LAUSR

Abstract In the present study, a novel database of compounds and a screening method based on ultra-high performance liquid chromatography coupled to high resolution orbitrap mass spectrometry (UHPLC-Orbitrap HRMS) were developed. The method was applied to the rapid screening and identification of targeted and non-targeted antitussive adulterants in herbal medicines. The database includes retention time, exact mass, fragments, isotopic pattern and MS2 spectra library of the target compounds and provides automated search and identification of the target adulterants with merely a single injection. On the other hand, the full MS scan and MS2 HRMS data allow the identification of non-targeted compounds in samples with the assisted analysis of XCalibur4.0, MassFrontier7.0 and TraceFinder3.3 software and Chemspider database. The established HRMS method also possesses excellent quantitative capacity. All LOD values were in the range of 0.006 to 0.03 μg/g, while the values of all determination coefficients were higher than 0.9992 for all analytes. The intra– and inter–day accuracies were in the range of 92.4 to 108.3%, while the intra– and inter–day precision ranged from 2.6% to 8.7%. The screening database and method were used to detect antitussive adulterants in herbal medicines. Among 87 batches of herbal medicines which claimed “all-natural” and function of antitussive, 12 batches of samples were found as positive. The detected antitussive adulterants include target adulterants such as theophylline, sulfamethoxazole, prednisone acetate, chlorphenamine, pentoxyverine and non-targeted adulterants such as trimethoprim, dioxopromethazine, aspirin, diclofenac and cephalexin, with levels in the range of 0.271 ∼ 135.21 mg/g. Our work demonstrates that this novel orbitrap HRMS screening database for adulterants is a very promising and powerful tool for routine screening of illegal adulterated antitussives in herbal medicines in order to ensure the drug safety and public health.