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1.
Chemosphere ; 240: 124898, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-31557644

RESUMO

Urinary polycyclic aromatic hydrocarbon (PAH) metabolites, biomarkers of internal PAH exposure, are commonly used to explore the effects of PAH on human health. However, the correlation between environmental PAH exposure and the species or levels of urinary PAH metabolites remains unclear. We collected detailed information on PAH exposure sources, including cigarette smoking, cooking, traffic and diet habits via structured questionnaires, and determined 12 urinary monohydroxylated PAH metabolites (OH-PAHs) among 4092 participants from the Wuhan-Zhuhai cohort. Linear mixed models and generalized linear models were conducted to explore the associations of urinary metabolite levels with single or multiple PAH exposure sources. We also calculated the standardized regression coefficients to further compare the contributions of different sources to urinary OH-PAH levels. Our results showed that increasing levels of urinary 1-, 2-hydroxynaphthalene (1-, 2- OHNa) and 2-hydroxyfluorene (2-OHFlu) were significantly correlated with tobacco smoking (all P < 0.01). The concentrations of 1-, 2- OHNa and 9-hydroxyfluorene (9-OHFlu) were positively correlated with dietary intake (all P < 0.05). Individuals who spent a long time in traffic showed elevated levels of 9-OHFlu and 1-hydroxyphenanthrene (1-OHPh) compared with individuals who spent a short time in traffic (all P < 0.05). Self-cooking was associated only with elevated 1-hydroxypyrene (1-OHP) levels. Moreover, good kitchen ventilation resulted in significantly decreased urinary low-molecular-weight OH-PAH levels. These findings suggested that cigarette smoking, self-cooking, high dietary PAH intake and a long time spent in traffic were associated with increased levels of specific urinary PAH metabolites, and good kitchen ventilation effectively reduced the exposure to low-molecular-weight PAHs in self-cooking participants.


Assuntos
Exposição Ambiental/análise , Poluentes Ambientais/urina , Hidrocarbonetos Policíclicos Aromáticos/urina , Adulto , Biomarcadores/urina , China , Estudos de Coortes , Estudos Transversais , Exposição Ambiental/estatística & dados numéricos , Feminino , Fluorenos , Humanos , Estilo de Vida , Modelos Lineares , Pulmão/metabolismo , Masculino , Naftóis , Fenantrenos
2.
Chemosphere ; 237: 124525, 2019 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31549648

RESUMO

Monohydroxylated polycyclic aromatic hydrocarbons (OH-PAHs), present in human urine at trace concentrations (viz. from ng L-1 to µg L-1), are considered the main biomarkers of human exposure to PAHs. In this work, we report a simple and high-throughput sample treatment platform to facilitate the biomonitoring of OH-PAHs by making it easier, greener and most cost-effective. This platform is based on the integration of analyte extraction and sample cleanup in a single step by the use of supramolecular solvents with restricted access properties (SUPRAS-RAM). The SUPRAS was spontaneously formed in situ in the urine by the addition of a colloidal suspension of decanoic acid in THF. Metabolites from naphthalene, fluorene, phenanthrene and pyrene were quantitatively extracted (absolute recoveries in the range 91-109%). Polysaccharides and proteins in the urine were excluded from extraction by physical and chemical mechanisms, which allowed the direct analysis of the SUPRAS extract by liquid chromatography tandem mass spectrometry. Absolute matrix effects for OH-PAHs were in the range 92-103%. Method quantification limits for OH-PAHs, without the need for evaporation of the SUPRAS extracts, were in the interval 1.0-6.7 ng L-1. The precision, evaluated in terms of repeatability and reproducibility, varied between 1.1 and 13.8%. The method was successfully applied to the analysis of urine from 16 smoking and non-smoking volunteers. Both analytical and operational features of this method make it suitable to evaluate human exposure to PAHs.


Assuntos
Poluentes Ambientais/urina , Hidrocarbonetos Policíclicos Aromáticos/urina , Cromatografia Líquida/métodos , Humanos , Hidrocarbonetos Policíclicos Aromáticos/análise , Reprodutibilidade dos Testes , Solventes/análise , Espectrometria de Massas em Tandem/métodos
3.
Ecotoxicol Environ Saf ; 183: 109500, 2019 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-31450033

RESUMO

Exposure to diesel engine exhaust (DEE) impairs lung function. But the underlying mechanisms are still not fully understood. The aim of this study was to investigate the effects of long-term DEE exposure on lung inflammation and the underlying mechanisms. Sprague-Dawley male rats were exposed to DEE with 3 mg/m3 of diesel exhaust particles (DEP) for 12 weeks. Then urine, blood, bronchoalveolar lavage fluid (BALF), and lung tissue were collected for the determination of biochemistry indexes, DNA methylation status, and histological changes in the lung. The results showed that the metabolites of polycyclic aromatic hydrocarbons (PAHs) 2-hydroxyphenanthrene (2-OHPh) and 9-OHPh, and 8-hydroxy-2'-deoxyguanosine (8-OHdG), and malondialdehyde (MDA) level were higher in urine of DEE-exposed rats than control group. The level of proinflammatory cytokines IL-8, IL-6, and TNF-α was significantly higher in serum (1.8, 3.5, and nearly 1.0-fold increase, respectively), BALF (2.2, 3.8, and 2.0-fold increase, respectively) and lung tissues (3.5, 4.3, and 2.4-fold increase, respectively) of DEE-exposed rats than control group. While the level of clara cell secretory protein (CC16) and pulmonary surfactant protein D (SP-D) with anti-inflammatory property was obviously lower in serum (reduction of 29% and 38%, respectively), BALF (reduction of 50% and 46%, respectively) and lung tissues (reduction of 50% and 55%, respectively) of DEE-exposed rats than control group. Exposure to DEE also resulted in significant increases in total white blood cell (WBC), neutrophil, eosinophil, and lymphocyte number in BALF. Airway inflammation and remolding were apparent in DEE group. The methylation level of CCAAT/enhancer-binding protein alpha (C/EBPα) promoter was markedly increased (about 3.2-fold increase), and its mRNA and protein expression were significantly decreased (about 62% and 68% decrease, respectively) in the lungs of DEE-exposed rats compared with the group. Further, cell experiments were performed to investigate the relationship between C/EBPα and CC16, and CC16 function under DEP conditions. The results showed that DEP inhibited CC16 expression via methylation of C/EBPα promoter, and the increase of CC16 level significantly relieved the proinflammatory effects caused by DEP exposure. In conclusion, our data indicated that long-term exposure to DEE can cause lung inflammation, at least in part via methylation of C/EBPα promoter, and inhibition of CC16 expression.


Assuntos
Proteína alfa Estimuladora de Ligação a CCAAT/genética , Exposição por Inalação/efeitos adversos , Pneumonia/induzido quimicamente , Emissões de Veículos/toxicidade , Animais , Citocinas/metabolismo , Metilação de DNA/efeitos dos fármacos , Masculino , Pneumonia/metabolismo , Pneumonia/patologia , Hidrocarbonetos Policíclicos Aromáticos/urina , Regiões Promotoras Genéticas , RNA Mensageiro/metabolismo , Ratos Sprague-Dawley , Uteroglobina/genética , Uteroglobina/metabolismo
4.
Environ Health Prev Med ; 24(1): 50, 2019 Jul 27.
Artigo em Inglês | MEDLINE | ID: mdl-31351468

RESUMO

Polycyclic aromatic hydrocarbons (PAHs) are widely found in the environment, and comparing to adults, children are more vulnerable to PAHs exposure. Urinary metabolites of PAHs are used as preferred biomarkers to estimate the PAHs exposure. Systematic review on the internal exposure level of children and adolescents is rare. We aimed to calculate the internal exposure levels of PAHs in children and adolescents and compare the levels of PAHs internal exposure in various children groups. We searched PubMed, OVID, Web of Science, EBSCO, ACS, and four Chinese databases, and all studies examining the urinary concentrations of PAHs in children and adolescent were identified. The total exposure level of 11 PAHs metabolites were pooled. Standard mean difference (SMD) and 95% confidence intervals (CIs) of PAHs urinary concentration were calculated and pooled by RevMan5.3 to compare the exposure levels of different children groups. We found that 1-OHPyr, 2-OHNap, 2-OHFlu, 3-OHPhe, and 4-OHPhe were five PAHs metabolites most commonly studied in existing studies in children, and their total exposure levels were 0.38 ± 0.98, 2.32 ± 4.83, 0.81 ± 1.54, 0.09 ± 0.14, 0.03 ± 0.10 µmol/mol creatinine, respectively. The meta-analysis showed that the levels of 1-OHPyr were higher in higher environmental exposure group (SMD = 0.21, 95% CI = 0.03~0.40), ETS exposure group (SMD = 0.31, 95% CI = 0.08~0.54), and 6~11 years group (SMD = 0.16, 95% CI = 0.09~0.24); the level of 2-OHNap (SMD = 0.27, 95% CI = 0.01~0.53) was higher in higher environmental exposure group; however, the levels of 3-OHPhe (SMD = - 0.34, 95% CI = - 0.57~- 0.12) and 4-OHPhe (SMD = - 0.48, 95% CI = - 0.69~- 0.28) were higher in lower environmental exposure group. The levels of 1-OHPyr (SMD = - 0.01, 95% CI = - 0.11~0.10) and 2-OHNap (SMD = 0.01, 95% CI = - 0.20~0.22) were not statistically different between boys and girls. In conclusions, we found that the internal diversity of PAHs existed in children and adolescents, and the level of 1-OHPyr in children and adolescents was in higher status compared with non-occupational people who do not smoke.


Assuntos
Exposição Ambiental/análise , Hidrocarbonetos Policíclicos Aromáticos/urina , Adolescente , Biomarcadores/urina , Criança , Feminino , Humanos , Masculino
5.
Ecotoxicol Environ Saf ; 182: 109384, 2019 Oct 30.
Artigo em Inglês | MEDLINE | ID: mdl-31272023

RESUMO

Exposure to polycyclic aromatic hydrocarbons (PAHs) and phthalates link to oxidative stress and inflammatory response, which exert cellular aging. However, modification effect of seasonal factor on the association of PAHs or phthalates exposure with relative telomere length (RTL) or mitochondrial DNA copy number (mtDNA-CN) has remained unclear. In this pilot study, 106 subjects were from an urban population (n = 1240) who lived in the two districts in Wuhan city, China. Participants completed physical examinations and provided 191 blood samples for RTL and mtDNA-CN analysis and 627 urine samples for monohydroxylated-PAHs (OH-PAHs) and phthalate metabolites measurements in the winter and summer seasons. We assessed the associations of urinary OH-PAHs or phthalates metabolites with RTL or mtDNA-CN by linear regression analysis and linear mixed-effect models. We found that urinary OH-PAHs were positively associated with mtDNA-CN at lag 2 day and 3-day moving average, but negatively related to RTL at lag 0, lag 1 and lag 2 day and 3-day moving average (p < 0.05). Urinary phthalate metabolites were negatively associated with mtDNA lag 0, lag 1 and lag 2 day and 3-day moving average, but positively related to RTL at lag 0 day (p < 0.05). Seasonal factor modified the association of urinary OH-PAHs with mtDNA-CN as well as urinary phthalate metabolites with RTL. In vitro experiment showed that under certain conditions, benzo[a]pyrene increased mtDNA-CN at 48 h and di (2-ethylhexyl) phthalate did RTL at 24 h in HepG2 cells. Seasonal variations in the metabolisms of PAHs or phthalates in human body may affect the relation of PAHs or phthalates exposure with cellular aging.


Assuntos
Senescência Celular/efeitos dos fármacos , Variações do Número de Cópias de DNA/efeitos dos fármacos , DNA Mitocondrial/sangue , Ácidos Ftálicos/toxicidade , Hidrocarbonetos Policíclicos Aromáticos/toxicidade , Telômero/efeitos dos fármacos , Adulto , Senescência Celular/genética , China , Células Hep G2 , Humanos , Masculino , Estresse Oxidativo/efeitos dos fármacos , Estresse Oxidativo/genética , Ácidos Ftálicos/urina , Projetos Piloto , Hidrocarbonetos Policíclicos Aromáticos/urina , Estações do Ano , Adulto Jovem
6.
Environ Sci Pollut Res Int ; 26(26): 27281-27290, 2019 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-31325095

RESUMO

Exposure to polycyclic aromatic hydrocarbons (PAHs) during pregnancy may pose adverse health risk to both the mothers and babies. In the present study, 188 pregnant women of different trimesters were recruited in Guangzhou, south China, and nine hydroxyl PAHs (OH-PAHs) and a biomarker of DNA oxidative damage, 8-hydroxy-2'-deoxyguanosine (8-OHdG), were determined in their urine samples. All OH-PAHs except for 4-hydroxyphenanthrene and 6-hydroxychrysene were found in > 90% samples, with total concentration in the range of 0.52 to 42.9 µg/g creatinine. In general, concentration levels of OH-PAHs in pregnant women were lower than those in general population in the same research area but with higher levels in working women than in housewives. The mean daily intakes of PAHs from dietary estimated by urinary OH-PAHs were 0.021, 0.004, 0.047, and 0.030 µg/kg_bw/day for naphthalene, fluorene, phenanthrene, and pyrene, respectively, which were much lower than the reference doses (20, 30, and 40 µg/kg_bw/day for naphthalene, pyrene, and fluorene, respectively) derived from chronic oral exposure data by the United States Environmental Protection Agency. The low exposure levels of PAHs may be attributed to the traditional dietary taboo of Chinese pregnant women, which is to minimize the consumption of "toxic" food. The concentrations of 8-OHdG (4.67-49.4 µg/g creatinine) were significantly positively correlated with concentrations of several OH-PAHs, such as metabolites of naphthalene, fluorene, and phenanthrene (r = 0.3-0.6). In addition, the concentrations of 8-OHdG were higher in working women than in housewives when exposed to the same levels of PAHs, partly indicating the possible relation between work-related pressure for working women and the oxidative stress.


Assuntos
/química , Biomarcadores/química , Dano ao DNA/genética , Naftalenos/química , Fenantrenos/química , Hidrocarbonetos Policíclicos Aromáticos/análise , Hidrocarbonetos Policíclicos Aromáticos/metabolismo , Pirenos/química , Adulto , Biomarcadores/metabolismo , China , Poluentes Ambientais/urina , Feminino , Humanos , Estresse Oxidativo , Hidrocarbonetos Policíclicos Aromáticos/urina , Gravidez
7.
Int J Occup Environ Med ; 10(3): 124-136, 2019 07.
Artigo em Inglês | MEDLINE | ID: mdl-31325295

RESUMO

BACKGROUND: Coke oven workers are exposed to polycyclic aromatic hydrocarbons (PAHs) with possible genotoxicity and carcinogenicity. Metabolizing enzymes genes and DNA repair genes are suspected to be correlated with the level of DNA damage. They may contribute to variable individual sensitivity to DNA damage induced by PAHs exposure at workplace. OBJECTIVE: To investigate the relationship between biomarkers of PAHs: 1-hydroxypyrene (1-OHP), DNA adducts, and 8-hydroxy-2-deoxyguanosine (8-OHdG) in coke oven workers, and to assess the role of cytochrome P2E1 (CYP2E1) gene expression and DNA repairing gene (XRCC1) polymorphism in detecting workers at risk. METHODS: 85 exposed workers and 85 unexposed controls were enrolled into this study. Urinary 1-OHP, 8-OHdG, and BPDE-DNA adduct were measured. CYP2E1 gene expression and genotyping of XRCC1 399 Arg/Gln were evaluated by real-time PCR. RESULTS: The median urinary 1-OHP levels (6.3 µmol/mol creatinine), urinary 8-OHdG (7.9 ng/mg creatinine), DNA adducts (6.7 ng/µg DNA) in the exposed group were significantly higher than those in the unexposed group. Carriers of the variant allele (Gln) of XRCC1 had the highest levels of 1-OHP, DNA adducts and 8-OHdG, and the lowest level of CYP2E1 gene expression. In exposed workers, significant positive correlations were found between 1-OHP level and each of the work duration, 8-OHdG, and DNA adducts levels. There was a significant negative correlation between 1-OHP level and CYP2E1 gene expression. Work duration and CYP2E1 gene expression were predictors of DNA adducts level; 1-OHP level and work duration were predictors of urinary 8-OHdG level. CONCLUSION: Workers with higher exposure to PAH were more prone to oxidative DNA damage and cancer development. DNA adducts level reflects the balance between their production by CYP2E1 and elimination by XRCC1 gene.


Assuntos
Citocromo P-450 CYP2E1/genética , Adutos de DNA/genética , Desoxiguanosina/análogos & derivados , Monitoramento Ambiental/métodos , Exposição Ocupacional/análise , Pirenos/urina , Proteína 1 Complementadora Cruzada de Reparo de Raio-X/genética , 7,8-Di-Hidro-7,8-Di-Hidroxibenzo(a)pireno 9,10-óxido , Adulto , Biomarcadores/urina , Coque , Citocromo P-450 CYP2E1/biossíntese , Adutos de DNA/urina , Dano ao DNA/efeitos dos fármacos , Reparo do DNA/genética , Desoxiguanosina/urina , Egito , Humanos , Masculino , Pessoa de Meia-Idade , Hidrocarbonetos Policíclicos Aromáticos/urina , Polimorfismo Genético , Medição de Risco , Proteína 1 Complementadora Cruzada de Reparo de Raio-X/biossíntese , Adulto Jovem
8.
Sci Total Environ ; 685: 723-728, 2019 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-31234134

RESUMO

Metabolites of polycyclic aromatic hydrocarbons measured in human samples are often used as biomarkers of exposure to diesel engine exhaust (DEE). The aim of this study was to assess the changes in urinary levels of 1-aminopyrene (1-AP) and 1-hydroxypyrene (1-OHP) and their relationship with Elemental Carbon (EC), as a component of diesel engine exhaust exposure, among a hard-rock gold-mining population. Urine samples were collected at the beginning and end of a 12-hour work shift from 100 underground and above ground gold miners. Miners were fitted with personal exposure monitoring equipment to quantify exposure to DEE, measured as Elemental Carbon (EC), across their 12-hour work shift. General linear regression assessed associations of the post-shift urinary 1-AP and 1-OHP concentrations with EC, controlling for age, gender, the pre-shift biomarker level, Body Mass Index (BMI), days on current shift, time in mining, smoking status and second-hand smoke exposure. The concentrations of 1-AP and 1-OHP increased significantly across a 12-hour mining work shift. Moreover, consistent with the sensitivity analysis, the concentration of 1-AP was significantly associated with EC after adjustments. Urinary 1-OHP, but not 1-AP was significantly associated with current smoking. Urinary 1-AP may be a more robust and specific biomarker of DEE than 1-OHP.


Assuntos
Poluentes Ocupacionais do Ar/urina , Exposição Ocupacional/estatística & dados numéricos , Hidrocarbonetos Policíclicos Aromáticos/urina , Pirenos/urina , Biomarcadores/urina , Monitoramento Ambiental , Humanos , Masculino , Mineração , Emissões de Veículos
9.
Talanta ; 201: 271-279, 2019 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-31122423

RESUMO

In this work, an innovative aptamer-based magnetic adsorbent (Fe3O4@PDA-aptamer MNPs) was prepared by hydrothermal synthesis method followed by the surface functionalization of nanoparticles. After fixing in a steel stainless tube as sorbent of magnetic solid phase extraction (MSPE), an online magnetic solid phase extraction-high performance liquid chromatography-mass spectrometry (online-MSPE-HPLC-MS) method was developed and applied for the determination of 8-hydroxy-2'-deoxyguanosine (8-OHdG) and monohydroxylated polycyclic aromatic hydrocarbons (OH-PAHs) simultaneously in urine. The synthesized sorbent presented outstanding features, including large specific surface area, high enrichment capacity and excellent stability. High throughput analysis can be achieved by affinity-specific adsorption of 8-OHdG and non-specific adsorption of OH-PAHs at the same time. In addition, online MSPE can greatly simplify the analysis process, reduce human errors and enhance the sensitivity. When compared with offline MSPE, a sensitivity enhancement of 30-400 times was obtained for the online method. Some experimental parameters such as the amount of the sorbent, sampling flow rate and sample volume, were optimized systematically. Under the optimal conditions, the limits of detection (LOD) were in the range of 0.028-0.114 ng mL-1, and the correlation coefficients (R2) were higher than 0.9962. The relative standard deviations (RSDs) were less than 16.1% (n = 5) and the recoveries ranged from 71% to 116%. The above results show that the rapid, sensitive and automated online-MSPE-HPLC-MS method has potential application in the simultaneous determination of 8-OHdG and PAHs in complex sample matrix to assess the environmental exposure level.


Assuntos
Aptâmeros de Nucleotídeos/química , Desoxiguanosina/análogos & derivados , Hidrocarbonetos Policíclicos Aromáticos/urina , Extração em Fase Sólida/métodos , Adolescente , Adsorção , Adulto , Sequência de Bases , Cromatografia Líquida de Alta Pressão , Desoxiguanosina/urina , Humanos , Limite de Detecção , Nanopartículas de Magnetita/química , Espectrometria de Massas , Adulto Jovem
10.
Chemosphere ; 228: 166-173, 2019 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-31029962

RESUMO

Polycyclic aromatic hydrocarbons (PAHs) metabolites was related to heart rate variability (HRV) reduction and atherosclerotic cardiovascular disease (ASCVD), and ASCVD was also affected by HRV. However, the mediating role of HRV in the association between PAHs exposure and ASCVD risk was largely unknown. We aimed to investigate whether the relation of PAHs exposure with ASCVD risk was mediated by HRV among coke oven workers. A total of 1100 subjects with complete data were qualified in the current study. We measured 12 urinary PAHs metabolites by gas chromatography-mass spectrometry (GC-MS) and HRV indices by 3-channel digital Holter monitors. The associations between urinary PAHs metabolites, HRV indices, and ASCVD risk were explored using generalized linear models or multivariate logistic regression models. A mediation analysis was conducted to examine the role of HRV on the association between PAHs exposure and ASCVD risk. We found that urinary 1-hydroxynaphthalene (1-OHNa), 2-OHNa, and total PAH metabolites (ΣOH-PAH) were dose-responsive associated with increased risk of ASCVD. Compared with lowest quartile, the adjusted odds ratio (OR) for ASCVD risk in the highest quartile were 2.36 for 1-OHNa, 6.58 for 2-OHNa, and 1.60 for ΣOH-PAH (all Ptrend<0.05). In addition, significant dose-dependent relationships were found across 2-OHNa quartiles with decreasing HRV indices, which in turn, were positively associated with elevated risk of ASCVD (all Ptrend<0.05). Mediation analyses indicated that HRV mediate 2.7%-4.3% of the association between 2-OHNa exposure and higher ASCVD risk. Our data suggested that occupational exposure to PAHs may increase ASCVD risk, which was partially mediated by HRV.


Assuntos
Aterosclerose/induzido quimicamente , Frequência Cardíaca/efeitos dos fármacos , Exposição Ocupacional/efeitos adversos , Hidrocarbonetos Policíclicos Aromáticos/urina , Adulto , Doenças Cardiovasculares/induzido quimicamente , Coque/efeitos adversos , Feminino , Cromatografia Gasosa-Espectrometria de Massas , Humanos , Masculino , Exposição Ocupacional/análise , Hidrocarbonetos Policíclicos Aromáticos/metabolismo , Análise de Regressão
11.
Se Pu ; 37(3): 252-258, 2019 Mar 08.
Artigo em Chinês | MEDLINE | ID: mdl-30900852

RESUMO

A method based on the magnetic solid-phase extraction using magnetic carbon nitride composites coupled with high performance liquid chromatography-fluorescence detector (HPLC-FLD) was developed for the simultaneous determination of three hydroxyl polycyclic aromatic hydrocarbons (OH-PAHs) in urine. The synthesized sorbent was characterized by scanning electron microscope, X-ray diffractometer, vibrating sample magnetometer and surface area analyzer. The extraction parameters such as amount of sorbent, extraction time, eluting solvent and volume (single eluting volume×eluting times) were investigated in detail. Under the optimized conditions, the method showed a linear range of 0.25-250 µg/L (correlation coefficient=0.999). The limit of detection was 0.08 µg/L and the limit of quantification was 0.25 µg/L for each analyte. The proposed method gave a recovery of 90.1%-102%. The relative standard deviations for the intra-day and inter-day were 1.5%-7.7% and 2.2%-8.7%, respectively. The feasibility of the developed method was further demonstrated during the analysis of real samples. The results indicate that the magnetic carbon nitride composites can be used for the effective purification and enrichment of three OH-PAHs in urine. In addition, the method can be applied for analysis of urinary OH-PAHs in a simple, fast, and effective manner.


Assuntos
Nitrilos , Hidrocarbonetos Policíclicos Aromáticos/urina , Cromatografia Líquida de Alta Pressão , Humanos , Limite de Detecção , Magnetismo , Extração em Fase Sólida
12.
Talanta ; 198: 137-145, 2019 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-30876541

RESUMO

An analytical method for the biomonitoring of arsenic, benzene and polycyclic aromatic hydrocarbons (PAHs) in human urine was developed using liquid chromatography tandem mass spectrometry (LC-MS/MS). The urinary metabolites of monomethylarsonic acid (MMAA), dimethylarsonic acid (DMAA), s-phenylmercapturic acid (S-PMA), and 1-hydroxypyrene (1-OHP) were selected as the corresponding marker compounds. After enzymatic deconjugation, 4 mL urine sample was extracted by 2 steps of solvent extractions. The 1-OHP was first extracted with n-hexane with 10% ethyl acetate, and MMAA, DMMA, and S-PMA were then extracted in a 2nd extraction/back-extraction using chloroform/ammonium bicarbonate aqueous solution. The two extracts were mixed and analyzed by LC-MS/MS. The method was validated with spiked urine samples. The obtained linear ranges (r2 > 0.99) of the urinary markers were 2-64 ng/mL MMAA, 1-64 ng/mL DMAA, 0.78-100 ng/mL S-PMA and 0.05-6.4 ng/mL 1-OHP. The measured accuracy (% Error) and precision (CV%) were -16.67 to 29.17% and 2.03-30.99% (3 spiked levels, 6 replicates), respectively. The method was applied to 10 real urine samples, and the presence of MMAA, DMAA, S-PMA and 1-OHP were clearly detected. The detected concentrations were BQL-8.38 ng/mL of MMAA, BQL-10.71 ng/mL of DMAA, BQL-2.55 ng/mL of SPMA, and BQL-0.17 ng/mL of 1-OHP, which were all consistent with the reported background levels.


Assuntos
Arsênico/urina , Benzeno/análise , Hidrocarbonetos Policíclicos Aromáticos/urina , Cromatografia Líquida , Humanos , Espectrometria de Massas em Tandem
13.
Environ Sci Pollut Res Int ; 26(11): 10719-10726, 2019 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-30778934

RESUMO

Polycyclic aromatic hydrocarbons (PAHs) are environmental pollutants. Exposure to PAHs is associated with several adverse health outcomes. However, no previous study has examined the relationship between PAH exposure and functional dependence in an elderly population. Our aim was to examine whether PAH exposure was associated with functional dependence including total disability, activities of daily living (ADL), instrumental activities of daily living (IADL), leisure and social activities (LSA), lower extremity mobility (LEM), and general physical activities (GPA) in an elderly population. A total of 5816 elderly adults from the National Health and Nutrition Examination Survey (NHANES) from 2001 to 2006 were examined. PAH exposure was measured by urinary biomarkers. Functional dependence was assessed by 19 structured questions. The association between PAH exposures with functional dependence was performed by using a multivariable linear regression model. After adjusting for pertinent variables, positive associations were observed between the total number of disabilities and 2-naphthalene and 1-pyrene quartiles (all Ptrend < 0.05). There was a dose-dependent relationship between 1-pyrene quartiles and all functional dependence domains, and the higher quartile of 1-pyrene was more closely associated with functional impairment (all Ptrend < 0.05). PAH exposure is associated with functional dependence in American elderly adults. Future research is needed to bring to light the pathophysiological underlying mechanisms related to these findings.


Assuntos
Atividades Cotidianas , Pessoas com Deficiência/estatística & dados numéricos , Exposição Ambiental/análise , Poluentes Ambientais/análise , Hidrocarbonetos Policíclicos Aromáticos/análise , Adulto , Idoso , Biomarcadores/urina , Poluentes Ambientais/urina , Feminino , Humanos , Masculino , Pessoa de Meia-Idade , Inquéritos Nutricionais , Hidrocarbonetos Policíclicos Aromáticos/urina , Medição de Risco , Estados Unidos
14.
Environ Pollut ; 248: 304-311, 2019 May.
Artigo em Inglês | MEDLINE | ID: mdl-30802744

RESUMO

Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous environmental contaminants with a number of them being carcinogenic. One of the approaches to assess human exposure to PAHs is to measure their urinary metabolites, monohydroxyl polycyclic aromatic hydrocarbons (OH-PAHs), with a method allowing for high throughput and short turn-around time. We developed a method to quantify nine urinary OH-PAHs by using supported liquid phase extraction (SLE) and isotope dilution gas chromatography tandem mass spectrometry (GC-MS/MS). SLE demonstrated advantages over the traditionally used liquid-liquid extraction techniques. The target analytes with spiked deuterated and 13C-labeled internal standards were extracted from urine by SLE after enzymatic cleavage of the glucuronide and sulfate conjugates. The extracted analytes were then derivatized with N-Methyl-N-(trimethylsilyl) trifluoroacetamide (MSTFA), and analyzed by GC-MS/MS. Six solvent mixtures were evaluated as the SLE extraction solvent, and pentane:chloroform (7:3, v/v) was selected due to its best overall analytical performance. Method detection limits for the 9 analytes ranged from 2.3 to 13.8 pg/mL. Precision and accuracy were satisfactory. SLE and internal isotope labeled standard combination reduced matrix effect effectively. This new method using SLE sample preparation techniques coupled with GC-MS/MS proves applicable to urinary measurements for PAH exposure studies for general population.


Assuntos
Exposição Ambiental/análise , Poluentes Ambientais/urina , Hidrocarbonetos Policíclicos Aromáticos/urina , Acetamidas , Fluoracetatos , Cromatografia Gasosa-Espectrometria de Massas/métodos , Humanos , Técnicas de Diluição do Indicador , Isótopos , Limite de Detecção , Extração Líquido-Líquido/métodos , Hidrocarbonetos Policíclicos Aromáticos/análise , Hidrocarbonetos Policíclicos Aromáticos/química , Espectrometria de Massas em Tandem/métodos
15.
Chem Commun (Camb) ; 55(15): 2146-2149, 2019 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-30601487

RESUMO

We propose a novel method for highly sensitive SERS detection of hydrophobic analytes based on cetyltrimethylammonium bromide (CTAB)-triggered Ag aggregates. In particular, we demonstrated its use in a SERS-based assay for urinary hydroxylated polycyclic aromatic hydrocarbons (OH-PAHs) with high sensitivity and reproducibility.


Assuntos
Cetrimônio/química , Hidrocarbonetos Policíclicos Aromáticos/urina , Prata/química , Análise Espectral Raman , Humanos , Hidroxilação , Hidrocarbonetos Policíclicos Aromáticos/metabolismo , Reprodutibilidade dos Testes
16.
Environ Pollut ; 246: 587-596, 2019 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-30597391

RESUMO

Lead (Pb) and polycyclic aromatic hydrocarbon (PAH) exposure is positively associated with cardiovascular disease (CVD), and the possible potential mechanism may be caused by damage to the endothelium by modulation of inflammatory processes. No comprehensive research shows co-exposure of Pb and PAH on cardiovascular endothelial inflammation in electronic waste (e-waste) exposed populations. Given this, the aim of this study is to provide evidence for a relationship between Pb and PAH co-exposure and cardiovascular endothelial inflammation, in an e-waste-exposed population, to delineate the link between a potential mechanism for CVD and environmental exposure. We recruited 203 preschool children (3-7 years) were enrolled from Guiyu (e-waste-exposed group, n = 105) and Haojiang (reference group, n = 98). Blood Pb levels and urinary PAH metabolites were measured. Percentages of T cells, CD4+ T cells and CD8+ T cells, complete blood counts, endothelial inflammation biomarker (serum S100A8/A9), and other inflammatory biomarkers [serum interleukin (IL)-6, IL-12p70, gamma interferon-inducible protein 10 (IP-10)] levels were evaluated. Blood Pb, total urinary hydroxylated PAH (ΣOHPAH), total hydroxynaphthalene (ΣOHNap) and total hydroxyfluorene (ΣOHFlu) levels, S100A8/A9, IL-6, IL-12p70 and IP-10 concentrations, absolute counts of monocytes, neutrophils, and leukocytes, as well as CD4+ T cell percentages were significantly higher in exposed children. Elevated blood Pb, urinary 2-hydroxynaphthalene (2-OHNap) and ΣOHFlu levels were associated with higher levels of IL-6, IL-12p70, IP-10, CD4+ T cell percentages, neutrophil and monocyte counts. Mediator models indicated that neutrophils exert the significant mediation effect on the relationship between blood Pb levels and S100A8/A9. IL-6 exerts a significant mediation effect on the relationship between blood Pb levels and IP-10, as well as the relationship between urinary ΣOHFlu levels and IP-10. Our results indicate that children with elevated exposure levels of Pb and PAHs have exacerbated vascular endothelial inflammation, which may indicate future CVD risk in e-waste recycling areas.


Assuntos
Doenças Cardiovasculares/induzido quimicamente , Resíduo Eletrônico/efeitos adversos , Endotélio Vascular/efeitos dos fármacos , Poluentes Ambientais/toxicidade , Chumbo/toxicidade , Hidrocarbonetos Policíclicos Aromáticos/toxicidade , Biomarcadores/sangue , Contagem de Células Sanguíneas , Doenças Cardiovasculares/imunologia , Pré-Escolar , China , Citocinas/sangue , Resíduo Eletrônico/análise , Endotélio Vascular/imunologia , Exposição Ambiental/análise , Poluentes Ambientais/sangue , Poluentes Ambientais/urina , Feminino , Humanos , Inflamação , Chumbo/sangue , Masculino , Hidrocarbonetos Policíclicos Aromáticos/urina , Reciclagem
17.
Environ Int ; 122: 369-380, 2019 01.
Artigo em Inglês | MEDLINE | ID: mdl-30503314

RESUMO

BACKGROUND: All humans are now co-exposed to multiple toxic chemicals, among which metals and polycyclic aromatic hydrocarbons (PAHs) are of special concern as they are often present at high levels in various human environments. They can also induce similar early health damage, such as genetic damage, oxidative stress, and heart rate variability (HRV). Exposure to metals, PAHs, and their combined pollutants can alter microRNA (miRNA) expression patterns. OBJECTIVES: To explore the associations of metal-PAH co-exposure with miRNA expression, and of the associated miRNAs with early health damage. METHODS: We enrolled 360 healthy male coke oven workers and quantified their exposure levels of metals and PAHs by urinary metals, urinary monohydroxy-PAHs (OH-PAHs), and plasma benzo[a]pyrene-r-7,t-8,t-9,c-10-tetrahydotetrol-albumin (BPDE-Alb) adducts, respectively. We selected and measured ten miRNAs: let-7b-5p, miR-126-3p, miR-142-5p, miR-150-5p, miR-16-5p, miR-24-3p, miR-27a-3p, miR-28-5p, miR-320b, and miR-451a. For miRNAs influenced by the effect modification of metals or PAHs and/or metal-PAH interactions, we further evaluated their associations with biomarkers for genetic damage, oxidative stress, and HRV. RESULTS: After adjusting for PAHs and other metals, miRNA expression was found to be negatively associated with aluminum, antimony, lead, and titanium, and positively associated with molybdenum and tin (p < 0.05). Antimony showed modifying effects on the PAH-miRNA associations, while OH-PAHs and BPDE-Alb adducts modified the associations of metals with miRNAs (p for modifying effect < 0.05). Furthermore, miRNA expression was influenced by the antagonistic interactions between antimony and OH-PAHs, and by the synergistical interactions between metals and BPDE-Alb adducts (pinteraction < 0.05). Let-7b-5p, miR-126-3p, miR-16-5p, and miR-320b were additionally found to be associated with increased genetic damage in the present study [false discovery rate (FDR)-adjusted p < 0.05]. CONCLUSIONS: Associations of metal-PAH co-exposure with miRNA expression, and of associated miRNAs with early health damage, suggested potential mechanistic connections between the complex metal-PAH interactions and their deleterious effects that are worthy of further investigation.


Assuntos
Coque , Doença/etiologia , Poluentes Ambientais/toxicidade , Metais/toxicidade , Exposição Ocupacional , Hidrocarbonetos Policíclicos Aromáticos/toxicidade , Adulto , Biomarcadores , Dano ao DNA/efeitos dos fármacos , Poluentes Ambientais/urina , Humanos , Masculino , Metais/urina , MicroRNAs/análise , Pessoa de Meia-Idade , Estresse Oxidativo , Hidrocarbonetos Policíclicos Aromáticos/urina
18.
Environ Int ; 123: 201-208, 2019 02.
Artigo em Inglês | MEDLINE | ID: mdl-30530162

RESUMO

BACKGROUND: Polycyclic aromatic hydrocarbons (PAHs) are environmental pollutants formed from incomplete combustion of organic matter; some PAHs are carcinogens. Smoking, diet, and other activities contribute to exposure to PAHs. Exposure data to PAHs among combustible tobacco product users (e.g. cigarette smokers) exist; however, among non-combustible tobacco products users (e.g., e-cigarette users), such data are rather limited. OBJECTIVES: We sought to evaluate exposure to PAHs among participants in Wave 1 (2013-2014) of the Population Assessment of Tobacco and Health (PATH) Study based on the type of tobacco product (combustible vs non-combustible), and frequency and intensity of product use. METHODS: We quantified seven PAH urinary biomarkers in 11,519 PATH Study participants. From self-reported information, we categorized 8327 participants based on their use of tobacco products as never-tobacco user (never user, n = 1700), exclusive current established combustible products user (combustible products user, n = 5767), and exclusive current established non-combustible products user (non-combustible products user, n = 860). We further classified tobacco users as exclusive cigarette user (cigarette user, n = 3964), exclusive smokeless product user (SLT user, n = 509), and exclusive e-cigarette user (e-cigarette user, n = 280). Last, we categorized frequency of product use (everyday vs some days) and time since use (last hour, within 3 days, over 3 days). We calculated geometric mean (GM) concentrations, and evaluated associations between tobacco product user categories and PAH biomarkers concentrations. RESULTS: Combustible products users had significantly higher GMs of all biomarkers than non-combustible products users and never users; non-combustible products users had significantly higher GMs than never users for four of seven biomarkers. For all biomarkers examined, cigarette users had the highest GMs compared to other tobacco-product users. Interestingly, GMs of 2-hydroxyfluorene, 3-hydroxyfluorene and ∑2,3-hydroxyphenanthrene were significantly higher in SLT users than in e-cigarette users; 3-hydroxyfluorene and 1-hydroxypyrene were also significantly higher in e-cigarette and SLT users than in never users. Everyday cigarette and SLT users had significantly higher GMs for most biomarkers than some days' users; cigarette and SLT users who used the product in the last hour had significantly higher GMs of most biomarkers than other occasional cigarette or SLT users respectively. By contrast, everyday e-cigarette users' GMs of most biomarkers did not differ significantly from those in some days' e-cigarette users; we did not observe clear trends by time of last use among e-cigarette users. CONCLUSIONS: Users of tobacco products had higher PAH urinary biomarker concentrations compared to never users, and concentrations differed by type and frequency of tobacco product use.


Assuntos
Hidrocarbonetos Policíclicos Aromáticos/urina , Produtos do Tabaco , Adolescente , Adulto , Biomarcadores , Sistemas Eletrônicos de Liberação de Nicotina , Feminino , Humanos , Masculino , Pessoa de Meia-Idade , Autorrelato , Fumar , Estados Unidos , Adulto Jovem
19.
Environ Pollut ; 245: 453-461, 2019 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-30458375

RESUMO

Polycyclic aromatic hydrocarbons (PAHs) are well-known carcinogenic and endocrine disrupting chemicals that have been concerned over the past few decades. We aimed to determine the hydroxylated PAH (OHPAH) metabolite concentrations in maternal urine collected from the e-waste-contaminated area of Guiyu and the reference area of Haojiang, China, and to evaluate their health effects on birth outcomes. The median Æ©OHPAH concentration was 6.87 µg/g creatinine from Guiyu, and 3.90 µg/g creatinine from Haojiang. 2-OHNap and 1-OHPyr were the predominant metabolites. Residence in Guiyu and recycling in houses were associated with elevated 2-OHNap and 1-OHPyr. Standardized mean difference revealed that compared to low PAH metabolite levels in the first quartile, high PAH metabolite levels in the fourth quartile especially for 1-OHPyr, Æ©OHPAHs and sometimes hydroxylphenanthrene compounds, presented a reduced size in birth outcomes (overall SMD: -0.09; 95% CI: -0.15, -0.03), including head circumference, BMI and Apgar 1 score, and increased size in height. After adjusting for confounders in regression models, an interquartile increase in ΣOHPAHs was associated with a decrease of 234.56 g in weight (95% CI: -452.00, -17.13), 1.72 cm in head circumference (95% CI: -2.96, -0.48), 1.06 kg/m2 in BMI (95% CI: -1.82, -0.31) and 0.42 in Apgar 1 score (95% CI: -0.66, -0.18), respectively. These findings suggest high exposure to PAHs during pregnancy in e-waste areas, posing a potential threat to neonatal development, which likely can be attributed to direct e-waste recycling activities. Ongoing studies should be continued to monitor human exposure and health, in particular for vulnerable individuals in e-waste-polluted areas.


Assuntos
Peso ao Nascer/efeitos dos fármacos , Carcinógenos/análise , Resíduo Eletrônico/análise , Disruptores Endócrinos/urina , Poluentes Ambientais/urina , Hidrocarbonetos Policíclicos Aromáticos/urina , China , Creatinina/urina , Feminino , Humanos , Hidroxilação , Recém-Nascido , Estudos Longitudinais , Masculino , Hidrocarbonetos Policíclicos Aromáticos/metabolismo , Gravidez , Resultado da Gravidez , Reciclagem
20.
Environ Pollut ; 245: 183-198, 2019 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-30419459

RESUMO

The relations of polycyclic aromatic hydrocarbons (PAHs) exposure with platelet indices remain unclear. Based on the baseline data from the Wuhan-Zhuhai Cohort Study, we used generalized linear model, multivariate logistic regression analysis and restricted cubic splines (RCS) to assess linear and nonlinear relationship of PAHs exposure with platelet indices. The results showed that among Wuhan individuals, there were the non-linear relations between total hydroxynaphthalene (ΣOHNa) and mean platelet volume (MPV) or ratio of mean platelet volume to platelet count (MPVP), total hydrophenanthrene (ΣOHPh) and MPV or platelet distribution width (PDW), the sum concentration of urinary monohydroxylated metabolites of PAHs (ΣOH-PAHs) and ratio of platelet count to lymphocyte count (PLR) or MPVP, 1-hydropyrene (1-OHP) and PLR or PDW. But among Zhuhai individuals, neither linear nor non-linear relations were found between each of OH-PAHs or ΣOH-PAHs and platelet indices. The findings indicate that serum MPV and MPVP may be independent biomarkers of effects of exposing to environmental PAHs on human bodies.


Assuntos
Plaquetas/efeitos dos fármacos , Exposição Ambiental , Poluentes Ambientais/toxicidade , Hidrocarbonetos Policíclicos Aromáticos/toxicidade , Adolescente , Adulto , Idoso , Idoso de 80 Anos ou mais , Biomarcadores/sangue , China , Estudos de Coortes , Feminino , Humanos , Contagem de Linfócitos , Masculino , Volume Plaquetário Médio , Pessoa de Meia-Idade , Hidrocarbonetos Policíclicos Aromáticos/metabolismo , Hidrocarbonetos Policíclicos Aromáticos/urina
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