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
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
Microalgae can effectively degrade polycyclic aromatic hydrocarbons (PAHs) in water.However,the remediation mechanism of microalgae in PAH-contaminated soil remains unclear.In this study,the growth-promoting effects o...Microalgae can effectively degrade polycyclic aromatic hydrocarbons (PAHs) in water.However,the remediation mechanism of microalgae in PAH-contaminated soil remains unclear.In this study,the growth-promoting effects of wheat by Chlorella vulgaris in PAH-contaminated soil were studied.Structural changes in the rhizosphere bacterial community and the bacterial metabolism were further explored.It revealed that the addition of C.vulgaris promoted wheat’s dry weight and height by 10.22% and 122.15%,respectively.One explanation was the degradation and transformation of PAHs by C.vulgaris,which relieved the inhibitory effect on wheat growth.Compared with the blank control group,C.vulgaris addition enhanced the degradation efficiencies of phenanthrene (Phe) and pyrene (Pry) by 4.81% and 8.34%,respectively (with the initial concentrations in soil of 1.03×10^(4) and 2.21×10^(4)μg/g,respectively).The binding state of Phe and Pyr changed to a free state,which facilitated microbial degradation.The Phe and Pyr contents in wheat decreased by 22.23% and 18.54%,respectively.The presence of C.vulgaris increased the abundance of Sphingosinomonas bacteria capable of degrading PAHs by 95.24%.Enzyme activities related to the transport,oxidation,and dehydrogenation of PAHs in the bacterial community also increased.This study demonstrated C.vulgaris’multiple pathways for remediating PAH-polluted soil,including PAH degradation,nutrient and hormone release,and bacterial community adjustment.In conclusion,C.vulgaris addition enhanced the algae-bacteria symbiosis,which was of great significance for the removal of PAHs from the soil and the promotion of plant growth.展开更多
The Yellow River Delta(YRD)is rich in oil,natural gas,and land resources.With the expansion of an important oil production base in North China,the increased discharge of Polycyclic aromatic hydrocarbons(PAHs)and alkyl...The Yellow River Delta(YRD)is rich in oil,natural gas,and land resources.With the expansion of an important oil production base in North China,the increased discharge of Polycyclic aromatic hydrocarbons(PAHs)and alkylated/nitrated/oxygenated PAHs(APAHs/NPAHs/OPAHs)into the Yellow River poses a potential risk to the aquatic ecosystem and human health.A total of 42 samples were gathered from trunk streams and tributaries within the YRD region during the wet and dry seasons,and 19 PAHs,5 APAHs,16 NPAHs,and 7 OPAHswere measured.The concentrations of ƩPAHs,ƩAPAHs,ƩNPAHs and ƩOPAHs ranged between 29 and 620 ng/L,6.9–81 ng/L,0.64–9.0 ng/L,and 7.2–81 ng/L in water,respectively,and 27–420 ng/g,5.1–130 ng/g,0.19–1.8 ng/g and 3.9–51 ng/g in sediment,respectively.The oil extraction activities resulted in an increased presence of middle-high molecular weight PAHs and APAHs in sediment,and port activities had a notable influence on the proportion of 1-methylpyrene in both water and sediment.The fugacity fraction analysis suggested that sediment was a secondary source of OPAHs,while benzo[k]fluoranthene,benzo[e]pyrene,benzo[a]pyrene,and 5-methylchrysene migrated from water to sediment.The main contributors to PAHs,APAHs,NPAHs,and OPAHs in water and sediment were combustion and petroleum sources.Compared to water,sediment displayed a heightened ecological risk associated with PAHs,APAHs,NPAHs,and OPAHs.Adults residing in the YRD region were at higher risk of cancer than children,which deserves special attention.展开更多
The coating material is considered as the key of solid-phase microextraction(SPME)due to the fact that which has much effect on the selectivity and sensitivity of the analytical method.Herein,the porous hollow carbon ...The coating material is considered as the key of solid-phase microextraction(SPME)due to the fact that which has much effect on the selectivity and sensitivity of the analytical method.Herein,the porous hollow carbon nanospheres(PHCNs)were synthesized by selectively removing the interior part of solid inhomogeneous nanospheres with acetone.Using PHCNs as new coating material,a SPME fiber was prepared.To the best of our knowledge,PHCNs was utilized as a SPME fiber coating for the first time.The fiber coating material PHCNs demonstrated excellent thermal stability(>800℃)and long usage lifespan(≥60 times).A headspace SPME(HS-SPME)was established to non-contact extract and enrich polycyclic aromatic hydrocarbons(PAHs)prior to gas chromatography-flame ionization detector(GC-FID)analysis.The HS-SPME not only can eliminate non-volatile interferences from matrix,but also be able to protect fiber coating and prolong lifespan of fiber prober.The linearity in the linear range of 0.01-30 ng/m L and limits of detection from 0.003 ng/mL to 0.006 ng/mL were obtained by HS-SPME-GC-FID with PHCNs as fiber coating.The enrichment factors were calculated as 5420-9211 compared with conventional direct introduce analysis.The spiked recoveries of real samples including campus lake water and lime tree honey were obtained from 80.93%to 118.0%with relative standard deviation no higher than 10.6%.The π-π stacking interaction,CH/π interaction,and unique built-in cavities significantly enhance the extraction performance of PHCNs coating fiber to PAHs.This work demonstrated that the PHCNs as fiber coating materials present good application prospects for the extraction and enrichment of trace PAHs from complex matrixes.展开更多
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.
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 Natural Science Foundation of China (Nos.U24A20613 and 52370043)China National Funds for Distinguished Young Scientists (No.51925803)。
文摘Microalgae can effectively degrade polycyclic aromatic hydrocarbons (PAHs) in water.However,the remediation mechanism of microalgae in PAH-contaminated soil remains unclear.In this study,the growth-promoting effects of wheat by Chlorella vulgaris in PAH-contaminated soil were studied.Structural changes in the rhizosphere bacterial community and the bacterial metabolism were further explored.It revealed that the addition of C.vulgaris promoted wheat’s dry weight and height by 10.22% and 122.15%,respectively.One explanation was the degradation and transformation of PAHs by C.vulgaris,which relieved the inhibitory effect on wheat growth.Compared with the blank control group,C.vulgaris addition enhanced the degradation efficiencies of phenanthrene (Phe) and pyrene (Pry) by 4.81% and 8.34%,respectively (with the initial concentrations in soil of 1.03×10^(4) and 2.21×10^(4)μg/g,respectively).The binding state of Phe and Pyr changed to a free state,which facilitated microbial degradation.The Phe and Pyr contents in wheat decreased by 22.23% and 18.54%,respectively.The presence of C.vulgaris increased the abundance of Sphingosinomonas bacteria capable of degrading PAHs by 95.24%.Enzyme activities related to the transport,oxidation,and dehydrogenation of PAHs in the bacterial community also increased.This study demonstrated C.vulgaris’multiple pathways for remediating PAH-polluted soil,including PAH degradation,nutrient and hormone release,and bacterial community adjustment.In conclusion,C.vulgaris addition enhanced the algae-bacteria symbiosis,which was of great significance for the removal of PAHs from the soil and the promotion of plant growth.
基金supported by the Natural Science Foundation of Qingdao(No.23-2-1-224-zyyd-jch).
文摘The Yellow River Delta(YRD)is rich in oil,natural gas,and land resources.With the expansion of an important oil production base in North China,the increased discharge of Polycyclic aromatic hydrocarbons(PAHs)and alkylated/nitrated/oxygenated PAHs(APAHs/NPAHs/OPAHs)into the Yellow River poses a potential risk to the aquatic ecosystem and human health.A total of 42 samples were gathered from trunk streams and tributaries within the YRD region during the wet and dry seasons,and 19 PAHs,5 APAHs,16 NPAHs,and 7 OPAHswere measured.The concentrations of ƩPAHs,ƩAPAHs,ƩNPAHs and ƩOPAHs ranged between 29 and 620 ng/L,6.9–81 ng/L,0.64–9.0 ng/L,and 7.2–81 ng/L in water,respectively,and 27–420 ng/g,5.1–130 ng/g,0.19–1.8 ng/g and 3.9–51 ng/g in sediment,respectively.The oil extraction activities resulted in an increased presence of middle-high molecular weight PAHs and APAHs in sediment,and port activities had a notable influence on the proportion of 1-methylpyrene in both water and sediment.The fugacity fraction analysis suggested that sediment was a secondary source of OPAHs,while benzo[k]fluoranthene,benzo[e]pyrene,benzo[a]pyrene,and 5-methylchrysene migrated from water to sediment.The main contributors to PAHs,APAHs,NPAHs,and OPAHs in water and sediment were combustion and petroleum sources.Compared to water,sediment displayed a heightened ecological risk associated with PAHs,APAHs,NPAHs,and OPAHs.Adults residing in the YRD region were at higher risk of cancer than children,which deserves special attention.
基金supported by National Natural Science Foundation of China(No.22376053)supported by the Natural Science Foundation of Henan Province,China(No.242300421034)Henan Key Scientific Research Programs to Universities and Colleges(No.22ZX003)。
文摘The coating material is considered as the key of solid-phase microextraction(SPME)due to the fact that which has much effect on the selectivity and sensitivity of the analytical method.Herein,the porous hollow carbon nanospheres(PHCNs)were synthesized by selectively removing the interior part of solid inhomogeneous nanospheres with acetone.Using PHCNs as new coating material,a SPME fiber was prepared.To the best of our knowledge,PHCNs was utilized as a SPME fiber coating for the first time.The fiber coating material PHCNs demonstrated excellent thermal stability(>800℃)and long usage lifespan(≥60 times).A headspace SPME(HS-SPME)was established to non-contact extract and enrich polycyclic aromatic hydrocarbons(PAHs)prior to gas chromatography-flame ionization detector(GC-FID)analysis.The HS-SPME not only can eliminate non-volatile interferences from matrix,but also be able to protect fiber coating and prolong lifespan of fiber prober.The linearity in the linear range of 0.01-30 ng/m L and limits of detection from 0.003 ng/mL to 0.006 ng/mL were obtained by HS-SPME-GC-FID with PHCNs as fiber coating.The enrichment factors were calculated as 5420-9211 compared with conventional direct introduce analysis.The spiked recoveries of real samples including campus lake water and lime tree honey were obtained from 80.93%to 118.0%with relative standard deviation no higher than 10.6%.The π-π stacking interaction,CH/π interaction,and unique built-in cavities significantly enhance the extraction performance of PHCNs coating fiber to PAHs.This work demonstrated that the PHCNs as fiber coating materials present good application prospects for the extraction and enrichment of trace PAHs from complex matrixes.
