基于超高效液相色谱-四极杆-飞行时间高分辨质谱法快速筛查中兽药中302种药物非法添加

Rapid screening of 302 kinds of illegal additives in traditional Chinese veterinary medicine by ultra performance liquid chromatography-quadrupole time of flight high resolution-mass spectrometry

中文关键词:  超高效液相色谱-四极杆-飞行时间高分辨质谱法  非法添加  化学药物  中兽药

英文关键词:ultra performance liquid chromatography-quadrupole time of flight high resolution-mass spectrometry  illegal additives  chemical drugs  Chinese veterinary medicine

中文摘要:

      目的 建立一种基于超高效液相色谱-四极杆-飞行时间高分辨质谱法(ultra performance liquid chromatography-quadrupole time of flight high resolution-mass spectrometry, UPLC-Q-TOF-MS)用于中兽药中的302种药物非法添加的快速筛查方法。方法 建立了包含302种药物名称、分子式、精确质量数等信息的高分辨质谱数据库。样品经甲醇提取后, 经过UPLC-Q-TOF-MS进行数据采集并分析, 当保留时间与数据库绝对偏差<0.2 min, 质量误差<5 ppm, 同位素比值偏差<5%, 且主要特征碎片离子的库比对分数>80时, 认为检出疑似阳性样品。结果 该方法选择性较好, 目标物最低检出质量浓度低至50 ng/mL(四环素类、青霉素类、雌激素类、及非甾体抗炎药检出质量浓度100 ng/mL; 氨基糖苷类检出质量浓度200 ng/mL), 实现了302种非法添加药物的高效筛查。实际样品筛查时, 检出了7批疑似阳性样品。结论 本研究建立的筛查手段具有快速、广谱的特点, 适用于多种中兽药中的非法添加药物的初步筛查, 为中兽药质量控制提供了有效技术支持。

英文摘要:

      Objective To establish a method based on ultra performance liquid chromatography-quadrupole time of flight high resolution-mass spectrometry (UPLC-Q-TOF-MS) use as a rapid screening method for the illegal addition of 302 kinds of drugs in Chinese veterinary medicine. Methods A high-resolution mass spectrometry database containing information such as the names, molecular formulas, and exact mass numbers of 302 kinds of drugs was established. Samples were extracted with methanol and then analyzed by UPLC-Q-TOF-MS. A sample was considered as a suspected positive if the retention time deviation was less than 0.2 min, the mass error was less than 5 ppm, the isotopic ratio deviation was less than 5%, and the library matching score of the main characteristic fragment ions was greater than 80. Results The method exhibited good selectivity, with a minimum detection concentration as low as 50 ng/mL for the target substances (100 ng/mL for tetracyclines, penicillins, estrogens, and nonsteroidal anti-inflammatory drugs; 200 ng/mL for aminoglycosides). This enabled the efficient screening of 302 kinds of illegally added drugs. In the screening of actual samples, 7 batches of suspected positive samples were detected. Conclusion This approach is applicable for the screening of illegal additives in various veterinary Chinese medicines, providing effective technical support for the quality control of veterinary Chinese medicines.