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Colloid-facilitated release of polybrominated diphenyl ethers at an e-waste recycling site: evidence from undisturbed soil core leaching experiments

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Frontiers of environmental Science & engineering 2024年第2期18卷 91-101页

作者： Zebin Huo Mengjun Xi Lianrui Xu Chuanjia Jiang Wei Chen College of environmental Science and engineering Ministry of Education Key Laboratory of Pollution Processes and Environmental CriteriaTianjin Key Laboratory of Environmental Remediation and Pollution ControlNankai UniversityTianjin 300350China

Polybrominated diphenyl ethers (PBDEs), a class of persistent organic pollutants, have been frequently detected in soil at e-waste recycling sites. However, the key factors controlling the transport of PBDEs from surface soil to the vadose zone and groundwater are unclear. Here, colloid-enhanced leaching of PBDEs from undisturbed soil cores collected at an e-waste recycling site in Tianjin, China, is reported. Spatially heterogeneous release of colloids and PBDEs was observed in all the tested soil cores under chemical and hydrodynamic perturbations, indicating the presence of preferential flow paths. Colloid concentration in the effluent significantly increased as ionic strength decreased (from 10 to 0.01 mmol/L), probably due to the stronger electrostatic repulsion between colloidal particles and the soil matrix at lower ionic strength. In contrast, colloid mobilization was not significantly affected by the changes in pH of the influent (from 4.0 to 10.0) and flow rate (from a Darcy velocity of 1.5 to 6.0 cm/h). The concentrations of 2,2′,3,3′,4,4′,5,5′,6,6′-decabromodiphenyl ether (BDE-209), the predominant PBDE congener at the site, detected in the leachate (ranging from 1.09 to 3.43 ng/L) were much lower than previously reported results from packed column leaching tests, and were positively correlated with colloid concentrations. This indicates that remobilization of colloids at e-waste recycling sites can promote the leaching and downward migration of PBDEs from surface soil. The findings highlight the potential risk of surface soil PBDE contamination to groundwater quality and call for further understanding of colloid-facilitated transport for predicting the fate of PBDEs at e-waste recycling sites.

关键词： Polybrominated diphenyl ether Colloid-facilitated transport E-waste recycling site Undisturbed soil core Groundwater quality

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Mechanisms of isomerization and hydration reactions of typicalβ-diketone at the air-droplet interface

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Journal of environmental Sciences 2024年第7期141卷 225-234页

作者： Yuemeng Ji Weiyong Luo Qiuju Shi Xiaohui Ma Ziqi Wu Weina Zhang Yanpeng Gao Taicheng An Guangdong-Hong Kong-Macao Joint laboratory for Contaminants Exposure and Health Guangdong Key Laboratory of Environmental Catalysis and Health Risk ControlInstitute Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006China Guangzhou key laboratory of environmental Catalysis and Pollution Control Key Laboratory for City Cluster Environmental Safety and Green Development of the Ministry of EducationSchool of Environmental Science and EngineeringGuangdong University of TechnologyGuangzhou 510006China

Acetylacetone(AcAc)is a typical class ofβ-diketones with broad industrial applications due to the property of the keto-enol isomers,but its isomerization and chemical reactions at the air-droplet interface are still unclear.Hence,using combined molecular dynamics and quantum chemistry methods,the heterogeneous chemistry of AcAc at the air-droplet interface was investigated,including the attraction of AcAc isomers by the droplets,the distribution of isomers at the air-droplet interface,and the hydration reactions of isomers at the air-droplet interface.The results reveal that the preferential orientation of two AcAc isomers(keto-and enol-AcAc)to accumulate and accommodate at the acidic air-droplet interface.The isomerization of two AcAc isomers at the acidic air-droplet interface is more favorable than that at the neutral air-droplet interface because the“water bridge”structure is destroyed by H_(3)O^(+),especially for the isomerization from keto-Ac Ac to enol-AcAc.At the acidic air-droplet interface,the carbonyl or hydroxyl O-atoms of two AcAc isomers display an energetical preference to hydration.Keto-diol is the dominant products to accumulate at the air-droplet interface,and excessive keto-diol can enter the droplet interior to engage in the oligomerization.The photooxidation reaction of AcAc will increase the acidity of the air-droplet interface,which indirectly facilitate the uptake and formation of more keto-diol.Our results provide an insight into the heterogeneous chemistry ofβ-diketones and their influence on the environment.

关键词： Acetylacetone Air-droplet interface Theoretical simulation Isomerization Hydration reaction mechanism

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A Unifi ed View of Carbon Neutrality:Solar-Driven Selective Upcycling of Waste Plastics

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Transactions of Tianjin University 2024年第1期30卷 1-26页

作者： Zhiyong Zhao Shuai Yue Gaohua Yang Pengfei Wang Sihui Zhan MOE key laboratory of Pollution Processes and environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution ControlCollege of Environmental Science and EngineeringTianjin 300350China

With the rapid development of plastic production and consumption globally,the amount of post-consumer plastic waste has reached levels that have posed environmental threats.Considering the substantial CO_(2)emissions throughout the plastic lifecycle from material production to its disposal,photocatalysis is considered a promising strategy for eff ective plastic recycling and upcycling.It can upgrade plastics into value-added products under mild conditions using solar energy,realizing zero carbon emissions.In this paper,we explain the basics of photocatalytic plastic reformation and underscores plastic feedstock reformation pathways into high-value-added products,including both degradation into CO_(2)followed by reformation and direct reformation into high-value-added products.Finally,the current applications of transforming plastic waste into fuels,chemicals,and carbon materials and the outlook on upcycling plastic waste by photocatalysis are presented,facilitating the realization of carbon neutrality and zero plastic waste.

关键词： Photocatalysis Photoreforming Plastics upcycling Carbon neutrality Energy storage and conversion

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Strategies of selective electroreduction of aqueous nitrate to N_(2) in chloride-free system:A critical review

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Green Energy & Environment 2024年第2期9卷 198-216页

作者： Fukuan Li Weizhe Zhang Peng Zhang Ao Gong Kexun Li College of environmental Science and engineering Nankai UniversityTianjin300350China MOE key laboratory of Pollution Processes and environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution ControlTianjin Key Laboratory of Environmental Technology for Complex Trans-Media PollutionNankai UniversityTianjin300350China

Electroreduction of nitrate has been gaining wide attention in recent years owing to it's beneficial for converting nitrate into benign N_(2) from the perspective of electrocatalytic denitrification or into value-added ammonia from the perspective of electrocatalytic NH_(3) synthesis.By reason of the undesired formation of ammonia is dominant during electroreduction of nitrate-containing wastewater,chloride has been widely used to improve N_(2) selectivity.Nevertheless,selective electroreduction of nitrate to N2 gas in chloride-containing system poses several drawbacks.In this review,we focus on the key strategies for efficiently enhancing N_(2) selectivity of electroreduction of nitrate in chloride-free system,including optimal selection of elements,combining an active metal catalyst with another metal,manipulating the crystalline morphology and facet orientation,constructing core–shell structure catalysts,etc.Before summarizing the strategies,four possible reaction pathways of electro-reduction of nitrate to N_(2) are discussed.Overall,this review attempts to provide practical strategies for enhancing N2 selectivity without the aid of electrochlorination and highlight directions for future research for designing appropriate electrocatalyst for final electrocatalytic denitrifi-cation.

关键词： Nitrate Chloride Electroreduction Selectivity Nitrogen

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Tailoring the surface and interface structures of photocatalysts to enhance hydrogen production

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Science China Chemistry 2024年第4期67卷 1161-1174页

作者： Tao Zhang Pengfei Wang Shuai Yue Fei Li Zhiyong Zhao Sihui Zhan MOE key laboratory of Pollution Processes and environmental Criteria/Tianjin key laboratory of environmental Remediation and Pollution Control College of Environmental Science and EngineeringNankai UniversityTianjin 300350China

Photocatalytic water splitting using semiconductor photocatalysts is a promising approach for the production of carbon-neutral,sustainable and clean hydrogen fuel.However,the separation and transport of photoinduced carriers are generally considered to be rate-limiting steps,and their low efficiency remains a major challenge.Therefore,much effort has been devoted to developing new strategies in surface/interface engineering of photocatalysts to improve the dynamics of charge separation/transport.This feature article briefly summarizes recent advances in photocatalyst surface/interface engineering by our research group,which have been achieved through the design of various novel photocatalysts,including interfacial modulation,heterostructure construction,heteroatom doping,single atom and diatom sites.The article is divided into three parts:first,we briefly introduce the three key processes involved in solar water splitting and reveal relationships between the properties of nanostructural photocatalysts and the fundamentals of water splitting;second,we detail methods and strategies for surface and interfacial structures to improve the efficiency of the fundamental processes,especially charge separation;finally,we explore prospects for photocatalytic water splitting applications.This article provides a valuable resource and strategies for researchers currently working in the field of photocatalytic water splitting.

关键词： photocatalytic water splitting surface/interface structures dual-functional photocatalysis

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Intake of tobacco nitrosamines of smokers in various provinces of China and their cancer risk:A meta-analysis

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Journal of environmental Sciences 2024年第7期141卷 249-260页

作者： Xiao Li Zhiwei Ye Jun Wang Pengfei Lin Xiaojin Zhang Shuguang Xie Chao Chen Research Institute for environmental Innovation(Suzhou) TsinghuaSuzhouJiangsu 215163China State key Joint laboratory of environmental Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China Shenzhen key laboratory of Organic Pollution Prevention and Control State Key Laboratory of Urban Water Resource and EnvironmentHarbin Institute of TechnologyShenzhen 518055China State key Joint laboratory of environmental Simulation and Pollution Control College of Environmental Science and EngineeringPeking UniversityBeijing 100871China

Nitrosamines are a class of carcinogens which have been detected widely in food,water,some pharmaceuticals as well as tobacco.The objectives of this paper include reviewing the basic information on tobacco consumption and nitrosamine contents,and assessing the health risks of tobacco nitrosamines exposure to Chinese smokers.We searched the publications in English from“Web of Science”and those in Chinese from the“China National Knowledge Infrastructure”in 2022 and collected 151 literatures with valid information.The content of main nitrosamines in tobacco,including 4-(methylnitrosoamino)-1-(3-pyridyl)-1-butanone(NNK),N-nitrosonornicotine(NNN),N-nitrosoanatabine(NAT),N-nitrosoanabasine(NAB),total tobacco-specific nitrosamines(TSNA),and N-nitrosodimethylamine(NDMA)were summarized.The information of daily tobacco consumption of smokers in 30 provinces of China was also collected.Then,the intakes of NNN,NNK,NAT,NAB,TSNAs,and NDMA via tobacco smoke were estimated as 1534ng/day,591 ng/day,685 ng/day,81 ng/day,2543 ng/day,and 484 ng/day by adult smokers in30 provinces,respectively.The cancer risk(CR)values for NNN and NNK inhalation intake were further calculated as 1.44×10^(-5)and 1.95×10^(-4).The CR value for NDMA intake via tobacco smoke(inhalation:1.66×10^(-4))indicates that NDMA is similarly dangerous in tobacco smoke when compared with the TSNAs.In China,the CR values caused by average nitrosamines intake via various exposures and their order can be estimated as the following:smoke(3.75×10^(-4))>food(1.74×10^(-4))>drinking water(1.38×10^(-5)).Smokers in China averagely suffer 200%of extra cancer risk caused by nitrosamines in tobacco when compared with non-smokers.

关键词： N-nitrosamine Tobacco Cancer risk Tobacco specific nitrosamines(TSNAs) N-nitrosodimethylamine(NDMA)

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Electrochemical filtration for drinking water purification:A review on membrane materials,mechanisms and roles

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Journal of environmental Sciences 2024年第7期141卷 102-128页

作者： Yuying Qi Donghao Li Shixuan Zhang Fengxiang Li Tao Hua College of environmental Science and engineering Nankai UniversityTianjin 300350China key laboratory of Pollution Process and environmental Criteria Ministry of EducationTianjin 300350China Tianjin engineering Center of environmental Diagnosis and Contamination Remediation Tianjin 300350China

Electrochemical filtration can not only enrich low concentrations of pollutants but also produce reactive oxygen species to interact with toxic pollutants with the assistance of a power supply,making it an effective strategy for drinking water purification.In addition,the application of electrochemical filtration facilitates the reduction of pretreatment procedures and the use of chemicals,which has outstanding potential for maximizing process simplicity and reducing operating costs,enabling the production of safe drinking water in smaller installations.In recent years,the research on electrochemical filtration has gradually increased,but there has been a lack of attention on its application in the removal of low concentrations of pollutants from low conductivity water.In this review,membrane substrates and electrocatalysts used to improve the performance of electrochemical membranes are briefly summarized.Meanwhile,the application prospects of emerging single-atom catalysts in electrochemical filtration are also presented.Thereafter,several electrochemical advanced oxidation processes coupled with membrane filtration are described,and the related working mechanisms and their advantages and shortcomings used in drinking water purification are illustrated.Finally,the roles of electrochemical filtration in drinking water purification are presented,and the main problems and future perspectives of electrochemical filtration in the removal of low concentration pollutants are discussed.

关键词： Electrochemical filtration Drinking water Conductive membrane Low concentration Electrocatalyst

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Cobalt doping amount determines dominant reactive species in peroxymonosulfate activation via porous carbon catalysts co-doped by cobalt and nitrogen

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Journal of environmental Sciences 2024年第4期138卷 212-226页

作者： Xiang Li Limeng Wu Aiqin Zhang Shaohua Wu Yan Lin Chunping Yang key laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle Nanchang Hangkong UniversityNanchang 330063China Academy of environmental and Resource Sciences School of Environmental Science and EngineeringGuangdong University of Petrochemical TechnologyMaoming 525000China College of environmental Science and engineering Hunan University and Key Laboratory of Environmental Biology and Pollution Control(Hunan University)Ministry of EducationChangsha 410082China

Switching the reaction routes in peroxymonosulfate(PMS)-based advanced oxidation processes have attracted much attention but remain challenging.Herein,a series of Co-N/C catalysts with different compositions and structures were prepared by using bimetallic zeolitic imidazolate frameworks based on ZIF-8 and ZIF-67(x Zn/Co-ZIFs).Results show that Co doping amount could mediate the transformation of the activation pathway of PMS over CoN/C.When Co doping amount was less than 10%,the constructed x Co-N/C/PMS system(x≤10%)was singlet oxygen-dominated reaction;however further increasing Co doping amount would lead to the generation and coexistence of sulfate radicals and high-valent cobalt,besides singlet oxygen.Furthermore,the nitrogen-coordinated Co(Co-NX)sites could serve as main catalytically active sites to generate singlet oxygen.While excess Co doping amount caused the formation of Co nanoparticles from which leached Co ions were responsible for the generation of sulfate radicals and high-valent cobalt.Compared to undoped N/C,Co doping could significantly enhance the catalytic performance.The 0.5%Co-N/C could achieve the optimum degradation(0.488 min^(-1))and mineralization abilities(78.4%)of sulfamethoxazole among the investigated Co-N/C catalysts,which was superior to most of previously reported catalysts.In addition,the application prospects of the two systems in different environmental scenarios(pH,inorganic anions and natural organic matter)were assessed and showed different degradation behaviors.This study provides a strategy to regulate the reactive species in PMS-based advanced oxidation process.

关键词： Peroxymonosulfate Sulfate radical Singlet oxygen Cobalt Zeolitic imidazolate framework Advanced oxidation process

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Effect of initial ammonium concentration on a one-stage partial nitrification/anammox biofilm system:Nitrogen removal performance and the microbial community

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Journal of environmental Sciences 2024年第9期143卷 176-188页

作者： Mengyu Zhou Yun Han Yang Zhuo Fen Yu Gaoyuan Hu Dangcong Peng School of Municipal and environmental engineering Xi’an University of Architecture and TechnologyXi’an 710055China Shaanxi key laboratory of environmental engineering Xi’an University of Architecture and TechnologyXi’an 710055China key laboratory of Northwest Water Resource Environment and EcologyMOEXi’an University of Architecture and TechnologyXi’an 710055China

One-stage partial nitrification coupled with anammox(PN/A)technology effectively reduces the energy consumption of a biological nitrogen removal system.Inhibiting nitrite-oxidizing bacteria(NOB)is essential for this technology to maintain efficient nitrogen removal performance.Initial ammonium concentration(IAC)affects the degree of inhibited NOB.In this study,the effect of the IAC on a PN/A biofilm was investigated in a moving bed biofilm reactor.The results showed that nitrogen removal efficiency decreased from 82.49%±1.90%to 64.57%±3.96%after the IAC was reduced from 60 to 20 mg N/L,while the nitrate production ratio increased from 13.87%±0.90%to 26.50%±3.76%.NOB activity increased to1,133.86 mg N/m^(2)/day after the IAC decreased,approximately 4-fold,indicating that the IAC plays an important inhibitory role in NOB.The rate-limiting step in the mature biofilm of the PN/A system is the nitritation process and is not shifted by the IAC.The analysis of the microbial community structure in the biofilm indicates that the IAC was the dominant factor in changes in community structure.Ca.Brocadia and Ca.Jettenia were the main anammox bacteria,and Nitrosomonas and Nitrospira were the main AOB and NOB,respectively.IAC did not affect the difference in growth between Ca.Brocadia and Ca.Jettenia.Thus,modulating the IAC promoted the PN/A process with efficient nitrogen removal performance at medium to low ammonium concentrations.

关键词： Biological nitrogen removal Partial nitrification Anammox Ammonium concentration Biofilm

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Research progress on metal-organic framework compounds(MOFs)in electrocatalysis

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Journal of environmental Sciences 2024年第7期141卷 261-276页

作者： Yutong Guo Shunzheng Zhao Xiaolong Tang Honghong Yi Department of environmental Science and engineering School of Energy and Environmental EngineeringUniversity of Science and Technology BeijingBeijing 100083China Beijing key laboratory of Resource-oriented Treatment of Industrial Pollutants Beijing 100083China

Metal-organic frameworks(MOFs)have favorable characteristics such as large specific surface area,high porosity,structural diversity,and pore surface modification,giving them great potential for development and attractive prospects in the research area of modern materials electrocatalysis.However,unsatisfactory catalytic activity and poor electronic conductivity are the main challenges facing MOFs.This review focuses on MOF-based materials used in electrocatalysis,based on the types of catalytic reactions that have used MOF-based materials in recent years along with their applications,and also looks at some new electrocatalytic materials and their future development prospects.

关键词： Metal-organic frame compounds Electrocatalysis Oxidation-reduction Nitrogen fixation to synthesize ammonia Carbon dioxide reduction

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