Polycyclic aromatic hydrocarbons(PAHs)and their nitrated derivatives(NPAHs)attract continuous attention due to their outstanding carcinogenicity and mutagenicity.In order to investigate the diurnal variations,sources,...Polycyclic aromatic hydrocarbons(PAHs)and their nitrated derivatives(NPAHs)attract continuous attention due to their outstanding carcinogenicity and mutagenicity.In order to investigate the diurnal variations,sources,formation mechanism,and health risk assessment of them in heating season,particulate matter(PM)were collected in Beijing urban area from December 26,2017 to January 17,2018.PAHs and NPAHs in PM were quantitatively analyzed via gas chromatography-mass spectrometry(GC-MS).Average daily concentrations of PAHs and NPAHs were(78±54)ng/m^(3)and(783±684)pg/m^(3),respectively.The concentrations of them were significantly higher at nighttime than at daytime,and NPAHs concentrations were 1-2 orders of magnitude lower than PAHs concentrations.In the heating season,the dominant species of PAHs include benzo[b]fluoranthene,fluoranthene,pyrene,and chrysene,while 9-nitroanthracene,2+3-nitrofluoranthene,and 2-nitropyrene were dominant species for NPAHs.NPAHs were found to have a single peak during heating and to be primarily distributed in the 0.4-0.7μm particle size.Primary emissions such as biomass burning,coal combustion,and traffic emissions were the major sources of PAHs.NPAHs were produced by the primary source of vehicle emissions and the secondary reaction triggered by OH radicals,as well as biomass burning during daytime.According to the health risk assessment,the total carcinogenic risk was higher in adults than in children.While upon oral ingestion,the carcinogenic risk in children was higher than that of adults,but the risk of adults was higher than children through skin contact and respiratory inhalation.展开更多
Nitrated polycyclic aromatic hydrocarbons(NPAHs)have toxic potentials that are higher than those of their corresponding parent polycyclic aromatic hydrocarbons(PAHs)and thus have received increasing attention in recen...Nitrated polycyclic aromatic hydrocarbons(NPAHs)have toxic potentials that are higher than those of their corresponding parent polycyclic aromatic hydrocarbons(PAHs)and thus have received increasing attention in recent years.In this study,the occurrence,distribution,source,and human health risk assessment of 15 NPAHs and 16 PAHs were investigated in the surface water from 20 sampling sites of Lake Taihu during the dry,normal,and flood seasons of 2018.The PAH concentrations ranged from 255 to 7298 ng/L and the NPAH concentrations ranged from not-detected(ND)to 212 ng/L.Among the target analytes,2-nitrofluorene(2-n Flu)was the predominant NPAH,with a detection frequency ranging from 85%to 90%and a maximum concentration of 56.2 ng/L.The three-ringed and four-ringed NPAHs and PAHs comprised the majority of the detected compounds.In terms of seasonal variation,the highest levels of the NPAHs and PAHs were in the dry season and flood season,respectively.Diagnostic ratio analysis indicated that the prime source of NPAHs was direct combustion,whereas in the case of PAHs the contribution was predominantly from a mixed pattern including pollution from unburned petroleum and petroleum combustion.The human health risk of NPAHs and PAHs was evaluated using a lifetime carcinogenic risk assessment model.The carcinogenic risk level of the targets ranged from 2.09×10^(-7)to 5.75×10^(-5)and some surface water samples posed a potential health risk.展开更多
Intensive daytime and nighttime sampling was carried out from 23 Oct to 31 Dec 2008 to investigate the occurrence of nitrated polycyclic aromatic hydrocarbons （NPAHs） in PM1o at a roadside site in Xiamen, China. At ...Intensive daytime and nighttime sampling was carried out from 23 Oct to 31 Dec 2008 to investigate the occurrence of nitrated polycyclic aromatic hydrocarbons （NPAHs） in PM1o at a roadside site in Xiamen, China. At the same time, six PMt0 samples were collected from a nearby roadway tunnel for comparison. Six NPAHs, namely 9-nitroanthracene, 2- and 3-nitrofluoranthene, 1- nitropyrene, 7-nitrobenz[a]anthracene, and 6-nitrobenzo[a]pyrene, were identified and quantified using GC/MS in negative ion chemical ionization mode. The average total concentration of six NPAHs （~NPAHs） in the cold season （26 Nov-31 Dec） was 2.3 （daytime） and 9.9 （nighttime） times higher than those in the warm season. Significant statistical difference （p 〈 0.01, 2-tailed） of ∑NPAHs between daytime and nighttime was found during both the warm and cold seasons. NPAHs were significantly positively correlated with their parent PAHs and nitrogen dioxide but negatively correlated with ambient temperature. The ratio of 2 ＋ 3-nitrofluoranthene to 1- nitropyrene exhibited a similar diurnal pattern as ZNPAHs and was generally greater than 5, indicating the importance of secondary atmospheric formation. The diurnal variations of NPAHs were all influenced by the diurnal variations of PAHs, nitrogen dioxide, sunlight, and temperature. The daily inhalable exposure to the six NPAHs in the tunnel was much higher than the roadside values in the warm season but only slightly higher than those in the cold season.展开更多
The direct cleavage of C–NO_(2)bonds for reductive denitration of nitroarenes remains a challenging transformation in synthetic organic chemistry.Herein,we report a biocompatible palladium-deposited graphdiyne nanoca...The direct cleavage of C–NO_(2)bonds for reductive denitration of nitroarenes remains a challenging transformation in synthetic organic chemistry.Herein,we report a biocompatible palladium-deposited graphdiyne nanocatalyst(Pd@GDY/DSPE-PEG)that can catalyze reductive denitration of nitroarenes under ambient physiological conditions.Mechanistic studies support this transformation via the oxidative addition of nitroarenes with Pd(0)and subsequent ligand exchange to form arylpalladium hydride.This one-step reductive denitration via Pd@GDY/DSPE-PEG successfully facilitates the repair of the nitrated proteins arising from endogenic ONOO−and restores their physiological function,including blocking the apoptosis pathway in living cells.Moreover,Pd@GDY/DSPE-PEG was further successfully applied for catalytic denitration to reduce the level of 3-nitrotyrosine residues of proteins located in the mouse brain hippocampus in vivo.This study provides an ideal strategy for designing highly active enzymatic mimicking synthetic catalysts for the regulation of the nitrated protein level and the detoxification of nitrative damage of living cells and tissues.展开更多
Nitrated polycyclic aromatic hydrocarbons(NPAHs)are widespread organic pollutants that possess carcinogenic and mutagenic properties,so they may pose a risk to the environment and human health.In this study,the concen...Nitrated polycyclic aromatic hydrocarbons(NPAHs)are widespread organic pollutants that possess carcinogenic and mutagenic properties,so they may pose a risk to the environment and human health.In this study,the concentrations of 15 NPAHs and 16 polycyclic aromatic hydrocarbons(PAHs)in 30 surface water samples and 26 sediment samples were measured in 2018 from the Taige Canal,one of the main rivers flowing into Taihu Lake,China.The total NPAH concentrations in water and sediment ranged from 14.7 to 235 ng/L and 22.9 to 96.5 ng/g dw,respectively.9-nitrophenanthrene(nd–76.3 ng/L)was the dominant compound in surface water,while 2+3-nitrofluoranthene(1.73–18.1 ng/g dw)dominated in sediment.Among PAHs,concentration ranging from 1,097 to 2,981 ng/L and 1,089 to 4,489 ng/g dw in surface water and sediment,respectively.There was a strong positive correlation between the log octanol-water partition coefficient(Kow)and log sediment-water partition coefficient due to hydrophobic interaction.The fugacity fraction value increased with the decrease of log Kow,and chrysene was transferred from water into sediment.The residual NPAHs in surface water and sediment of the Taige Canal have partial correlation.Diesel engine and coal combustion emissions were probably the principal sources of NPAHs in surface water and sediment.The results of ecological risk assessment showed that some NPAHs inwater(e.g,1-nitropyrene and 6-nitrochrysene)and sediment(e.g.,2-nitrobiphenyl,5-nitroacenaphthene,9-nitrophenanthrene and 2+3-nitrofluoranthene)had moderate ecological risks,which should be of concern.展开更多
Methamphetamine is an amphetamine-type psychostimulant that can damage dopaminergic neurons and cause characteristic pathological changes similar to neurodegenerative diseases such as Parkinson's disease. However,...Methamphetamine is an amphetamine-type psychostimulant that can damage dopaminergic neurons and cause characteristic pathological changes similar to neurodegenerative diseases such as Parkinson's disease. However, its specific mechanism of action is still unclear. In the present study, we established a Parkinson's disease pathology model by exposing SH-SY5 Y cells and C57 BL/6 J mice to methamphetamine. In vitro experiments were performed with 0, 0.5, 1.0, 1.5, 2.0 or 2.5 mM methamphetamine for 24 hours or 2.0 mM methamphetamine for 0-, 2-, 4-, 8-, 16-, and 24-hour culture of SH-SY5 Y cells. Additional experimental groups of SH-SY5 Y cells were administered a nitric oxide inhibitor, 0.1 mM N-nitro-L-arginine, 1 hour before exposure to 2.0 mM methamphetamine for 24 hours. In vivo experiments: C57 BL/6 J mice were intraperitoneally injected with N-nitro-L-arginine(8 mg/kg), eight times, at intervals of 12 hours. Methamphetamine 15 mg/kg was intraperitoneally injected eight times, at intervals of 12 hours, but 0.5-hour after each N-nitro-L-arginine injection in the combined group. Western blot assay was used to determine the expression of nitric oxide synthase, α-synuclein(α-Syn), 5 G4, nitrated α-synuclein at the residue Tyr39(nT39 α-Syn), cleaved caspase-3, and cleaved poly ADP-ribose polymerase(PARP) in cells and mouse brain tissue. Immunofluorescence staining was conducted to measure the positive reaction of NeuN, nT39 α-Syn and 5 G4. Enzyme linked immunosorbent assay was performed to determine the dopamine levels in the mouse brain. After methamphetamine exposure, α-Syn expression increased; the aggregation of α-Syn 5 G4 increased; nT39 α-Syn, nitric oxide synthase, cleaved caspase-3, and cleaved PARP expression increased in the cultures of SH-SY5 Y cells and in the brains of C57 BL/6 J mice; and dopamine levels were reduced in the mouse brain. These changes were markedly reduced when N-nitro-L-arginine was administered with methamphetamine in both SH-SY5 Y cells and C57 BL/6 J mice. These results sugge展开更多
基金supported by the National Natural Science Foundation of China(No.41907197)the Fundamental Research Funds for Central Public Welfare Scientific Research Institutes of China,Chinese Research Academy of Environmental Sciences(No.2019YSKY-018)+1 种基金the National Key R&D Program of China(No.2019YFC0214800)the Standard System and Key Standards Research of National Ecological Environment Protection and Risk Prevention(No.2020YFC18063)。
文摘Polycyclic aromatic hydrocarbons(PAHs)and their nitrated derivatives(NPAHs)attract continuous attention due to their outstanding carcinogenicity and mutagenicity.In order to investigate the diurnal variations,sources,formation mechanism,and health risk assessment of them in heating season,particulate matter(PM)were collected in Beijing urban area from December 26,2017 to January 17,2018.PAHs and NPAHs in PM were quantitatively analyzed via gas chromatography-mass spectrometry(GC-MS).Average daily concentrations of PAHs and NPAHs were(78±54)ng/m^(3)and(783±684)pg/m^(3),respectively.The concentrations of them were significantly higher at nighttime than at daytime,and NPAHs concentrations were 1-2 orders of magnitude lower than PAHs concentrations.In the heating season,the dominant species of PAHs include benzo[b]fluoranthene,fluoranthene,pyrene,and chrysene,while 9-nitroanthracene,2+3-nitrofluoranthene,and 2-nitropyrene were dominant species for NPAHs.NPAHs were found to have a single peak during heating and to be primarily distributed in the 0.4-0.7μm particle size.Primary emissions such as biomass burning,coal combustion,and traffic emissions were the major sources of PAHs.NPAHs were produced by the primary source of vehicle emissions and the secondary reaction triggered by OH radicals,as well as biomass burning during daytime.According to the health risk assessment,the total carcinogenic risk was higher in adults than in children.While upon oral ingestion,the carcinogenic risk in children was higher than that of adults,but the risk of adults was higher than children through skin contact and respiratory inhalation.
基金supported by the National Natural Science Foundation of China(No.41671493)the State Key Laboratory of Pollution Control and Resource Reuse Foundation(No.PCRRF17030)the National Major Project of the Science and Technology Ministry of China(No.2017ZX07202-004 and 2017X07301002-3)。
文摘Nitrated polycyclic aromatic hydrocarbons(NPAHs)have toxic potentials that are higher than those of their corresponding parent polycyclic aromatic hydrocarbons(PAHs)and thus have received increasing attention in recent years.In this study,the occurrence,distribution,source,and human health risk assessment of 15 NPAHs and 16 PAHs were investigated in the surface water from 20 sampling sites of Lake Taihu during the dry,normal,and flood seasons of 2018.The PAH concentrations ranged from 255 to 7298 ng/L and the NPAH concentrations ranged from not-detected(ND)to 212 ng/L.Among the target analytes,2-nitrofluorene(2-n Flu)was the predominant NPAH,with a detection frequency ranging from 85%to 90%and a maximum concentration of 56.2 ng/L.The three-ringed and four-ringed NPAHs and PAHs comprised the majority of the detected compounds.In terms of seasonal variation,the highest levels of the NPAHs and PAHs were in the dry season and flood season,respectively.Diagnostic ratio analysis indicated that the prime source of NPAHs was direct combustion,whereas in the case of PAHs the contribution was predominantly from a mixed pattern including pollution from unburned petroleum and petroleum combustion.The human health risk of NPAHs and PAHs was evaluated using a lifetime carcinogenic risk assessment model.The carcinogenic risk level of the targets ranged from 2.09×10^(-7)to 5.75×10^(-5)and some surface water samples posed a potential health risk.
基金supported by the National Natural Science Foundation of China (No. 40971257,41171365)the Environmental Nonprofit Research and Special Project of China (No. 201009004)the Program for Changjiang Scholars and Innovative Research Team in University (No.IRT0941)
文摘Intensive daytime and nighttime sampling was carried out from 23 Oct to 31 Dec 2008 to investigate the occurrence of nitrated polycyclic aromatic hydrocarbons （NPAHs） in PM1o at a roadside site in Xiamen, China. At the same time, six PMt0 samples were collected from a nearby roadway tunnel for comparison. Six NPAHs, namely 9-nitroanthracene, 2- and 3-nitrofluoranthene, 1- nitropyrene, 7-nitrobenz[a]anthracene, and 6-nitrobenzo[a]pyrene, were identified and quantified using GC/MS in negative ion chemical ionization mode. The average total concentration of six NPAHs （~NPAHs） in the cold season （26 Nov-31 Dec） was 2.3 （daytime） and 9.9 （nighttime） times higher than those in the warm season. Significant statistical difference （p 〈 0.01, 2-tailed） of ∑NPAHs between daytime and nighttime was found during both the warm and cold seasons. NPAHs were significantly positively correlated with their parent PAHs and nitrogen dioxide but negatively correlated with ambient temperature. The ratio of 2 ＋ 3-nitrofluoranthene to 1- nitropyrene exhibited a similar diurnal pattern as ZNPAHs and was generally greater than 5, indicating the importance of secondary atmospheric formation. The diurnal variations of NPAHs were all influenced by the diurnal variations of PAHs, nitrogen dioxide, sunlight, and temperature. The daily inhalable exposure to the six NPAHs in the tunnel was much higher than the roadside values in the warm season but only slightly higher than those in the cold season.
基金support from the National Natural Science Foundation of China(grant nos.22021002,22020102005,and 22022705)the CAS-Croucher Funding Scheme for Joint Laboratories.
文摘The direct cleavage of C–NO_(2)bonds for reductive denitration of nitroarenes remains a challenging transformation in synthetic organic chemistry.Herein,we report a biocompatible palladium-deposited graphdiyne nanocatalyst(Pd@GDY/DSPE-PEG)that can catalyze reductive denitration of nitroarenes under ambient physiological conditions.Mechanistic studies support this transformation via the oxidative addition of nitroarenes with Pd(0)and subsequent ligand exchange to form arylpalladium hydride.This one-step reductive denitration via Pd@GDY/DSPE-PEG successfully facilitates the repair of the nitrated proteins arising from endogenic ONOO−and restores their physiological function,including blocking the apoptosis pathway in living cells.Moreover,Pd@GDY/DSPE-PEG was further successfully applied for catalytic denitration to reduce the level of 3-nitrotyrosine residues of proteins located in the mouse brain hippocampus in vivo.This study provides an ideal strategy for designing highly active enzymatic mimicking synthetic catalysts for the regulation of the nitrated protein level and the detoxification of nitrative damage of living cells and tissues.
基金supported by the National Natural Science Foundation of China (No. 41671493)the Natural Science Foundation of Jiangsu Province (No. BK20191372)the National Major Project of the Science and Technology Ministry of China (No. 2017ZX07202-004)
文摘Nitrated polycyclic aromatic hydrocarbons(NPAHs)are widespread organic pollutants that possess carcinogenic and mutagenic properties,so they may pose a risk to the environment and human health.In this study,the concentrations of 15 NPAHs and 16 polycyclic aromatic hydrocarbons(PAHs)in 30 surface water samples and 26 sediment samples were measured in 2018 from the Taige Canal,one of the main rivers flowing into Taihu Lake,China.The total NPAH concentrations in water and sediment ranged from 14.7 to 235 ng/L and 22.9 to 96.5 ng/g dw,respectively.9-nitrophenanthrene(nd–76.3 ng/L)was the dominant compound in surface water,while 2+3-nitrofluoranthene(1.73–18.1 ng/g dw)dominated in sediment.Among PAHs,concentration ranging from 1,097 to 2,981 ng/L and 1,089 to 4,489 ng/g dw in surface water and sediment,respectively.There was a strong positive correlation between the log octanol-water partition coefficient(Kow)and log sediment-water partition coefficient due to hydrophobic interaction.The fugacity fraction value increased with the decrease of log Kow,and chrysene was transferred from water into sediment.The residual NPAHs in surface water and sediment of the Taige Canal have partial correlation.Diesel engine and coal combustion emissions were probably the principal sources of NPAHs in surface water and sediment.The results of ecological risk assessment showed that some NPAHs inwater(e.g,1-nitropyrene and 6-nitrochrysene)and sediment(e.g.,2-nitrobiphenyl,5-nitroacenaphthene,9-nitrophenanthrene and 2+3-nitrofluoranthene)had moderate ecological risks,which should be of concern.
基金supported by the National Natural Science Foundation of China,No.81373240(to PMQ)and 81671865(to PMQ)
文摘Methamphetamine is an amphetamine-type psychostimulant that can damage dopaminergic neurons and cause characteristic pathological changes similar to neurodegenerative diseases such as Parkinson's disease. However, its specific mechanism of action is still unclear. In the present study, we established a Parkinson's disease pathology model by exposing SH-SY5 Y cells and C57 BL/6 J mice to methamphetamine. In vitro experiments were performed with 0, 0.5, 1.0, 1.5, 2.0 or 2.5 mM methamphetamine for 24 hours or 2.0 mM methamphetamine for 0-, 2-, 4-, 8-, 16-, and 24-hour culture of SH-SY5 Y cells. Additional experimental groups of SH-SY5 Y cells were administered a nitric oxide inhibitor, 0.1 mM N-nitro-L-arginine, 1 hour before exposure to 2.0 mM methamphetamine for 24 hours. In vivo experiments: C57 BL/6 J mice were intraperitoneally injected with N-nitro-L-arginine(8 mg/kg), eight times, at intervals of 12 hours. Methamphetamine 15 mg/kg was intraperitoneally injected eight times, at intervals of 12 hours, but 0.5-hour after each N-nitro-L-arginine injection in the combined group. Western blot assay was used to determine the expression of nitric oxide synthase, α-synuclein(α-Syn), 5 G4, nitrated α-synuclein at the residue Tyr39(nT39 α-Syn), cleaved caspase-3, and cleaved poly ADP-ribose polymerase(PARP) in cells and mouse brain tissue. Immunofluorescence staining was conducted to measure the positive reaction of NeuN, nT39 α-Syn and 5 G4. Enzyme linked immunosorbent assay was performed to determine the dopamine levels in the mouse brain. After methamphetamine exposure, α-Syn expression increased; the aggregation of α-Syn 5 G4 increased; nT39 α-Syn, nitric oxide synthase, cleaved caspase-3, and cleaved PARP expression increased in the cultures of SH-SY5 Y cells and in the brains of C57 BL/6 J mice; and dopamine levels were reduced in the mouse brain. These changes were markedly reduced when N-nitro-L-arginine was administered with methamphetamine in both SH-SY5 Y cells and C57 BL/6 J mice. These results sugge
