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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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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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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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In-situ construction of abundant active centers on hierarchically porous carbon electrode toward high-performance phosphate electrosorption: Synergistic effect of electric field and capture sites

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Green Energy & Environment 2024年第1期9卷 126-137页

作者： Peng Zhang Fukuan Li Mingming He Silu Huo Xueli Zhang Benqiang Cen Dezhi Fang Kexun Li Hao Wang 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 State key laboratory of Simulation and Regulation of Water Cycles in River Basins China Institute of Water Resources and Hydropower ResearchBeijing100038China

Phosphate removal is crucial for eutrophication control and water quality improvement.Electro-assisted adsorption,an eco-friendly elec-trosorption process,exhibited a promising potential for wastewater treatment.However,there are few works focused on phosphate electro-sorption,and reported electrodes cannot attach satisfactory removal capacities and rates.Herein,electro-assisted adsorption of phosphate via in-situ construction of La active centers on hierarchically porous carbon(LaPC)has been originally demonstrated.The resulted LaPC composite not only possessed a hierarchically porous structure with uniformly dispersed La active sites,but also provided good conductivity for interfacial electron transfer.The LaPC electrode achieved an ultrahigh phosphate electrosorption capability of 462.01 mg g^(-1) at 1 V,outperforming most existing electrodes.The superior phosphate removal performance originates from abundant active centers formed by the coupling of electricﬁeld and capture sites.Besides,the stability and selectivity toward phosphate capture were maintained well even under comprehensive conditions.Moreover,a series of kinetics and isotherms models were employed to validate the electrosorption process.This work demonstrates a deep understanding and promotes a new level of phosphate electrosorption.

关键词： Electro-assisted adsorption Electrosorption Phosphate removal Active centers MOF-derived carbon

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Recent progress on copper catalysts with different surface states for CO_(2)electroreduction

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Journal of Energy Chemistry 2024年第1期88卷 10-27,I0001页

作者： Wenjun Zhang Yang Yang Donggang Guo Lu Liu tianjin key laboratory of environmental remediation and pollution control College of Environmental Science and EngineeringNankai UniversityTianjin 300350China Shanxi laboratory for Yellow River College of Environment and ResourceShanxi UniversityTaiyuan 030006ShanxiChina

The electrochemical carbon dioxide reduction reaction(eCO_(2)RR),which converts CO_(2)into various hydrocarbons or alcohols,has been extensively researched because it promises a sustainable energy economy.However,only copper(Cu)can currently achieve stable and efficient hydrocarbon conversion in the eCO_(2)RR.Therefore,understanding the catalytic mechanisms and summarizing the research progress on synthesis strategies of Cu catalysts are essential for the eCO_(2)RR.This paper reviews Cu catalysts with different surface states of Cu catalysts:oxide-derived Cu,Cu nanoparticles,Cu single atoms,and Cu nanoclusters.It then reviews the development and progress of different Cu-catalyst preparation methods in recent years,focusing on the activity and selectivity of materials.Besides revealing the tendencies of catalytic selection and deep reactive mechanisms of Cu catalysts with four different surface states,this review can guide the subsequent construction of catalysts and provides an understanding of catalytic mechanisms.

关键词： eCO_(2)RR Oxide-derived Cu Cu nanoparticles Cu single atoms Cu nanoclusters

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Recycling of waste aluminum scraps to fabricate sulfidated zero-valent iron-aluminum particles for enhanced chromate removal

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Journal of environmental Sciences 2024年第4期138卷 650-659页

作者： Yahui Zhang Liguo Zhang Jiajia Zeng Shuqun Xu Jianyu Pan Wenzhuo Huang Jianliang Sun Feng Jiang Guangdong Provincial key laboratory of Chemical pollution and environmental Safety&MOE key laboratory of Theoretical Chemistry of Environment School of EnvironmentSouth China Normal UniversityGuangzhou 510006China Guangdong Provincial key Lab of environmental pollution control and remediation Technology School of Environmental Science&EngineeringSun Yat-Sen UniversityGuangzhou 510275China

Massive waste aluminum scraps produced from the spent aluminum products have high electron capacity and can be recycled as an attractive alternative to materials based on zerovalent iron(Fe^(0))for the removal of oxidative contaminants from wastewater.This study thus proposed an approach to fabricate micron-sized sulfidated zero-valent iron-aluminum particles(S-Al^(0)@Fe^(0))with high reactivity,electron selectivity and capacity using recycled waste aluminum scraps.S-Al^(0)@Fe^(0)with a three-layer structure contained zero-valent aluminum(Al^(0))core,Fe^(0) middle layer and iron sulfide(FeS)shell.The rates of chromate(Cr(Ⅵ))removal by S-Al^(0)@Fe^(0)at pH 5.0-9.0 were 1.6-5.9 times greater than that by sulfidated zero-valent iron(S-Fe^(0)).The Cr(Ⅵ)removal capacity of S-Al^(0)@Fe^(0)was 8.2-,11.3-and 46.9-fold greater than those of S-Fe0,zero-valent iron-aluminum(Al^(0)-Fe^(0))and Fe^(0),respectively.The chemical cost of S-Al^(0)@Fe^(0) for the equivalent Cr(Ⅵ)removal was 78.5%lower than that of S-Fe^(0).Negligible release of soluble aluminum during the Cr(Ⅵ)removal was observed.The significant enhancement in the reactivity and capacity of S-Al^(0)@Fe^(0)was partially ascribed to the higher reactivity and electron density of the Al0core than Fe^(0).More importantly,S-Al^(0)@Fe^(0) served as an electric cell to harness the persistent and selective electron transfer from the Al^(0)-Fe^(0) core to Cr(Ⅵ)at the surface via coupling Fe^(0)-Fe^(2+)-Fe^(3+)redox cycles,resulting in a higher electron utilization efficiency.Therefore,S-Al^(0)@Fe^(0) fabricated using recycled waste aluminum scraps can be a cost-effective and environmentally-friendly alternative to S-Fe^(0) for the enhanced removal of oxidative contaminants in industrial wastewater.

关键词： Recycled waste aluminum scraps Oxidative contaminants Cr(Ⅵ)reduction Sulfidated Al^(0)@Fe^(0)particle Electron transfer

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Migration and transformation of Pb,Cu,and Zn during co-combustion of high-chlorine-alkaline coal and Si/Al dominated coal

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Journal of environmental Sciences 2024年第7期141卷 26-39页

作者： Jiangze Luo Qiwei Yang Jianqiao Wang Boxiong Shen Zhuozhi Wang Qiqi Shi Zhong Zhao Chao Huang Jie Xu tianjin key laboratory of Clean Energy and pollution control School of Energy and Environmental EngineeringHebei University of TechnologyTianjin 300103China School of Chemical Engineering Hebei University of TechnologyTianjin 300103China

Shaerhu(SEH)coal is abundant in Xinjiang,China.The utilization of SEH suffers from severe ash deposition,slagging,and fouling problems due to its high-chlorine-alkaline characteristics.The co-combustion of high-alkaline coal and other type coals containing high Si/Al oxides has been proven to be a simple and effective method that will alleviate ash-related problems,but the risk of heavy metals(HMs)contamination in this process is nonnegligible.Hence,the volatilization rates and chemical speciation of Pb,Cu,and Zn in co-combusting SEH and a high Si/Al oxides coal,i.e.,Yuanbaoshan(YBS)coal were investigated in this study.The results showed that the addition of SEH increased the volatilization rates of Pb,Cu,and Zn during the co-combustion at 800℃from 23.70%,23.97%,and 34.98%to 82.31%,30.01%,and 44.03%,respectively,and promoted the extractable state of Cu and Zn.In addition,the interaction between SEH and YBS inhibited the formation of the Pb residue state.SEM-EDS mapping results showed that compared to Zn and Cu,the signal intensity of Pb was extremely weak in regions where some of the Si and Al signal distributions overlap.The DFT results indicated that the O atoms of the metakaolin(Al_(2)O_(3)·2SiO_(2))(001)surface were better bound to the Zn and Cu than Pb atoms after adsorption of the chlorinated HMs.These results contribute to a better understanding of the effects of high-alkaline coal blending combustion on Pb,Cu,and Zn migration and transformation.

关键词： Heavy metals High-chlorine-alkaline coal Coal blending combustion Density functional theory

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Synthesis of chitosan-based grafting magnetic flocculants for flocculation of kaolin suspensions

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Journal of environmental Sciences 2024年第5期139卷 193-205页

作者： Chuang Liu Xiaoyu Wang Sicong Du Wenyan Liang Beijing key Lab for Source control Technology of Water pollution/Engineering Research Center for Water pollution Source control&Eco-remediation/College of environmental Science and Engineering Beijing Forestry UniversityBeijing 100083China

A series of novel chitosan-based magnetic flocculants FS@CTS-P(AM-DMC)was prepared by molecular structure control.The characterization results showed that FS@CTS-P(AM-DMC)had a uniform size of about 21.46 nm,featuring a typical core-shell structure,and the average coating layer thickness of CTS-P(AM-DMC)was about 5.03 nm.FS@CTS-P(AM-DMC)exhibited excellent flocculation performance for kaolin suspension,achieved 92.54% turbidity removal efficiency under dosage of 150 mg/L,pH 7.0,even at high turbidity(2000 NTU)with a removal efficiency of 96.96%.The flocculation mechanism was revealed to be dominated by charge neutralization under acidic and neutral conditions,while adsorption and bridging effects play an important role in alkaline environments.The properties of magnetic aggregates during flocculation,breakage,and regeneration were studied at different pH levels and dosages.In the process of magnetophoretic,magnetic particles collide and adsorb with kaolin particles continuously due to magnetic and electrostatic attraction,transform into magnetic chain clusters,and then further form three-dimensional network magnetic aggregates that can capture free kaolin particles and other chain clusters.Particle image velocimetry confirmed the formation of eddy current of magnetic flocs and experienced three stages:acceleration,stabilization,and deceleration.

关键词： Magnetic flocculation Chitosan Fe_(3)O_(4) Graft copolymerization PIV

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