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Abundance and sources of particulate polycyclic aromatic hydrocarbons and aromatic acids at an urban site in central China

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Journal of Environmental Sciences 2024年第8期142卷 155-168页

作者： Luqi Shang Zhe Dong Zihan Li Mingkai Wang Zihan Kong Xiao Li Ruiqin Zhang School of Ecology and Environment Zhengzhou UniversityZhengzhou 450001China College of Chemistry Zhengzhou UniversityZhengzhou 450001China Institute of Environmental Sciences Zhengzhou UniversityZhengzhou 450001China

We conducted a simultaneous field study of PM_(2.5)-bound particulate polycyclic aromatic hydrocarbons(PAHs)and aromatic acids(AAs)in a polluted city Zhengzhou to explore the concentration,sources and potential conversion pathways between PAHs and AAs in different seasons.The average concentrations of PM_(2.5),28PAHs and 8AAs during the sampling period were 77μg/m^(3),75 ng/m^(3),and 283 ng/m^(3),respectively.The concentration of both28PAHs and 8AAs were highest in winter and lowest in summer with ratios of 6.3 and 2.3,respectively.PAHs with 5-7 rings were the main components of PAHs(52%),followed by 4rings PAHs(30%)and 2-3 rings PAHs(18%).According to the source appointment results obtained by positive matrix factorization,the main sources of PAHs were combustion and vehicle emissions,which account for 37%and 34%,respectively.8AAs were divided into three groups,including four benzene dicarboxylic acids(B2CAs),three benzene tricarboxylic acids(B3CAs)and one benzene tetracarboxylic acid(B4CA).And interspecies correlation analysis with PM_(2.5)source markers were used to investigate potential sources.Phthalic acid(o-Ph)was the most abundant specie of 8AAs(157 ng/m^(3),55%of 8AAs),which was well correlated with sulfate.Meanwhile,B3CAs and B4CA were highly correlated with sulfate and weakly correlated with levoglucosan,suggesting that secondary formation was their main source.As logical oxidation products of PAHs,o-Ph and B3CAs showed good correlations with a number of PAHs,indicating possible photochemical oxidation pathway by PAHs.In addition,O_(3),NO_(2),temperature and relative humidity have positive effects on the secondary formation of B3CAs.

关键词： polycyclic aromatic hydrocarbons aromatic acids Source appointment Secondary formation

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Migration and fate of polycyclic aromatic hydrocarbons in bioretention systems with different media:experiments and simulations

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Frontiers of Environmental Science & Engineering 2024年第4期18卷 17-33页

作者： Zhaoxin Zhang Jiake Li Zhe Liu Yajiao Li Bei Zhang Chunbo Jiang Institute of Land Engineering and Technology Shaanxi Provincial Land Engineering Construction Group Co.Ltd.Xi’an 710075China State Key Laboratory of Eco-hydraulics in Northwest Arid Region of China Xi’an University of TechnologyXi’an 710048China School of Architecture and Civil Engineering Xi’an University of Science and TechnologyXi’an 710054China College of Landscape Architecture and Art Northwest A&F UniversityYangling 712100China

polycyclic aromatic hydrocarbons(PAHs)present significant risks to human health owing to their carcinogenic,teratogenic,and mutagenic properties.The contamination of surface water with PAHs via runoff has become a prominent source of water pollution.While the capacity of bioretention systems to remove PAHs from runoff is recognized,the dynamics of PAH migration and degradation in these systems are not well-understood.This study aims to explain the migration and fate of PAHs in bioretention systems through a series of experiments and model simulations.This study constructed bioretention systems with three different media types and found that these systems achieved PAH load reductions exceeding 92%.Notably,naphthalene(NAP),fluoranthene(FLT),and pyrene(PYR)tended to accumulate in the media’s upper layer,at depths of 10 to 40 cm.To further analyze the migration and fate of PAHs during multi-site rainfall events and across prolonged operation,we applied the HYDRUS-1D model under three distinct scenarios.The findings of this study indicated that NAP degraded in 40 d,whereas FLT and PYR showed incomplete degradation after 120 d.During continuous rainfall events,there was no clear pattern of PAH accumulation;however,FLT and PYR persisted in the bioretention systems.The combination of experimental and simulation findings highlights the inevitable accumulation of PAHs during extended use of bioretention systems.This research provides a theoretical basis for improving operational efficiency,advancing PAH degradation in bioretention systems,and reducing their toxicity.

关键词： Bioretention polycyclic aromatic hydrocarbons HYDRUS-1D Model simulation Migration

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Changes in the Non-targeted Metabolomic Profile of Three-year-old Toddlers with Elevated Exposure to polycyclic aromatic hydrocarbons

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Biomedical and Environmental Sciences 2024年第5期37卷 479-493页

作者： LI Yang LIN Dan ZHANG Xiu Qin JU Guang Xiu SU Ya ZHANG Qian DUAN Hai Ping YU Wei Sen WANG Bing Ling PANG Shu Tao Department of Epidemiology and Health Statistics School of Public HealthQingdao UniversityQingdao 266021ShandongChina Department of Environmental Health Qingdao Municipal Center for Disease Control and PreventionQingdao Institute of Preventive MedicineQingdao 266033ShandongChina Physicochemical Laboratory Qingdao Municipal Center for Disease Control and PreventionQingdao Institute of Preventive MedicineQingdao 266033ShandongChina Section of Child Health Care Huangdao Maternity and Child Health Care Hospital of QingdaoQingdao 266499ShandongChina Qingdao Blood Center Qingdao 266071ShandongChina

Objective To investigate changes in the urinary metabolite profiles of children exposed to polycyclic aromatic hydrocarbons(PAHs)during critical brain development and explore their potential link with the intestinal microbiota.Methods Liquid chromatography-tandem mass spectrometry was used to determine ten hydroxyl metabolites of PAHs(OH-PAHs)in 36-month-old children.Subsequently,37 children were categorized into low-and high-exposure groups based on the sum of the ten OH-PAHs.Ultra-high-performance liquid chromatography coupled with quadrupole time-of-flight mass spectrometry was used to identify non-targeted metabolites in the urine samples.Furthermore,fecal flora abundance was assessed by 16S rRNA gene sequencing using Illumina MiSeq.Results The concentrations of 21 metabolites were significantly higher in the high exposure group than in the low exposure group(variable importance for projection>1,P<0.05).Most of these metabolites were positively correlated with the hydroxyl metabolites of naphthalene,fluorine,and phenanthrene(r=0.336–0.531).The identified differential metabolites primarily belonged to pathways associated with inflammation or proinflammatory states,including amino acid,lipid,and nucleotide metabolism.Additionally,these distinct metabolites were significantly associated with specific intestinal flora abundances(r=0.34–0.55),which were mainly involved in neurodevelopment.Conclusion Higher PAH exposure in young children affected metabolic homeostasis,particularly that of certain gut microbiota-derived metabolites.Further investigation is needed to explore the potential influence of PAHs on the gut microbiota and their possible association with neurodevelopmental outcomes.

关键词： Child Gut microbiota Non-targeted metabolomics polycyclic aromatic hydrocarbons Urinary metabolite profile

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Selective separation of pyrene from mixed polycyclic aromatic hydrocarbons by a hexahedral metal-organic cage

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Chinese Chemical Letters 2024年第1期35卷 523-527页

作者： Ya-Liang Lai Juan Su Le-Xiong Wu Dong Luo Xue-Zhi Wang Xian-Chao Zhou Chuang-Wei Zhou Xiao-Ping Zhou Dan Li College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China

polycyclic aromatic hydrocarbons(PAHs)play an important role in the industry,and the development of new materials for the selective separation of PAHs is of great significance.In this work,we report a hexahedral metal-organic cage with low symmetry by subcomponent self-assembly.In this cage,the eight ZnII centers adopt an interestin∧∧/△△△△△△or∧∧∧∧∧∧/△△configuration.This cage with a cavity volume of 520˚A3 can bind anthracene,phenanthrene,and pyrene to form 1:1 host-guest complexes,while the bigger triphenylene,chrysene,perylene,and coronene cannot be encapsulated.The binding constant Ka of pyrene is about 1.110×10^(3)(mol/L)^(−1),which is more than an order of magnitude larger than that of anthracene and phenanthrene(111(mol/L)^(−1),277(mol/L)^(−1),respectively).X-ray structure studies reveal that the pyrene is located in the cavity and stabilized by multiple C–H…πinteractions.After separation from a mixture of PAHs,pyrene with>96.1%purity can be obtained.This work provides a useful method for the first time for the selective separation of pyrene from PAHs mixture by utilizing a metal-organic cage as the material,making it a useful tool for purifying and separating specific compounds from complex mixtures.

关键词： polycyclic aromatic hydrocarbons Metal-organic cage Host-guest chemistry Selective separation

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Study on Adsorption Removal of polycyclic aromatic hydrocarbons by Modified Mussel Shells

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Meteorological and Environmental Research 2024年第1期15卷 83-86页

作者： Jiaxing LIU Muchen LANG Mei LIU Kecun MA Qingguo CHEN Zhejiang Provincial Key Laboratory of Petrochemical Pollution Control Zhejiang Ocean UniversityZhoushan 316022China School of Petrochemical Engineering&Environment Zhejiang Ocean UniversityZhoushan 316022China School of Marine Science&Technology Zhejiang Ocean UniversityZhoushan 316022China ZPC(Zhejiang Pilot Free Trade Zone)Green Petrochemical Research Institute Co. Ltd.Zhoushan 316000China Zhejiang Petroleum&Chemical Co. Ltd.(ZPC)Zhoushan 316000China

polycyclic aromatic hydrocarbons(PAHs)are typical persistent organic pollutants(POPs)that are commonly found in the environment.They are carcinogenic,teratogenic,mutagenic and biodegradable obviously.In this paper,the modified mussel shells were used to adsorb and remove anthracene.The results show that the adsorption removal rate of the mussel shells was higher after calcination at 600℃.5%H_(3)PO_(4) solution was more suitable for shell treatment than 3 mol/L ZnCl_(2) solution.As the dosage of the modified shells was 0.5 g/L,the adsorption reached a stable state,and the removal rate of PAHs was about 69.44%;the adsorption efficiency rose with the increase of time.It can be seen that as a new and cheap biological adsorbent,the modified shells can be used to remove PAHs from wastewater.

关键词： Mussel shells Adsorption polycyclic aromatic hydrocarbons

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polycyclic aromatic hydrocarbons (PAHs) in a sediment core from Lake Taihu and their associations with sedimentary organic matter

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Journal of Environmental Sciences 2023年第7期129卷 79-89页

作者： Yong He Xiangyu Wang Zhaobin Zhang College of Urban and Environmental Sciences Peking UniversityBeijing 100871China

Sediment core is the recorder of polycyclic aromatic hydrocarbon(PAH)pollutions and the associated sedimentary organic matter(SOM),acting as crucial supports for pollution control and environmental management.Here,the sedimentary records of PAHs and SOM in the past century in Lake Taihu,China,were reconstructed from a 50-cm sediment core.On the one hand,the presence of PAHs ranged from 8.99 to 199.2 ng/g.Vertically,PAHs declined with the depth increased,and the sedimentation history of PAHswas divided into two stages with a discontinuity at 20 cm depth.In composition,PAHs in the sediment core were dominated by three-ring PAHs(44.6%±9.1%,mean±standard deviation),and were followed by four-ring(27.0%±3.3%),and five-ring(12.1%±4.0%)PAHs.In toxicity assessment,the sedimentary records of benzo[a]pyrene-based toxic equivalency were well described by an exponential model with R-square of 0.95,and the environmental background toxic value was identified as 1.62 ng/g.On the other hand,different components of SOM were successfully identified by n-alkanemarkers(p<0.01)and the variations of SOMwerewell explained(84.6%).A discontinuity of SOM was recognized at 22 cm depth.Association study showed that the sedimentary PAHs were associated with both anthropogenic and biogenic SOM(p<0.05)with explained variances for most individual PAHs of 60%.It indicated the vertical distributions of PAHs were driven by sedimentary SOM.Therefore,environmental processes such as biogenic factors should attract more attentions as well as PAH emissions to reduce the impacts of PAHs.

关键词： polycyclic aromatic hydrocarbons (PAHs) N-alkanes Sedimentary records Composition Toxicity assessment Lake Taihu

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Detection of polycyclic aromatic hydrocarbons using a high performance-single particle aerosol mass spectrometer

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Journal of Environmental Sciences 2023年第2期124卷 806-822页

作者： Yao Zhang Chenglei Pei Jinwen Zhang Chunlei Cheng Xiufeng Lian Mubai Chen Bo Huang Zhong Fu Zhen Zhou Mei Li Institute of Mass Spectrometry and Atmospheric Environment Guangdong Provincial Engineering Research Center for On-line Source Apportionment System of Air pollutionJinan UniversityGuangzhou 510632China Guangdong-Hongkong-Macao Joint Laboratory of Collaborative Innovation for Environmental Quality Guangzhou 510632China Guangzhou Environmental Monitoring Center Guangzhou 510030China Guangzhou Hexin Analytical Instrument Company Limited Guangzhou 510530China

The real-time detection of the mixing states of polycyclic aromatic hydrocarbons(PAHs)and nitro-PAHs in ambient particles is of great significance for analyzing the source,aging process,and health effects of PAHs and nitro-PAHs;yet there is still few effective technology to achieve this type of detection.In this study,11 types of PAH and nitro-PAH standard sampleswere analyzed using a high performance-single particle aerosolmass spectrometer(HP-SPAMS)in lab studies.The identification principles‘parent ions’and‘mass-to-charge(m/z)=77’of each compound were obtained in this study.It was found that different laser energies did not affect the identification of the parent ions.The comparative experiments of ambient atmospheric particles,cooking and biomass burning emitted particles with and without the addition of PAHs were conducted and ruled out the interferences from primary and secondary organics on the identification of PAHs.Besides,the reliability of the characteristic ions extraction method was evaluated through the comparative study of similarity algorithm and deep learning algorithm.In addition,the real PAH-containing particles from vehicle exhaust emissions and ambient particles were also analyzed.This study improves the ability of single particle mass spectrometry technology to detect PAHs and nitro-PAHs,and HP-SPAMS was superior to SPAMS for detecting single particles containing PAHs and nitro-PAHs.This study provides support for subsequent ambient observations to identify the characteristic spectrum of single particles containing PAHs and nitro-PAHs.

关键词： Single particle polycyclic aromatic hydrocarbons Identification principles Mass spectrometry Aerosol

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Determination of particulate polycyclic aromatic hydrocarbons in ambient air by gas chromatography-mass spectrometry after molecularly imprinted polymer extraction

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Journal of Environmental Sciences 2023年第2期124卷 644-654页

作者： Maria Chiara Pietrogrande Giorgia Demaria Mara Russo Department of Chemical Pharmaceutical and Agraricultural SciencesUniversity of FerraraVia Fossato di Mortara 17/1944121 FerraraItaly

A solid phase extraction procedure(SPE)is described for the quantitative analysis of polycyclic aromatic hydrocarbons(PAHs)in atmospheric particulate matter(PM),as ubiquitous environmental pollutants routinely measured in air qualitymonitoring.A SPE cartridge was used based on a molecular imprinted polymer(MIP-SPE)properly tailored for selective retention of PAHs with 4 and more benzene fused rings.The performance of the clean-up procedure was evaluated with the specific concern of selective purification towards saturated hydrocarbons,which are the PM components mostly interfering GC analysis of target PAHs.Under optimized operative conditions,the MIP-SPE provided analyte recovery close to 95%for heavier PAHs,from benzo(α)pyrene to benzo(ghi)perylene,and close to 90%for four benzene rings PAHs,with good reproducibility(RSDs:2.5%-5.9%).Otherwise,C_(17)-C_(32) n-alkanes were nearly completely removed.The proposed method was critically compared with Solid Phase Micro Extraction(SPME)using a polyacrylate fiber.Both methods were successfully applied to the analysis of ambient PM2.5 samples collected at an urban polluted site.Between the two procedures,the MIP-SPE provided the highest recovery(R%≥93%)for PAHs with 5 and more benzene rings,but lower for lighter PAHs.In contrast,SPME showed a mean acceptable R%value(∼80%)for all the investigated PAHs,except for the heaviest PAHs in the most polluted samples(R%:110%-138%),suggesting an incomplete purification from the interfering n-hydrocarbons.

关键词： polycyclic aromatic hydrocarbons Atmospheric particle matter Molecularly imprinted polymers-solid-phase extraction Solid phase micro extraction GC/MS analysis

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polycyclic aromatic hydrocarbons in benthos of the northern Bering Sea Shelf and Chukchi Sea Shelf

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Journal of Environmental Sciences 2020年第11期32卷 194-199页

作者： Yuxin Ma Yurong Sun Yunkai Li Hongyuan Zheng Wenying Mi School of Oceanography Shanghai Jiao Tong UniversityShanghai 200030China College of Marine Sciences Shanghai Ocean UniversityShanghai 201306China State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China MINJIE Institute of Environmental Science and Health Research Max-Plank Street 2Geesthacht 21502Germany

Eighteen polycyclic aromatic hydrocarbons(PAHs)were detected in benthos collected onboard the‘Snow Dragon’in the Northern Bering Sea Shelf and Chukchi Sea Shelf during the 6 th Chinese National Arctic Research Expedition(CHINARE 2014).18 PAHs for all biota samples ranged from 34.2 to 128.1 ng/g dry weight(dw),with the highest concentration observed in fish muscle(Boreogadus saida)samples close to St.Lawrence Island.The PAH composition pattern was dominated by the presence of lighter 3 ring(57%)and 2 ring(28%)PAHs,indicating oil-related or petrogenic sources as important origins of PAH contamination.Concentrations of alkyl-PAHs(1-methylnaphthalene and 2-methylnaphthalene)were lower than their parent PAH(naphthalene)in all biological tissue,and their percentage also decreased significantly(p<0.05)compared with those in the corresponding sediment.There were no significant relationships between PAH concentrations and trophic levels,which is possibly due to the combined results of the complex benthic foodweb in the subarctic/Arctic shelf region,as well as a low assimilation/effective metabolism for PAHs.According to toxic potency evaluation results from TCDD toxic equivalents(TEQs)and Ba P-equivalent(Ba PE)values,whelk(Neptunea heros)and starfish(Ctenodiscus crispatus)are two macroinvertebrate species showing relatively higher dioxin-like toxicity and carcinogenic risk.

关键词： polycyclic aromatic hydrocarbons Arctic shelf Benthos Toxic potency Bioaccumulation

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High-precision standard enthalpy of formation for polycyclic aromatic hydrocarbons predicting from general connectivity based hierarchy with discrete correction of atomization energy

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Frontiers of Chemical Science and Engineering 2022年第12期16卷 1743-1750页

作者： Zihan Xu Huajie Xu Lu Liu Rongpei Jiang Haisheng Ren Xiangyuan Li School of Chemical Engineering Sichuan UniversityChengdu 610065China Beijing Institute of Aerospace Testing Technology Beijing 100074China Engineering Research Center of Combustion and Cooling for Aerospace Power Ministry of Education Chengdu 610065China

The standard enthalpy of formation is an important predictor of the reaction heat of a chemical reaction.In this work,a high-precision method was developed to calculate accurate standard enthalpies of formation for polycyclic aromatic hydrocarbons based on the general connectivity based hierarchy(CBH)with the discrete correction of atomization energy.Through a comparison with available experimental findings and other high-precision computational results,it was found that the present method can give a good description of enthalpy of formation for polycyclic aromatic hydrocarbons.Since CBH schemes can broaden the scope of application,this method can be used to investigate the energetic properties of larger polycyclic aromatic hydrocarbons to achieve a high-precision calculation at the CCSD(T)/CBS level.In addition,the energetic properties of CBH fragments can be accurately calculated and integrated into a database for future use,which will increase computational efficiency.We hope this work can give new insights into the energetic properties of larger systems.

关键词： standard enthalpy of formation polycyclic aromatic hydrocarbons connectivity based hierarchy high-precision calculation

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