3种尼泊金酯类防腐剂对发光菌Q67联合毒性相互作用的定量评估
Quantitative Evaluation of Combined Toxicity Interaction of Three Parabens to Luminescent Bacteria Q67
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摘要: 尼泊金酯类防腐剂广泛用于化妆品、食品等领域，可能会随使用过程进入环境中，给环境健康带来威胁。以3种尼泊金酯类防腐剂尼泊金甲酯(methylparaben, MET)、尼泊金乙酯(ethylparaben, ETH)、尼泊金丙酯(propylparaben, PRO)为研究对象，运用直接均分和均匀设计射线法分别设计3个二元混合物体系(MET-ETH、MET-PRO、ETH-PRO)和一个三元混合物体系(MET-ETH-PRO)，采用时间毒性微板分析法(t-MTA)测定3种防腐剂及其混合物体系对发光菌青海弧菌(Vibrio qinghaiensis sp. -Q67, Q67)在暴露时间0.25、2、4、8和12 h的毒性数据，应用浓度加和(CA)模型分析混合物体系的联合毒性相互作用，并采用绝对残差模型(dCA)定量评估毒性相互作用强度。结果表明，3种防腐剂MET、ETH、PRO对Q67的浓度-效应曲线呈现“S”型，具有明显的急性毒性，但时间依赖性不明显；3种防腐剂的所有混合体系对Q67的毒性均具有浓度依赖性，即混合污染物的毒性随着混合体系的浓度增大而增大，但随暴露时间的延长毒性逐渐减小；3个二元混合体系的毒性大小(pEC50)与混合物体系的组分浓度比(pi)呈良好的线性关系，但三元混合体系的线性关系不明显；CA和dCA对3种防腐剂的联合毒性相互作用分析结果一致：所有混合体系均呈现出毒性相互作用，其中MET-ETH混合体系呈现协同作用，MET-PRO、ETH-PRO和MET-ETH-PRO混合体系呈现拮抗作用，且均具有时间依赖性；依据dCA三维曲面图，4个混合物体系的毒性相互作用强度(dCA绝对值)均受暴露时间和混合物浓度的影响，在二元混合体系中，MET-PRO-R5射线在混合物体系浓度为6.26E-4 mol·L-1、暴露时间为12 h的拮抗作用强度最大，其dCA绝对值的最大值为0.380；在三元混合体系MET-ETH-PRO中，R4射线在混合物体系浓度为6.34E-4 mol·L-1、暴露时间为12 h时的协同作用强度最大，其dCA绝对值的最大值为0.384。dCA三维曲面图可以直观且定量地评估3种尼泊金酯类防腐剂污染物的毒性相互作用，可用于评估混合污染物的生态环境风险。Abstract: Parabens, which are widely used in cosmetics, food and other fields, are likely to enter the environment with the use process, posing a threat to environmental health. Three parabens including methylparaben (MET), ethylparaben (ETH) and propylparaben (PRO) were selected as research objects. Three binary mixture systems (MET-ETH, MET-PRO, ETH-PRO) and one ternary mixture system (MET-ETH-PRO) were designed by the direct equipartition ray design and uniform design ray, respectively. The toxicity data of the three parabens and their binary and ternary mixture systems towards luminescent bacteria Vibrio qinghaiensis sp. -Q67 (Q67) in exposure time of 0.25, 2, 4, 8 and 12 h were determined by the time-dependent microplate toxicity analysis (t-MTA). The concentration addition model (CA) was used to analyze the joint toxicity interaction within the mixtures, and the deviation from CA model (dCA) was used to dynamically and quantitatively evaluate the toxicity interaction intensity. The results showed that the concentration-response curves of three parabens MET, ETH and PRO to Q67 exhibited S-shaped and obvious acute toxicity, but showed no obvious time-dependence. The toxicity of all the mixture systems was concentration-dependent, i.e., toxicity increased with the increase of the concentration of mixture systems. However, their toxicity gradually decreased with the extension of exposure time. In addition, the toxicities (pEC50 values) of three binary mixture systems had good linear relationships with the components’ concentration ratios (pi), while the ternary mixture system did not have obvious linear relationship. The analysis results of the toxicity interaction by CA and dCA were consistent. According to CA and dCA, the binary and ternary mixture systems all showed toxic interaction. MET-ETH system showed synergism, while MET-PRO, ETH-PRO and MET-ETH-PRO systems showed antagonisms, and all of which were time-dependent. According to three dimensional dCA diagrams, the toxicity interaction intensity (absolute value of dCA) of binary and ternary mixture systems was affected by exposure time and mixture concentration. For the binary systems, the antagonism of ray R5 in MET-PRO system with concentration of 6.26E-4 mol·L-1 was the highest in the exposure time of 12 h, and the maximum absolute value of dCA was 0.380. For MET-ETH-PRO system, R4 showed the maximum absolute value of dCA (0.384) when its concentration was 6.34E-4 mol·L-1 in 12 h. The three dimensional dCA diagram method can intuitively and quantitatively evaluate the toxicity interactions of the three paraben mixture pollutants, and can be recommended to evaluate the ecological and environmental risks of mixed pollutants.
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Key words:
- paraben /
- Vibrio qinghaiensis sp. -Q67 /
- antagonism /
- synergism /
- the deviation from CA model
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