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Oxidation of emerging organic contaminants by in-situ H_(2)O_(2) fenton system

Green Energy & Environment 2024年第3期9卷 417-434页

作者： Yuqin Ni Chuxiang Zhou Mingyang Xing Yi Zhou State Environmental Protection Key Lab of Environmental Risk Assessment and Control on Chemical Processes School of Resources&Environmental EngineeringEast China University of Science and TechnologyShanghai200237China Key Laboratory for Advanced Materials and Institute of Fine Chemicals National Engineering Laboratory for Industrial Wastewater TreatmentSchool of Chemistry and Molecular EngineeringEast China University of Science and Technology130 Meilong RoadShanghai200237China Department of Applied Natural Sciences Technische Hochschule LubeckMonkhofer Weg 23923562 LubeckGermany

The existence and risk of emerging organic contaminants(EOCs)have been under consideration and paid much effort to degrade these pollutants.Fenton system is one of the most widely used technologies to solve this problem.The original Fenton system relies on the hydroxyl radicals produced by Fe(Ⅱ)/H_(2)O_(2) to oxidize the organic contaminants.However,the application of the Fenton system is limited by its low iron cycling efficiency and the high risks of hydrogen peroxide transportation and storage.The introduction of external energy(including light and electricity etc.)can effectively promote the Fe(Ⅲ)/Fe(Ⅱ)cycle and the reduction of oxygen to produce hydrogen peroxide in situ.This review introduces three in-situ Fenton systems,which are electro-Fenton,Photo-Fenton,and chemical reaction.The mechanism,influencing factors,and catalysts of these three in-situ Fenton systems in degrading EOCs are discussed systematically.This review strengthens the understanding of Fenton and in-situ Fenton systems in degradation,offering further insight into the real application of the in-situ Fenton system in the removal of EOCs.

关键词： In-situ H_(2)O_(2)production Fenton emerging organic contaminants Photocatalysis Electrocatalysis

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emerging organic contaminants in Chinese Surface Water:Identification of Priority Pollutants

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Engineering 2022年第4期8卷 111-125页

作者： Mengmeng Zhong Tielong Wang Wenxing Zhao Jun Huang Bin Wang Lee Blaney Qingwei Bu Gang Yu Beijing Key Laboratory for emerging organic contaminants Control State Key Joint Laboratory of Environment Simulation and Pollution Control(SKLESPC)School of EnvironmentTsinghua UniversityBeijing 100084China Department of Chemical Biochemicaland Environmental EngineeringUniversity of Maryland Baltimore CountyBaltimoreMD 21250USA School of Chemical and Environmental Engineering China University of Mining and Technology-BeijingBeijing 100083China

The occurrence and impacts of emerging organic contaminants(EOCs)in the aquatic environment have gained widespread attention over the past two decades.Due to large number of potential contaminants,monitoring campaigns,treatment plants,and proposed regulations should preferentially focus on specific pollutants with the highest potential for ecological and human health effects.In the present study,a multi-criteria screening approach based on hazard and exposure potentials was developed for prioritization of 405 unregulated EOCs already present in Chinese surface water.Hazard potential,exposure potential,and risk quotients for ecological and human health effects were quantitatively analyzed and used to screen contaminants.The hazard potential was defined by contaminant persistence,bioaccumulation,ecotoxicity,and human health effects;similarly,the exposure potential was a function of contaminant concentration and detection frequency.In total,123 compounds passed the preselection process,which involved a priority index equal to the normalized hazard potential multiplied by the normalized exposure potential.Based on the prioritization scheme,11 compounds were identified as top-priority,and 37 chemicals were defined as high-priority.The results obtained by the priority index were compared with four other prioritization schemes based on exposure potential,hazard potential,or risk quotients for ecological effects or human health.The priority index effectively captured and integrated the results from the more simplistic prioritization schemes.Based on identified data gaps,four uncertainty categories were classified to recommend:①regular monitoring,derivation of environmental quality standards,and development of control strategies;②increased monitoring;③fortified hazard assessment;and④increased efforts to collect occurrence and toxicity data.Overall,20 pollutants were recommended as priority EOCs.The prioritized list of contaminants provides the necessary information for authoritative regulations to monitor,control,evaluate

关键词： Prioritization emerging organic contaminants Hazard potential Ecotoxicity Risk assessment

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Engineering carbon nanocatalysts towards efficient degradation of emerging organic contaminants via persulfate activation:A review

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Chinese Chemical Letters 2022年第1期33卷 1-10页

作者： Dongli Guo Shijie You Fang Li Yanbiao Liu State Key Laboratory of Urban Water Resource and Environment School of EnvironmentHarbin Institute of TechnologyHarbin 150090China Textile Pollution Controlling Engineering Center of Ministry of Environmental Protection College of Environmental Science and EngineeringDonghua UniversityShanghai 201620China

The engineering of carbon nanocatalysts for the persulfate activated elimination of emerging organic contaminants(EOCs)demonstrates promising potential compared with metal-based counterparts due to their unique advantage of high stability and low toxicity.The early reviews introduced the theoretical background of persulfate activation together with a detailed summary of different mechanisms responsible for degradation of EOCs.To further unify the state of knowledge,identify the research gaps,and prompt new research in this area,we present a thorough review on current trends in research on metal-free carbon nanocatalysts(e.g.,0D nanodiamond,1D carbon nanotubes and carbon nanofibers,2D graphene and graphitic carbon nitride,and 3D carbon nanocatalysts),with emphasis on their applications in persulfate activation and EOCs decontamination.We also discuss the current challenges and future perspectives in practically relevant applications.Last,we highlight that the development of sustainable carbon nanocatalysts/persulfate systems lies at the interface of multiple disciplines,which calls for future in-depth interdisciplinary collaborations.

关键词： Carbon nanocatalysts Persulfate activation Advanced oxidation processes emerging organic contaminants Water purification

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Construction of MoFs-based nanocomposite membranes for emerging organic contaminants abatement in water

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Frontiers of Environmental Science & Engineering 2023年第7期17卷 151-174页

作者： Yuxin Lu Xiang Li Cagnetta Giovanni Bo Wang Advanced Research Institute of Multidisciplinary Science School of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China School of Environment Tsinghua UniversityBeijing 100084China

Presence of emerging organic contaminants(EOCs)in water is one of the major threats to water safety.In recent decades,an increasing number of studies have investigated new approaches for their effective removal.Among them,metal-organic frameworks(MOFs)have_attracted increasing attention since their first development thanks to their tunable metal nodes and versatile,functional linkers.However,whether or not MOFs have a promising future for practical application in emerging contaminants-containing wastewater is debatabie.This review summarizes recent studies about the removal of EOCs using MOFs-related material.The synthesis strategies of both MOF particles and composites,including thin-film nanocomposite and mixed matrix membranes,are criticaily reviewed,as well as various characterization technologies.The application of the MOF-based composite membranes in adsorption,separation(nanofiltration and ultrafiltration),and catalytic degradation are discussed.Overall,literature survey shows that MOFs-based composite could play a crucial role in eliminating EOCs in the future.In particular,modified membranes that realize separation and degradation might be the most promising materials for such application.

关键词： emerging organic contaminants Metalorganicframeworks Synthesis Adsorption Catalysis

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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

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Remediation of preservative ethylparaben in water using natural sphalerite:Kinetics and mechanisms

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Journal of Environmental Sciences 2022年第3期34卷 72-80页

作者： Yanpeng Gao Teng Guo Xiaolin Niu Na Luo Jia Chen Junlang Qiu Yuemeng Ji Guiying Li Taicheng An Guangdong-Hong Kong-Macao Joint Laboratory for contaminants Exposure and Health Guangdong Key Laboratory of Environmental Catalysis and Health Risk ControlInstitute of Environmental Health and Pollution controlGuangdong University of TechnologyGuangzhou 510006China Guangzhou Key Laboratory of Environmental Catalysis and Pollution Control Key Laboratory of City Cluster Environmental Safety and Green developmentSchool of Environmental Science and EngineeringGuangdong University of TechnologyGuangzhou 510006China Division of Analytical and Environmental Toxicology Department of Laboratory Medicine and PathologyFaculty of Medicine and DentistryUniversity of AlbertaEdmontonAB T6G 2G3Canada

As a typical class of emerging organic contaminants(EOCs), the environmental transformation and abatement of preservative parabens have raised certain environmental concerns. However, the remediation of parabens-contaminated water using natural matrixes(such as, naturally abundant minerals) is not reported extensively in literature. In this study, the transformation kinetics and the mechanism of ethylparaben using natural sphalerite(NS) were investigated. The results show that around 63% of ethylparaben could be absorbed onto NS within 38 hr, whereas the maximum adsorption capacity was 0.45 mg/g under room temperature. High temperature could improve the adsorption performance of ethylparaben using NS. In particular, for the temperature of 313 K, the adsorption turned spontaneous. The well-fitted adsorption kinetics indicated that both the surface adsorption and intra-particle diffusion contribute to the overall adsorption process. The monolayer adsorption on the surface of NS was primarily responsible for the elimination of ethylparaben. The adsorption mechanism showed that hydrophobic partitioning into organic matter could largely govern the adsorption process, rather than the Zn S that was the main component of NS. Furthermore, the ethylparaben adsorbed on the surface of NS was stable, as only less than 2% was desorbed and photochemically degraded under irradiation of simulated sunlight for 5 days. This study revealed that NS might serve as a potential natural remediation agent for some hydrophobic EOCs including parabens, and emphasized the significant role of naturally abundant minerals on the remediation of EOCs-contaminated water bodies.

关键词： emerging organic contaminants Paraben Naturally abundant minerals Natural sphalerite Adsorption mechanism

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Activation of peracetic acid by metal-organic frameworks(ZIF-67)for efficient degradation of sulfachloropyridazine

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Chinese Chemical Letters 2022年第6期33卷 3172-3176页

作者： Jun Duan Long Chen Haodong Ji Peishen Li Fan Li Wen Liu The Key Laboratory of Water and Sediment Science Ministry of EducationCollege of Environment Science and EngineeringPeking UniversityBeijing 100871China State Environmental Protection Key Laboratory of All Material Fluxes in River Ecosystems Peking UniversityBeijing 100871China

Peracetic acid(PAA)-based system is becoming an emerging advanced oxidation process(AOP)for effective removal of organic contaminants from water.Various approaches have been tested to activate PAA,while no previous researches reported the application of metal-organic frameworks(MOFs)materials for PAA activation.In this study,zeolitic imidazole framework(ZIF)-67,a representative MOFs,was facile synthesized via direct-mixing method at room temperature,and tested for PAA activation and sulfachloropyridazine(SCP)degradation.The as-synthesized ZIF-67 exhibited excellent performance for PAA activation and SCP degradation with 100%of SCP degraded within 3 min,owing to the specific MOFs structure and abundant Co^(2+) sites.The pseudo-first-order kinetic model was applied to fit the kinetic data,with rate constant k_(1) of ZIF-67 activated PAA system 34.2 and 156.5 times higher than those of conventional Co_(3)O_(4)activated PAA and direct oxidation by PAA.Radical quenching experiments and electron paramagnetic resonance(EPR)analysis indicated that CH_(3)C(O)OO^(·)played a major role in this PAA activation system.Then,the Fukui index based on density functional theory(DFT)calculation was used to predict the possible reaction sites of SCP for electrophilic attack by CH_(3)C(O)OO^(·).In addition,the degradation pathway of SCP was proposed based on Fukui index values and intermediates detection,which mainly included the S-N bond cleavage and SO_(2)extrusion and followed by further oxidation,dechlorination,and hydroxylation.Therefore,ZIF-67 activated PAA is a novel strategy and holds strong potential for the removal of emerging organic contaminants(EOCs)from water.

关键词： Peracetic acid activation Metal-organic frameworks Zeolitic imidazole framework(ZIF)-67 emerging organic contaminants Acetylperoxy radical DFT calculation

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