironmentSichuan UniversityChengdu 610065China Sino-German Centre for Water and Health Research Sichuan UniversityChengdu 610065China Department of Ultrasound Laboratory of Ultrasound Imaging DrugWest China HospitalSichuan UniversityChengdu 610041China Institute of Environmental Engineering RWTH Aachen UniversityAachen 52072Germany

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.

关键词： Bacterial inactivation Photocatalysis Visible light Peroxymonosulfate

Review of advanced oxidation processes for treating hospital sewage to achieve decontamination and disinfection

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Chinese Chemical Letters 2024年第1期35卷 140-152页

作者： Si-Ying Yu Zhi-Hui Xie Xiaoyu Wu Yun-Zhe Zheng Yang Shi Zhao-Kun Xiong Peng Zhou Yang Liu Chuan-Shu He Zhi-Cheng Pan Kai-Jun Wang Bo Lai State Key Laboratory of Hydraulics and Mountain River Engineering College of Architecture and EnvironmentSichuan UniversityChengdu 610065China Sino-German Centre for Water and Health Research Sichuan UniversityChengdu 610065China State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China water Safety and water Pollution Control Engineering Technology research Center in Sichuan Province Haitian Water GroupChengdu 610041China

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.

关键词： Hospital sewage treatment Advanced oxidation processes Pharmaceutical contaminants Disinfection Decontamination

Metagenomic analysis to determine the characteristics of antibiotic resistance genes in typical antibiotic-contaminated sediments

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Journal of Environmental Sciences 2023年第6期128卷 12-25页

作者： Han Yang Mu Xu Liqing Wang Xianyun Wang Erik Jeppesen Wei Zhang Engineering research Center of Environmental DNA and Ecological water health Assessment Centre for Research on Environmental Ecology and Fish Nutrient of the Ministry of AgricultureShanghai Ocean UniversityShanghai 201306China Shanghai National Engineering research Center for Urban water Resources Co. Ltd.Shanghai 200082China Department of Ecoscience Aarhus UniversityC.F.MФlers Allé38000 Aarhus CDenmark sino-Danish centre for Education and research(SDC) University of Chinese Academy of SciencesBeijing 100190China Limnology Laboratory Department of Biological Sciences and Centre for Ecosystem Research and ImplementationMiddle East Technical UniversityAnkara 06800Turkey Institute of Marine Sciences Middle East Technical University33731 MersinTurkey

Comprehensive studies of the effects of various physical and chemical variables(including heavymetals),antibiotics,and microorganisms in the environment on antibiotic resistance genes are rare.We collected sediment samples from the Shatian Lake aquaculture area and surrounding lakes and rivers located in Shanghai,China.The spatial distribution of sediment ARGs was assessed by metagenomic analysis that revealed 26 ARG types(510 subtypes),dominated by Multidrug,β-lactam,Aminoglycoside,Glycopeptides,Fluoroquinolone,and Tetracyline.Redundancy discriminant analysis indicated that antibiotics(SAs and MLs)in the aqueous environment and sediment along with water TN and TP were the key variables affecting the abundance distribution of total ARGs.However,the main environmental drivers and key influences differed among the different ARGs.For total ARGs,the environmental subtypes affecting their structural composition and distribution characteristics were mainly antibiotic residues.Procrustes analysis showed a significant correlation between ARGs and microbial communities in the sediment in the survey area.Network analysis revealed that most of the target ARGs were significantly and positively correlated with microorganisms,and a small number of ARGs(e.g.,rpoB,mdtC,and efpA)were highly significantly and positively correlated with microorganisms(e.g.,Knoellia,Tetrasphaera,and Gem-matirosa).Potential hosts for the major ARGs included Actinobacteria,Proteobacteria,and Gemmatimonadetes.Our study provides new insight and a comprehensive assessment of the distribution and abundance of ARGs and the drivers of ARG occurrence and transmission.

关键词： Metagenomic analysis Antibiotic resistance genes Environmental drivers Sediments Shatian Lake

Manganese oxide and derivative-modified materials in advanced oxidation processes:A review of modification enhancement and activation mechanisms

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Chinese Chemical Letters 2024年第3期35卷 40-51页

作者： Si Sun Shuang Song Shuai Yang Yong-Li He Yang Shi Peng Zhou Zhao-kun Xiong Yang Liu Heng Zhang Ye Du Chuan-Shu He Bo Lai State Key Laboratory of Hydraulics and Mountain River Engineering College of Architecture and EnvironmentSichuan UniversityChengdu 610065China Sino-German Centre for Water and Health Research Sichuan UniversityChengdu 610065China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaSichuanChengdu 610054China

Manganese oxides(MNO_(x)),as low-toxicity and high-abundance catalysts,have been demonstrated to hold great promise for application in advanced oxidation processes(AOPs).However,further application of this material is restricted due to its unsatisfactory oxidant activation efficiency.Fortunately,recently remarkable research on deep activation mechanisms and modification of MNO_(x)have been undertaken to improve its reactivity.Herein,modification enhancement mechanisms of MNO_(x)to efficiently degrade various organic contaminants were discussed and highlighted,including metal doping,coupling with other metal oxides,composite with carbonaceous material,and compounding with other support.The activation mechanisms of different MNO_(x)and derivative-modified material(such as doped MNO_(x),metal oxide-MNO_(x)hybrids,and MNO_(x)-carbonaceous material hybrids)were summarized in great details,which was specifically categorized into both radical and non-radical pathways.The effects of pH,inorganic ions,and natural organic matter on degradation reactions are also discussed.Finally,future research directions and perspectives are presented to provide a clear interpretation on the MNO_(x)initiated AOPs.

关键词： Manganese oxide Derivative-modified materials Modification enhancement mechanisms Advanced oxidation process Activation mechanism

Activation of peroxymonosulfate by FeVO_(3-x)for the degradation of carbamazepine:Vanadium mediated electron shuttle and oxygen vacancy modulated interface chemistry

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Chinese Chemical Letters 2024年第1期35卷 435-440页

作者： Leiduo Lai Hongyu Zhou Yichen Hong Mengfan Luo Yang Shi Heng Zhang Zhaokun Xiong Gang Yao Bo Lai State Key Laboratory of Hydraulics and Mountain River Engineering College of Architecture and EnvironmentSichuan UniversityChengdu 610065China Sino-German Centre for Water and Health Research Sichuan UniversityChengdu 610065China Chengdu Baixi Environmental Technology Company Chengdu 610065China d Institute of Environmental Engineering RWTH Aachen UniversityGermany

Fast Fe(III)/Fe(II)circulation in heterogeneous peroxymonosulfate(PMS)activation remains as a bottleneck issue that restricts the development of PMS based advanced oxidation processes.Herein,we proposed a facile ammonia reduction strategy and synthesized a novel FeVO3-x catalysts to activate PMS for the degradation of a typical pharmaceutical,carbamazepine(CBZ).Rapid CBZ removal could be achieved within 10 min,which outperforms most of the other iron or vanadium-based catalysts.Electron paramagnetic resonance analysis and chemical probe experiments revealed SO_(4)^(·-),·OH,O_(2)^(·-)and high valent iron(Fe(IV))were all generated in this system,but SO4·-and Fe(IV)primarily contributed to the degradation of CBZ.Besides,X-ray photoelectron spectroscopy and X-ray adsorption spectroscopy indicated that both the generated low-valent V provides and oxygen vacancy acted as superior electron donors and accelerated internal electron transfer via the unsaturated V-O-Fe bond.Finally,the proposed system also exhibited satisfactory performance in practical applications.This work provides a promising platform in heterogeneous PMS activation.

关键词： Peroxymonosulfate Fe(III) Fe(II)cycle Electron shuttles Oxygen vacancy Bimetallic catalysts