Urban rainwater runoff is an important source of nonpoint source pollution due to its transport of diverse contaminants,including polycyclic aromatic hydrocarbons(PAHs)and chlorinated derivatives.Importantly,these chl...Urban rainwater runoff is an important source of nonpoint source pollution due to its transport of diverse contaminants,including polycyclic aromatic hydrocarbons(PAHs)and chlorinated derivatives.Importantly,these chlorinated polycyclic aromatic hydrocarbons(Cl-PAHs)exhibit elevated toxicological potential compared to their non-halogenated parent compounds.In this study,we proposed an approach that combined multivariate receptor model with integration of SHapley Additive exPlanations and Random Forest model.This method identifies the possible sources and reveals the impact of source apportionment results and environmental driving factors(such as geographical and meteorological data)on pollutant concentrations.Sixteen PAHs and nine ClPAHs were detected in 79 runoff samples from all three sites.TheΣ_(16)PAHs average concentration(2923.93 to 6071.83 ng/L)was significantly higher than theΣ_(9)Cl-PAHs(384.34 to 1314.73 ng/L).The source apportionment was conducted by positive matrix factorization(PMF),and six potential pollution sources for PAHs and three for Cl-PAHs were quantified.PAHs primarily originate from the combustion of fossil fuels such as traffic,industrial emissions and coal tar,while Cl-PAHs are mainly derived from atmospheric deposition and industrial emissions.Meanwhile,the self‑organizing map classified PAHs and Cl-PAHs into 2 and 3 groups,respectively.The k-means algorithm yielded 4 clusters for runoff samples.Among machine learning models,Random Forest(RF)demonstrated optimal predictive performance and integrated with SHapley Additive exPlanations(RF-SHAP)revealed the effects of driving factors on the predicted concentration of PAHs and Cl-PAHs in urban runoff samples.展开更多
Studies on the elevation gradient distribution of polycyclic aromatic hydrocarbons(PAHs)have mainly focused on high-altitude regions like the Tibetan Plateau.Investigation of the PAHs distribution in Shennongjia regio...Studies on the elevation gradient distribution of polycyclic aromatic hydrocarbons(PAHs)have mainly focused on high-altitude regions like the Tibetan Plateau.Investigation of the PAHs distribution in Shennongjia region and the effects of total organic carbon(TOC),black carbon(BC)and elevation gradient on PAHs distribution are of great practical significance for protecting the Tibetan Plateau’s environment.This study collected soil and peat samples across varying vegetation types and altitudes in Shennongjia.Results showed that theΣ16PAHs concentrations ranged from 15.44 to 199.13 ng/g in surface soil and 300.15 to 555.52 ng/g in surface peat,respectively,both dominated by low molecular weight PAHs(LMW-PAHs),and the distribution line of PAHs in the soil of Shennongjia area is 1500-1700 m.Above 1700 m,PAH concentrations increased with altitude,influenced significantly by TOC and BC,though dependence on BC was stronger than on TOC.However,the dependence of PAHs on BC is higher than TOC.Through soil-air partition coefficient(KSA)and soil fugacity,it is found that the absorption capacity of PAHs is mainly concentrated in Dajiuhu,which is equivalent to a"trap".The ILCRs induced by PAHs in the soil of Shennongjia area are within the safe range.Shennongjia serves as a barrier,preventing pollutant transport from central emission areas to the Tibetan Plateau.Thus,amid tourism development,addressing traffic-related PAH sources,promoting green energy,and controlling air pollutants in central emission areas are vital for ecological protection in Shennongjia and the Tibetan Plateau.展开更多
Polycyclic Aromatic Hydrocarbons(PAHs),along with their derivatives nitro-PAHs and oxy-PAHs,are globally recognized toxic pollutants.This research conducted daily PM_(2.5)sampling in winter 2021 at three urban(YNCE,SW...Polycyclic Aromatic Hydrocarbons(PAHs),along with their derivatives nitro-PAHs and oxy-PAHs,are globally recognized toxic pollutants.This research conducted daily PM_(2.5)sampling in winter 2021 at three urban(YNCE,SWP,and NG)and three suburban sites(HC,CTV,and YNE)in the Ili River Valley(IRV).For the first time in the IRV,a comprehensive study on 39 PAHs and derivatives was carried out.The results showed that the average∑_(16)PAHs concentration was 130.21±98.94 ng/m^(3),with 16PAHs constituting the dominant fraction(112.51±86.48 ng/m^(3)).The mean BaP and the total BaP equivalent quotient(TEQ)concentrations were 10.28±8.85 ng/m^(3)and 19.74±16.70 ng/m^(3),respectively.Approximately 88%of the daily BaP averages and 98%of the daily TEQ averages exceeded the national daily average standard of BaP(2.5 ng/m^(3)),indicating severe local BaP pollution.Urban sites had notably higher∑PAHs and TEQ concentrations than suburban sites,attributed to increased vehicular traffic and coal combustion in urban areas.PMF results showed that traffic emissions(32.7%-60.5%),coal combustion(13.9%-24.3%)and secondary formation(14.7%-22.7%)were the primary contributors to∑PAHs.Urban sites experienced a greater influence from traffic,while suburban sites were more impacted by coal and biomass burning.On polluted days,traffic sources’contributions increased significantly at HC,YNE,NG and YNCE sites,and secondary formation sources’contributions grew at CTV and YNCE sites.The sourcedependent BaPeq results underscored the role of secondary-formed PAH derivatives in TEQ.展开更多
This study investigated environmental distribution and human exposure of polycyclic aromatic hydrocarbons(PAHs)and their derivatives in one Chinese petroleum refinery facility.It was found that,following with high con...This study investigated environmental distribution and human exposure of polycyclic aromatic hydrocarbons(PAHs)and their derivatives in one Chinese petroleum refinery facility.It was found that,following with high concentrations of 16 EPA PAHs(∑Parent-PAHs)in smelting subarea of studied petroleum refinery facility,total derivatives of PAHs[named as XPAHs,including nitro PAHs(NPAHs),chlorinated PAHs(Cl-PAHs),and brominated PAHs(Br-PAHs)]in gas(mean=1.57×10^(4)ng/m^(3)),total suspended particulate(TSP)(mean=4.33×10^(3) ng/m^(3))and soil(mean=4.37×10^(3) ng/g)in this subarea had 1.76-6.19 times higher levels than those from other subareas of this facility,surrounding residential areas and reference areas,indicating that petroleum refining processes would lead apparent derivation of PAHs.Especially,compared with those in residential and reference areas,gas samples in the petrochemical areas had higher∑NPAH/∑PAHs(mean=2.18),but lower∑Cl-PAH/∑PAHs(mean=1.43×10^(-1))and∑Br-PAH/∑PAHs ratios(mean=7.49×10^(-2)),indicating the richer nitrification of PAHs than chlorination during petrochemical process.The occupational exposure to PAHs and XPAHs in this petroleum refinery facility were 24-343 times higher than non-occupational exposure,and the ILCR(1.04×10^(-4))for petrochemical workers was considered to be potential high risk.Furthermore,one expanded high-resolution screening through GC Orbitrap/MS was performed for soils from petrochemical area,and another 35 PAHs were found,including alkyl-PAHs,phenyl-PAHs and other species,indicat-ing that profiles and risks of PAHs analogs in petrochemical areas deserve further expanded investigation.展开更多
基金supported by Guangdong Basic and Applied Basic Research Foundation(Nos.2021B1515120055 and 2022A1515010499).
文摘Urban rainwater runoff is an important source of nonpoint source pollution due to its transport of diverse contaminants,including polycyclic aromatic hydrocarbons(PAHs)and chlorinated derivatives.Importantly,these chlorinated polycyclic aromatic hydrocarbons(Cl-PAHs)exhibit elevated toxicological potential compared to their non-halogenated parent compounds.In this study,we proposed an approach that combined multivariate receptor model with integration of SHapley Additive exPlanations and Random Forest model.This method identifies the possible sources and reveals the impact of source apportionment results and environmental driving factors(such as geographical and meteorological data)on pollutant concentrations.Sixteen PAHs and nine ClPAHs were detected in 79 runoff samples from all three sites.TheΣ_(16)PAHs average concentration(2923.93 to 6071.83 ng/L)was significantly higher than theΣ_(9)Cl-PAHs(384.34 to 1314.73 ng/L).The source apportionment was conducted by positive matrix factorization(PMF),and six potential pollution sources for PAHs and three for Cl-PAHs were quantified.PAHs primarily originate from the combustion of fossil fuels such as traffic,industrial emissions and coal tar,while Cl-PAHs are mainly derived from atmospheric deposition and industrial emissions.Meanwhile,the self‑organizing map classified PAHs and Cl-PAHs into 2 and 3 groups,respectively.The k-means algorithm yielded 4 clusters for runoff samples.Among machine learning models,Random Forest(RF)demonstrated optimal predictive performance and integrated with SHapley Additive exPlanations(RF-SHAP)revealed the effects of driving factors on the predicted concentration of PAHs and Cl-PAHs in urban runoff samples.
基金supported by the National Natural Science Foundations of China(No.42377235)the National Key Research and Development Program of China(No.2023YFC3709803)+1 种基金the Open Research Fund of Hubei Key Laboratory of Mine Environmental Pollution Control and Remediation(No.2023XZ103)Hubei Polytechnic University talent introduction project(No.24xjz13R).
文摘Studies on the elevation gradient distribution of polycyclic aromatic hydrocarbons(PAHs)have mainly focused on high-altitude regions like the Tibetan Plateau.Investigation of the PAHs distribution in Shennongjia region and the effects of total organic carbon(TOC),black carbon(BC)and elevation gradient on PAHs distribution are of great practical significance for protecting the Tibetan Plateau’s environment.This study collected soil and peat samples across varying vegetation types and altitudes in Shennongjia.Results showed that theΣ16PAHs concentrations ranged from 15.44 to 199.13 ng/g in surface soil and 300.15 to 555.52 ng/g in surface peat,respectively,both dominated by low molecular weight PAHs(LMW-PAHs),and the distribution line of PAHs in the soil of Shennongjia area is 1500-1700 m.Above 1700 m,PAH concentrations increased with altitude,influenced significantly by TOC and BC,though dependence on BC was stronger than on TOC.However,the dependence of PAHs on BC is higher than TOC.Through soil-air partition coefficient(KSA)and soil fugacity,it is found that the absorption capacity of PAHs is mainly concentrated in Dajiuhu,which is equivalent to a"trap".The ILCRs induced by PAHs in the soil of Shennongjia area are within the safe range.Shennongjia serves as a barrier,preventing pollutant transport from central emission areas to the Tibetan Plateau.Thus,amid tourism development,addressing traffic-related PAH sources,promoting green energy,and controlling air pollutants in central emission areas are vital for ecological protection in Shennongjia and the Tibetan Plateau.
基金supported by the National Key R&D Program of China(No.2017YFC0212501)the Fundamental Research Funds for the Central Universities(No.2021YJSMT09)the research project on deep source apportionment of urban air pollution and pollution control strategies in the core area of the Ili River Valley。
文摘Polycyclic Aromatic Hydrocarbons(PAHs),along with their derivatives nitro-PAHs and oxy-PAHs,are globally recognized toxic pollutants.This research conducted daily PM_(2.5)sampling in winter 2021 at three urban(YNCE,SWP,and NG)and three suburban sites(HC,CTV,and YNE)in the Ili River Valley(IRV).For the first time in the IRV,a comprehensive study on 39 PAHs and derivatives was carried out.The results showed that the average∑_(16)PAHs concentration was 130.21±98.94 ng/m^(3),with 16PAHs constituting the dominant fraction(112.51±86.48 ng/m^(3)).The mean BaP and the total BaP equivalent quotient(TEQ)concentrations were 10.28±8.85 ng/m^(3)and 19.74±16.70 ng/m^(3),respectively.Approximately 88%of the daily BaP averages and 98%of the daily TEQ averages exceeded the national daily average standard of BaP(2.5 ng/m^(3)),indicating severe local BaP pollution.Urban sites had notably higher∑PAHs and TEQ concentrations than suburban sites,attributed to increased vehicular traffic and coal combustion in urban areas.PMF results showed that traffic emissions(32.7%-60.5%),coal combustion(13.9%-24.3%)and secondary formation(14.7%-22.7%)were the primary contributors to∑PAHs.Urban sites experienced a greater influence from traffic,while suburban sites were more impacted by coal and biomass burning.On polluted days,traffic sources’contributions increased significantly at HC,YNE,NG and YNCE sites,and secondary formation sources’contributions grew at CTV and YNCE sites.The sourcedependent BaPeq results underscored the role of secondary-formed PAH derivatives in TEQ.
基金supported by the National Key Research and Development Program of China(No.2019YFC1804501)the National Natural Science Foundation of China(Nos.22036007 and 22122611)+1 种基金the Natural Science Foundation of Shandong Province(No.ZR2020ME228)the Introduction and Cultivation Plan for Young Innovative Talents of Colleges and Universities.
文摘This study investigated environmental distribution and human exposure of polycyclic aromatic hydrocarbons(PAHs)and their derivatives in one Chinese petroleum refinery facility.It was found that,following with high concentrations of 16 EPA PAHs(∑Parent-PAHs)in smelting subarea of studied petroleum refinery facility,total derivatives of PAHs[named as XPAHs,including nitro PAHs(NPAHs),chlorinated PAHs(Cl-PAHs),and brominated PAHs(Br-PAHs)]in gas(mean=1.57×10^(4)ng/m^(3)),total suspended particulate(TSP)(mean=4.33×10^(3) ng/m^(3))and soil(mean=4.37×10^(3) ng/g)in this subarea had 1.76-6.19 times higher levels than those from other subareas of this facility,surrounding residential areas and reference areas,indicating that petroleum refining processes would lead apparent derivation of PAHs.Especially,compared with those in residential and reference areas,gas samples in the petrochemical areas had higher∑NPAH/∑PAHs(mean=2.18),but lower∑Cl-PAH/∑PAHs(mean=1.43×10^(-1))and∑Br-PAH/∑PAHs ratios(mean=7.49×10^(-2)),indicating the richer nitrification of PAHs than chlorination during petrochemical process.The occupational exposure to PAHs and XPAHs in this petroleum refinery facility were 24-343 times higher than non-occupational exposure,and the ILCR(1.04×10^(-4))for petrochemical workers was considered to be potential high risk.Furthermore,one expanded high-resolution screening through GC Orbitrap/MS was performed for soils from petrochemical area,and another 35 PAHs were found,including alkyl-PAHs,phenyl-PAHs and other species,indicat-ing that profiles and risks of PAHs analogs in petrochemical areas deserve further expanded investigation.
