为研究兽药残留高通量检测方法,使用超高效液相色谱-四极杆飞行时间串联质谱(ultra performance liquid chromatography-quadrupole time of flight tandem mass spectrometry, UPLC-Q-TOF-MS/MS)对畜禽基质样品以及21种兽药标准品进行检测,得到各兽药标准品的保留时间和特征碎片离子质谱图等信息,获得各目标化合物的线性方程、相关系数、线性范围以及测定底限。利用GNPS(global natural products social molecular networking)网站进一步探究了兽药的二级质谱裂解规律,对化合物进行结构解析和确证,发现同一种类的兽药分子裂解规律存在相似性,可以借助兽药分子的二级质谱裂解碎片实现畜禽肉中兽药残留的快速高通量筛查。基于UPLC-Q-TOF-MS/MS及GNPS分子网络技术,在24个猪肉、鱼肉样品中检出10种抗生素阳性,其中有3种不包含在已建立的兽药标准品信息库中。结果表明,相比于常规检测方法,UPLC-Q-TOF-MS/MS结合GNPS分子网络技术可以快速、简便地实现畜禽肉中兽药残留检测,且能发现未知兽药。
To investigate the high throughput detection method of veterinary drug residues, ultra performance liquid chromatography-quadrupole time of flight tandem mass spectrometry (UPLC-Q-TOF-MS/MS) was used to detect livestock and poultry matrix samples and 21 standard veterinary drugs.The retention time and characteristic fragment ion mass spectra of each standard veterinary drug were obtained.The linear equation, correlation coefficient, linear range, and limit of detection were obtained.Based on the GNPS (global natural products social molecular networking) website, the secondary mass spectrometry cleavage of veterinary drugs was further explored, and the structure of the compound was analyzed and confirmed.Results showed that the cleavage pattern of the same type of veterinary drug molecule was similar, and the rapid high throughput screening of veterinary drug residues in livestock and poultry meat could be realized based on the secondary mass spectrometry lysis fragments of veterinary drug molecule.According to UPLC-Q-TOF MS/MS and GNPS molecular network technology, 10 drugs were detected positive in 24 matrix samples of pork and fish, and 3 positive drugs were not included in the established standard veterinary drug information database.Indicating that compared with the conventional detection methods, UPLC-Q-TOF MS/MS combined with GNPS molecular network technology can realize the identification of veterinary drug residues in livestock and poultry meat quickly and accurately, and it can also find unknown veterinary drugs.
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