超高效液相色谱-串联质谱法测定贝类中抗病毒药物及其风险评估

Determination of antiviral drugs in shellfish by ultra performance liquid chromatography-tandem mass spectrometry and its risk assessment

中文关键词:  抗病毒药物  超高效液相色谱-串联质谱  贝类及贝类干制品  风险评估

英文关键词:antiviral drugs  ultra performance liquid chromatography-tandem mass spectrometry  shellfish and dried shellfish products  risk assessment

中文摘要:

      目的 建立了超高效液相色谱-串联质谱法测定贝类及贝类干制品中12种抗病毒类药物(antiviral drugs, ATVs)的方法。方法 样品经含有1%甲酸乙腈溶液提取, FaVEx-NM50多兽残检测净化柱-净化除杂, 水浴氮吹浓缩, 复溶液定容后制备成样液备检。样液经ZORBAX Eclipse Plus C18-色谱柱进行分离, 以含乙腈甲醇(80:20, V:V, 含0.1%甲酸)-5 mmol/L乙酸铵(含0.1%甲酸)溶液作为流动相梯度洗脱, 采用超高效液相色谱-串联质谱法-多反应监测模式分析检测, 内标法定量。结果 12种目标化合物在一定质量浓度范围内线性关系良好, 检出限及回收率等均满足检测需求。其中, 标准曲线相关系数(r)为0.9931~0.9997, 检出限为0.07~1.50 μg/kg, 定量限为0.14~3.00 μg/kg。3个添加水平(n=6)下贻贝基质的平均回收率为66.7%~106.2%, 相对标准偏差为1.0%~11.6%, 干贝基质的平均回收率为69.1%~109.5%, 相对标准偏差为0.9%~10.3%。同时, 采购了161批次贝类及贝类干制品, 并用该方法对样品中的目标化合物进行了分析, 结果显示37批次样品检出金刚烷胺。结合膳食数据和人群数据, 进行了金刚烷胺残留的膳食暴露风险评估, 结果表明当前的金刚烷胺残留贝类对人体健康影响较小。结论 该方法灵敏度高, 准确性好, 前处理过程简单、快速, 适用于开展贝类中ATVs残留的检测。

英文摘要:

      Objective To establish a method for the determination of 12 kinds of antiviral drugs (ATVs) in shellfish and dried shellfish products by ultra performance liquid chromatography-tandem mass spectrometry. Methods Samples were extracted with acetonitrile containing 1% formic acid, purified using FaVEx-NM50 multi-veterinary drug residue clean-up columns, concentrated under nitrogen in a water bath, and reconstituted with a redissolving solution to obtain the test solution. The analytes were separated on a ZORBAX Eclipse Plus C18 column using gradient elution with a mobile phase consisting of acetonitrile?methanol (80:20, V:V, containing 0.1% formic acid) and 5 mmol/L ammonium acetate (containing 0.1% formic acid). Detection was carried out by ultra performance liquid chromatography-tandem mass spectrometry in multiple reaction monitoring mode, and quantification was performed using the internal standard method. Results The 12 kinds of target compounds showed good linearity over certain concentration ranges, and the limits of detection and recoveries met the requirements. The correlation coefficients (r) of the calibration curves ranged from 0.9931 to 0.9997, limits of detection were 0.07–1.50 μg/kg, and limits of quantitation were 0.14–3.00 μg/kg. At 3 spiked levels (n=6), the average recoveries in mussel matrix ranged from 66.7% to 106.2% with relative standard deviations of 1.0%–11.6%, while in dried scallop matrix the average recoveries ranged from 69.1% to 109.5% with relative standard deviations of 0.9%–10.3%. Meanwhile, 161 batches of shellfish and dried shellfish products were purchased and analyzed for the target compounds using this method. The results showed that amantadine was detected in 37 batches. A dietary exposure risk assessment of amantadine residues was conducted by combining the residue data with dietary consumption and population data. The assessment indicated that the current amantadine residues in shellfish posed a low risk to human health. Conclusion The method is sensitive, accurate, simple and rapid in sample pretreatment, making it suitable for the determination of ATVs residues in shellfish.