PDF(Pubmed)
Abstract：
Rapid industrial and agricultural developments in China have led to the wide use and discharge of chemical products and pesticides, resulting in extensive residues in environmental media. These residues can enter the human body through various pathways, leading to high exposure risks and health hazards. Because the human body is exposed to a variety of chemical pollutants, accurately quantifying the exposure levels of these pollutants in the human body and evaluating their health risks are of great importance. In this study, the serum concentrations of 97 typical chemical pollutants of 60 adults in central China were simultaneously determined using solid-phase extraction coupled with gas chromatography-tandem mass spectrometry (SPE-GC-MS/MS). In this method, 200 μL of a serum sample was mixed with 10 μL of an isotope-labeled internal standard solution. The sample was vortexed and refrigerated overnight at 4 ℃. Each sample was then deproteinized by the addition of 200 μL of 15% formic acid aqueous solution and vortexed. The serum sample was loaded into a preconditioned Oasis® PRiME HLB SPE cartridge and rinsed with 3 mL of methanol-water (6∶1, v/v). The SPE cartridge was subsequently vacuumed. The analytes were eluted with 3 mL of dichloromethane followed by 3 mL of n-hexane. The eluent was concentrated to near dryness under a gentle nitrogen stream and reconstituted with 100 μL of acetone. The samples were determined by GC-MS/MS and separated on a DB-5MS capillary column (30 m×0.25 mm×0.25 μm) with temperature programming. The column temperature was maintained at 70 ℃ for 2 min, increased at a rate of 25 ℃/min to 150 ℃, increased at a rate of 3 ℃/min to 200 ℃, and then held for 2 min. Finally, the column temperature was increased at a rate of 8 ℃/min to 300 ℃ and maintained at this temperature for 8 min. The samples were detected in multiple-reaction monitoring (MRM) mode and quantitatively analyzed using the internal standard method. Multiple linear regression models were used to analyze the effects of demographic characteristics, lifestyle habits, and diet on the concentrations of the chemical pollutants in the serum samples, and known biomonitoring equivalents (BEs) and human biomonitoring (HBM) values were combined to compute hazard quotients (HQs) and hazard indices (HIs) and evaluate the health risks of single and cumulative exposures to the chemical pollutants. The results showed that the main pollutants detected in human serum were organochlorine pesticides (OCPs), polychlorinated biphenyls (PCBs), and polycyclic aromatic hydrocarbons (PAHs). The detection rates of eight pollutants, including hexachlorobenzene (HCB) (100%), pentachlorophenol (PCP) (100%), p,p\'-dichlorodiphenylene (p,p\'-DDE) (100%), PCB-138 (100%), PCB-153 (98.3%), β-hexachlorocyclohexane (β-HCH) (91.7%), fluorene (Flu) (85.0%), and anthracene (Ant) (75.0%), were greater than 70%. The serum levels of β-HCH were higher in females than in males, and age was positively correlated with exposure to p,p\'-DDE, PCB-138, PCB-153, and β-HCH. Increased exposure levels to p,p\'-DDE and β-HCH may be associated with a high frequency of meat intake, whereas increased exposure level to PCP may be associated with a high frequency of vegetable intake. The serum HQ of PCP was greater than 1 in 6.7% of the samples, and no risk was observed for HCB and p,p\'-DDE exposure in the study population. Approximately 28.3% of the study subjects had HI values greater than 1. Overall, the general adult population in this region is widely exposed to a wide range of chemical pollutants, and gender, age, and diet are likely to be the main factors influencing the concentration of chemical pollutants. The health risk of single and compound exposures to chemical pollutants should not be ignored.
摘要：
中国工农业的快速发展,导致化学产品和农药的广泛使用和排放,导致环境介质中大量残留。这些残基可以通过各种途径进入人体，导致高暴露风险和健康危害。因为人体暴露于各种化学污染物中，准确量化这些污染物在人体中的暴露水平并评估其健康风险非常重要。在这项研究中,采用固相萃取-气相色谱-串联质谱法(SPE-GC-MS/MS)同时测定了华中地区60名成年人97种典型化学污染物的血清浓度。在这种方法中，将200μL血清样品与10μL同位素标记的内标溶液混合。将样品涡旋并在4°C下冷藏过夜。然后通过加入200μL的15%甲酸水溶液并涡旋将每个样品脱蛋白。将血清样品加载到预处理的Oasis®PRiMEHLBSPE柱中，并用3mL甲醇-水（6∶1，v/v）冲洗。随后将SPE盒抽真空。用3mL二氯甲烷,然后用3mL正己烷洗脱分析物。在温和的氮气流下将洗脱液浓缩至接近干燥,并用100μL丙酮重构。样品通过GC-MS/MS测定，并在DB-5MS毛细管柱（30m×0.25mm×0.25μm）上进行温度编程分离。柱温在70℃下保持2分钟,以25℃/min的速度增加到150℃，以3℃/min的速率增加到200℃，然后保持2分钟。最后,柱温以8℃/min的速率升至300℃,并在此温度下保持8min。采用多反应监测(MRM)模式检测样品,采用内标法进行定量分析。采用多元线性回归模型分析人口学特征的影响,生活习惯,和饮食对血清样本中化学污染物浓度的影响，将已知的生物监测当量（BE）和人类生物监测（HBM）值结合起来，以计算危害商（HQs）和危害指数（HIs），并评估化学污染物单次和累积暴露的健康风险。结果表明,人血清中检测到的主要污染物为有机氯农药(OCPs),多氯联苯（PCBs），和多环芳烃(PAHs)。八种污染物的检出率,包括六氯苯(HCB)(100%)，五氯苯酚(PCP)(100%),p,对二氯二亚苯基(p，p'-DDE)(100%),PCB-138(100%),PCB-153(98.3%),β-六氯环己烷(β-HCH)(91.7%)，芴（流感）（85.0%），和蒽（Ant）（75.0%），大于70%。女性血清β-HCH水平高于男性,年龄与接触P呈正相关，p\'-DDE,PCB-138、PCB-153和β-HCH。增加对p的暴露水平，p-DDE和β-HCH可能与肉类摄入频率高有关，而PCP暴露水平的增加可能与蔬菜摄入的高频率有关。6.7%的样本中PCP的血清HQ大于1,没有观察到HCB和p，研究人群中的p'-DDE暴露。大约28.3%的研究对象具有大于1的HI值。总的来说,该地区的一般成年人口广泛接触各种化学污染物，和性别,年龄,和饮食可能是影响化学污染物浓度的主要因素。化学污染物单一和复合暴露的健康风险不容忽视。
