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Prediction model on hydrolysis kinetics of phthalate monoester:A density functional theory study

Journal of environmental sciences 2024年第1期135卷 51-58页

作者： Tong Xu Jingwen Chen Deming Xia Weihao Tang Jiansheng Cui Chun Liu Shuangjiang Li College of environmental science and Engineering Hebei University of Science and TechnologyShijiazhuang 050000China Key laboratory of Industrial Ecology and environmental Engineering(Ministry of Education) School of Environmental Science and TechnologyDalian University of TechnologyDalian 116024China National-Regional joint Engineering Research Center for Soil Pollution Control and Remediation in South China Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and ManagementInstitute of Eco-environmental and Soil SciencesGuangdong Academy of SciencesGuangzhou 510650China

As primary degradation products of phthalate esters,phthalate monoesters(MPEs)have been widely detected in various aquatic environments and drawn growing toxicological concerns.Hydrolysis kinetics that is of importance for assessing environmental persistence of chemicals remain elusive for MPEs.Herein,kinetics of base-catalyzed and neutral hydrolysis for 18 MPEs with different leaving groups was investigated by density functional theory calculation.Results indicate that MPEs with leaving groups having p Kaof<10 prefer dissociative transition states.MPEs are more persistent than their parents,and their hydrolysis half-lives were calculated to vary from 3.4 min to 79.2 years(p H=7–9).A quantitative structure-activity relationship model was developed for predicting the hydrolysis kinetics parameters.It was found that p Kaof the leaving groups and electronegativity of the MPEs are key factors determining the hydrolysis kinetics.This work may lay a theoretical foundation for better understanding the chemical process that governs MPE persistence in aquatic environments.

关键词： Phthalate monoesters Phthalate esters Hydrolysis Density functional theory Quantitative structure-activity relationship

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Atmospheric VOCs in an industrial coking facility and the surrounding area:Characteristics,spatial distribution and source apportionment

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Journal of environmental sciences 2024年第4期138卷 660-670页

作者： Meicheng Wen Weiqiang Deng Jin Huang Shu Zhang Qinhao Lin ChaoWang Shengtao Ma Wanjun Wang Xin Zhang 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 Guangdong Engineering technology Research Center for Photocatalytic technology Integration and Equipment Guangzhou Key Laboratory of Environmental Catalysis and Pollution ControlSchool of Environmental Science and EngineeringGuangdong University of TechnologyGuangzhou 510006China Institute of environmental science Shanxi UniversityTaiyuan 030006China

Industrial coking facilities are an important emission source for volatile organic compounds(VOCs).This study analyzed the atmospheric VOC characteristics within an industrial coking facility and its surrounding environment.Average concentrations of total VOCs(TVOCs)in the surrounding residential activity areas(R1 and R2),the coking facility(CF)and the control area(CA)were determined to be 138.5,47.8,550.0,and 15.0μg/m^(3),respectively.The cold drum process and coking and quenching areas within the coking facility were identified as the main polluting processes.The spatial variation in VOCs composition was analyzed,showing that VOCs in the coking facility and surrounding areas were mainly dominated by aromatic compounds such as BTX(benzene,toluene,and xylenes)and naphthalene,with concentrations being negatively correlated with the distance from the coking facility(p<0.01).The sources of VOCs in different functional areas across the monitoring area were analyzed,finding that coking emissions accounted for 73.5%,33.3% and 27.7% of TVOCs in CF,R1 and R2,respectively.These results demonstrated that coking emissions had a significant impact on VOC concentrations in the areas surrounding coking facility.This study evaluates the spatial variation in exposure to VOCs,providing important information for the influence of VOCs concentration posed by coking facility to surrounding residents and the development of strategies for VOC abatement.

关键词： Coking facility Volatile organic compounds Emission inventory Spatial distribution Source apportionment

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Photodegradation of xylene isomers:Kinetics,mechanism,secondary pollutant formation potential and health risk evaluation

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Journal of environmental sciences 2024年第2期136卷 658-669页

作者： Xiaoyan Chen Weikun Zhu Sufen Feng Jiangyao Chen Guangdong Key laboratory of environmental Catalysis and Health Risk Control Guangdong Technology Research Center for Photocatalytic Technology Integration and Equipment EngineeringInstitute of Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006China Guangzhou Key laboratory of environmental Catalysis and Pollution Control Guangdong-Hong Kong-Macao Joint Laboratory for Contaminants Exposure and HealthSchool of Environmental Science and EngineeringGuangdong University of TechnologyGuangzhou 510006China

Photodegradation technology has been widely applied in the purification of industrial aromatic hydrocarbons.However,whether this technology efficiently removes the pollutants to prevent secondary pollution and health risk is still unclear.Here,the photodegradation processes of three xylenes were compared under designed reaction atmospheres and light sources.Xe lamp showed poor photodegradation ability toward xylenes,no matter in N_(2) or N_(2)+O_(2)system,while much higher photodegradation performance of xylenes were obtained under ultraviolet(UV)and vacuum ultraviolet(VUV)irradiation,especially in N_(2)+O_(2)+VUV system,where 97.9%of m-xylene,99.0%of o-xylene or 87.5%of p-xylene with the initial concentration of 860 mg/m^(3) was removed within 240 min.The xylenes underwent three processes of photo-isomerization,photodecomposition and photo-oxidation to produce intermediates of aromatics,alkanes and carbonyls.Among them,the photo-isomerization products showed the highest concentration percentage(e.g.,≥50%in o-xylene system),confirming that photo-isomerization reaction was the dominated photodegradation process of xylenes.Moreover,these isomerized products not only contributed about 97%and91%to the formation potential of O3(OFP)and secondary organic aerosols(SOAFP),but also displayed obvious non-carcinogenic risk,although one of photodecomposition product—benzene showed the highest occupational exposure risk.Therefore,the secondary pollution and health risks of photodegradation products of xylenes were non-ignorable,although the OFP,SOAFP and health risks of the generated products reduced at least 4.5 times in comparison with that of the degraded xylenes.The findings are helpful for the appropriate application of this technology in the purification of industrial organic waste gas.

关键词： Isomer aromatics Photodegradation Ozone formation Secondary organic aerosols Health risk

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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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Dissolved organic matter accelerates microbial degradation of 17 alpha-ethinylestradiol in the presence of iron mineral

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Journal of environmental sciences 2024年第5期139卷 364-376页

作者： Huan He Min Shi Xiaoxia Yang Juhong Zhan Yanting Lin Ziwei Guo Zhicheng Liao Chaochao Lai Xiaomin Ren Bin Huang Xuejun Pan Faculty of environmental science and Engineering Kunming University of Science and TechnologyKunming 650500China Yunnan Provincial Key lab of Soil Carbon Sequestration and Pollution Control Kunming 650500China Research Institute for environmental Innovation(Suzhou)Tsinghua Suzhou 215163China

Dissolved organic matter(DOM)and iron minerals widely existing in the natural aquatic environment can mediate the migration and transformation of organic pollutants.However,the mechanism of interaction between DOM and iron minerals in the microbial degradation of pollutants deserves further investigation.In this study,the mechanism of 17 alphaethinylestradiol(EE2)biodegradation mediated by humic acid(HA)and three kinds of iron minerals(goethite,magnetite,and pyrite)was investigated.The results found that HA and iron minerals significantly accelerated the biodegradation process of EE2,and the highest degradation efficiency of EE2(48%)was observed in the HA-mediated microbial system with pyrite under aerobic conditions.Furthermore,it had been demonstrated that hydroxyl radicals(HO·)was the main active substance responsible for the microbial degradation of EE2.HO·is primarily generated through the reaction between hydrogen peroxide secreted by microorganisms and Fe(II),with aerobic conditions being more conducive.The presence of iron minerals and HA could change the microbial communities in the EE2 biodegradation system.These findings provide new information for exploring the migration and transformation of pollutants by microorganisms in iron-rich environments.

关键词： Dissolved organic matter Iron mineral 17 alpha-ethinylestradiol Biodegradation

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Superhydrophobic magnetic Fe_(3)O_(4) polyurethane sponges for oil-water separation and oil-spill recovery

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Journal of environmental sciences 2024年第5期139卷 160-169页

作者： Shiyu Wu Yunjie Xiang Yaqi Cai Jingfu Liu Sino-Danish College University of Chinese Academy of SciencesBeijing 100049China State Key laboratory of environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China School of Environment Hangzhou Institute for Advanced StudyUCASHangzhou 310024China School of environmental science and Engineering Southern University of Science and TechnologyShenzhen 518055China

The effective and affordable separation of oil and water,a crucial process in the safe han dling of environmental disasters such as crude oil spills and recovery of valuable resources is a highly sought-after yet challenging task.Herein,superhydrophobic PU sponge was fab ricated for the fast and cost-effective adsorptive separation of oil and different organic sol vents from water.Octadecyltrichlorosilane(OTS)-functionalized Fe_(3)O_(4)@SiO_(2)core-shell mi crospheres were dip-coated on the surface of porous materials via a dip-coating process thereby endowing them with superhydrophobicity.Owing to the hydrophobic interaction between OTS molecules and oil and increased capillary force in the micropores,the result ing superhydrophobic sponge served as a selective oil-sorbent scaffold for absorbing oil from oil-water mixtures,including oil-water suspensions and emulsions.Remarkably,after the recovery of the adsorbed oil via mechanical extrusion,these superhydrophobic materials could be reused multiple times and maintain their oil-water separation efficacy even afte 10 oil-water separation cycles.

关键词： Fe_(3)O_(4)@SiO_(2)-OTS polyurethane sponge Oil-water separation Adsorption capacity Oil-spill recovery

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Engineering Strategies for Suppressing the Shuttle Effect in Lithium–Sulfur Batteries

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Nano-Micro Letters 2024年第1期16卷 187-221页

作者： Jiayi Li Li Gao Fengying Pan Cheng Gong Limeng Sun Hong Gao Jinqiang Zhang Yufei Zhao Guoxiu Wang Hao Liu joint International laboratory On environmental and Energy Frontier Materials School of Environmental and Chemical EngineeringShanghai UniversityShanghaiPeople’s Republic of China Centre for Clean Energy technology University of Technology SydneyBroadwaySydneyNSW 2007Australia

Lithium–sulfur(Li–S)batteries are supposed to be one of the most potential next-generation batteries owing to their high theoretical capacity and low cost.Nevertheless,the shuttle effect of firm multi-step two-electron reaction between sulfur and lithium in liquid electrolyte makes the capacity much smaller than the theoretical value.Many methods were proposed for inhibiting the shuttle effect of polysulfide,improving corresponding redox kinetics and enhancing the integral performance of Li–S batteries.Here,we will comprehensively and systematically summarize the strategies for inhibiting the shuttle effect from all components of Li–S batteries.First,the electrochemical principles/mechanism and origin of the shuttle effect are described in detail.Moreover,the efficient strategies,including boosting the sulfur conversion rate of sulfur,confining sulfur or lithium polysulfides(LPS)within cathode host,confining LPS in the shield layer,and preventing LPS from contacting the anode,will be discussed to suppress the shuttle effect.Then,recent advances in inhibition of shuttle effect in cathode,electrolyte,separator,and anode with the aforementioned strategies have been summarized to direct the further design of efficient materials for Li–S batteries.Finally,we present prospects for inhibition of the LPS shuttle and potential development directions in Li–S batteries.

关键词： Shuttle effect Designed strategies Li-S battery Lithium polysulfides

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Numerical insight into heat transfer enhancement by granules inner-migration in a moving bed:A performance comparison between slanted-stick and plow-shaped agitator

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Particuology 2024年第6期89卷 109-116页

作者： Binfan Jiang Hao Pei Dehong Xia Haiyang Wang School of Energy and environmental Engineering University of Science and Technology BeijingBeijing 100083China Shunde Graduate School of University of science and technology Beijing Guangdong 528399China Jianlong Group&USTB joint laboratory Beijing 100083China

Waste heat recovery of high-temperature granules is one of the most promising sustainable energy supply and carbon reduction ways for industry.A moving bed indirect heat exchanger(MBIHE)with inner-migration was proposed for granular heat recovery.Granule migration and the enhanced heat transfer induced by two types of agitators(i.e.,agitator with slanted stick A_(s)and with plow-shaped surface A_(p))in the MBIHE are analyzed based on DEM coupled with CFD.Owing to the effective agitation,the average heat transfer coefficient in the granule side is enhanced to∼3 times compared to that without agitation.The heat recovery efficiency in the moving bed reached more than 70%with the agitations of either A_(s)or A_(p).The heat efficiency of A_(s)is∼7%higher than that of A_(p),but with at least 60%greater rotational torque.To ensure reliable agitation,the A_(p)is suggested to be adopted in the MBIHE to induce granule migration.

关键词： Waste heat recovery High-temperature granule Granule migration Heat transfer enhancement Industry energy saving

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Dynamic coupling of ferrihydrite transformation and associated arsenic desorption/redistribution mediated by sulfate-reducing bacteria

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Journal of environmental sciences 2024年第1期135卷 39-50页

作者： Wenjing Zhou Huiyan Zhu Shiwen Hu Bowei Zhang Kun Gao Zhi Dang Chongxuan Liu State environmental Protection Key laboratory of Integrated Surface Water-Groundwater Pollution Control School of Environmental Science and EngineeringSouthern University of Science and TechnologyShenzhen 518055China The Key lab of Pollution Control and Ecosystem Restoration in Industry Clusters Ministry of EducationSouth China University of TechnologyGuangzhou 510006China

Sulfate-reducing bacteria play an important role in the geochemistry of iron(oxyhydr)oxide and arsenic(As)in natural environments;however,the associated reaction processes are yet to be fully understood.In this study,batch experiments coupled with geochemical,spectroscopic,microscopic,and thermodynamic analyses were conducted to investigate the dynamic coupling of ferrihydrite transformation and the associated As desorption/redistribution mediated by Desulfovibrio vulgaris(D.vulgaris).The results indicated that D.vulgaris could induce ferrihydrite transformation via S^(2-)-driven and direct reduction processes.In the absence of SO_(4)^(2-),D.vulgaris directly reduced ferrihydrite,and As desorption and re-sorption occurred simultaneously during the partial transformation of ferrihydrite to magnetite.The increase in SO_(4)^(2-)loading promoted the S^(2-)-driven reduction of ferrihydrite and accelerated the subsequent mineralogical transformation.In the low and medium SO_(4)^(2-)treatments,ferrihydrite was completely transformed to a mixture of magnetite and mackinawite,which increased the fraction of As in the residual phase and stabilized As.In the high SO_(4)^(2-)treatment,although the replacement of ferrihydrite by only mackinawite also increased the fraction of As in the residual phase,22.1%of the total As was released into the solution due to the poor adsorption affinity of As to mackinawite and the conversion of As^(5+)to As^(3+).The mechanisms of ferrihydrite reduction,mineralogy transformation,and As mobilization and redistribution mediated by sulfate-reducing bacteria are closely related to the surrounding SO_(4)^(2-)loadings.These results advance our understanding of the biogeochemical behavior of Fe,S,and As,and are helpful for the risk assessment and remediation of As contamination.

关键词： Sulfate-reducing bacteria Arsenic Ferrihydrite Transformation Redistribution

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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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