Zhou Wei, Pawliszyn Janusz
Department of Chemistry, University of Waterloo, Waterloo, Ontario, N2L 3G1, Canada.
Angew Chem Int Ed Engl. 2025 Aug 18;64(34):e202504080. doi: 10.1002/anie.202504080. Epub 2025 Jul 22.
Ambient mass spectrometry (AMS) offers rapid screening but faces challenges in analyzing complex samples due to high matrix effects. The absence of a separation step can also lead to false positives due to the isomers or isobars. In this study, a sequential analysis strategy which combines ambient MS and LC-MS based on the non-exhaustive microdesorption in solid-phase microextraction (SPME) was developed for the first time. By combining coated blade spray (CBS)-MS with LC-MS, in the first step, a few microliters of solvent were used for non-exhaustive desorption with high enrichment factor for rapid screening by CBS-MS. For the suspicious samples, the remaining analytes on the SPME coating undergo exhaustive desorption, then followed by LC-MS confirmation. The matrix-compatible coating used in the SPME device significantly reduces matrix effects while enhancing sensitivity through analyte enrichment. This method is environmentally friendly, utilizing only a few microliters of organic solvents for screening. The approach was rigorously validated, both theoretically and experimentally, and successfully applied to anti-doping testing, enabling detection of 53 prohibited substances in urine samples by integrating CBS-MS with LC-MS.
常压质谱(AMS)可提供快速筛查,但由于基质效应高,在分析复杂样品时面临挑战。由于异构体或同量异位素的存在,缺少分离步骤也可能导致假阳性。在本研究中,首次开发了一种基于固相微萃取(SPME)中不完全微解吸的,将常压质谱与液相色谱-质谱联用的顺序分析策略。通过将涂层刀片喷雾(CBS)-质谱与液相色谱-质谱联用,第一步,使用几微升溶剂进行不完全解吸,以获得高富集因子,通过CBS-质谱进行快速筛查。对于可疑样品,SPME涂层上剩余的分析物进行完全解吸,然后通过液相色谱-质谱进行确认。SPME装置中使用的与基质兼容的涂层显著降低了基质效应,同时通过分析物富集提高了灵敏度。该方法环境友好,仅使用几微升有机溶剂进行筛查。该方法在理论和实验上都经过了严格验证,并成功应用于反兴奋剂检测,通过将CBS-质谱与液相色谱-质谱联用,能够检测尿液样品中的53种违禁物质。