The targeted analysis of veterinary drug residues in honey traditionally involves a series of extraction and purification steps prior to quantification with high performance liquid chromatography coupled to high resolution or tandem mass spectrometry. These steps, designed to separate the target analytes from interferences, are generally time-consuming and costly. In addition, traditional cleanup steps are likely to eliminate other compounds whose analysis could prove decisive in current or future assessment of the honey sample. Alternatively, direct injection without complex sample preparation steps has been introduced for the fast analysis of trace compounds in environmental and food matrices. The aim of this study was to develop a rapid method for the targeted analysis of 7 key veterinary drug residues in honey based on direct injection high performance liquid chromatography coupled to quadrupole time-of-flight, while simultaneously recording data-independent MS/MS (e.g. All Ions MS/MS data) for future re-examination of the data for other purposes. The new method allowed for the detection of the target residues at levels approximately 20-100 times lower than current regulatory limits, for a total analysis time of about 45 min. The recoveries (103-119%), the linearity (R ≥ 0.996) and the repeatability (RSD ≤ 7%) were satisfactory. The method was then applied to 35 honey samples from the Canadian market. Residues of tylosin A, tylosin B, sulfamethazine and sulfadimethoxine were detected in 6, 9, 6 and 23% of the samples respectively, at levels below the regulatory limits in Canada. The possibility of adding a hydrolysis step to study sulfonamides in honey was tested, which provided good results for this family of compounds but lead to degradation of some of the other analytes. Finally, the non-targeted identification of several compounds was demonstrated as a proof of concept of future re-examination of All Ions MS/MS data. This paper illustrates the capacity of this novel method to combine targeted and non-targeted screening of chemical residues in honey.

中文翻译：

---

直接注射高效液相色谱与数据独立采集质谱联用，用于筛选蜂蜜中的抗生素

蜂蜜中兽药残留的靶向分析传统上涉及一系列提取和纯化步骤，然后使用高效液相色谱与高分辨率或串联质谱联用进行量化。这些旨在将目标分析物与干扰物分离的步骤通常既耗时又昂贵。此外，传统的净化步骤可能会消除其他化合物，这些化合物的分析可能对当前或未来的蜂蜜样品评估具有决定性意义。或者，引入了无需复杂样品制备步骤的直接进样，用于快速分析环境和食品基质中的痕量化合物。本研究的目的是开发一种基于直接注射高效液相色谱结合四极杆飞行时间的快速靶向分析蜂蜜中 7 种关键兽药残留的方法，同时记录与数据无关的 MS/MS。例如，所有离子 MS/MS 数据）以供将来出于其他目的重新检查数据。新方法可以检测到比当前监管限值低约 20-100 倍的目标残留物，总分析时间约为 45 分钟。回收率 (103-119%)、线性 (R ≥ 0.996) 和重复性 (RSD ≤ 7%) 令人满意。然后将该方法应用于来自加拿大市场的 35 个蜂蜜样品。分别有 6%、9%、6% 和 23% 的样本检出泰乐菌素 A、泰乐菌素 B、磺胺二甲嘧啶和磺胺二甲氧嘧啶的残留物，低于加拿大监管限制的水平。测试了添加水解步骤来研究蜂蜜中的磺胺类药物的可能性，这为这一系列化合物提供了良好的结果，但会导致一些其他分析物的降解。最后，几种化合物的非靶向鉴定被证明是未来重新检查全离子 MS/MS 数据的概念证明。本文说明了这种新方法结合靶向和非靶向筛查蜂蜜中化学残留物的能力。几种化合物的非靶向鉴定被证明是未来重新检查全离子 MS/MS 数据的概念证明。本文说明了这种新方法结合靶向和非靶向筛查蜂蜜中化学残留物的能力。几种化合物的非靶向鉴定被证明是未来重新检查全离子 MS/MS 数据的概念证明。本文说明了这种新方法结合靶向和非靶向筛查蜂蜜中化学残留物的能力。