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Drop-on-demand sample introduction system coupled with the flowing atmospheric-pressure afterglow for direct molecular analysis of complex liquid micro-volume samples

机译：按需样品引入系统加上流动的大气压力余辉用于复合液体微量样品的直接分子分析

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One of the fastest developing fields in analytical spectrochemistry in recent years is ambient desorption/ionization mass spectrometry (ADI-MS). This burgeoning interest has been due to the demonstrated advantages of the method: simple mass spectra, little or no sample preparation, and applicability to samples in the solid, liquid, or gaseous state. One such ADI-MS source, the flowing atmospheric-pressure afterglow (FAPA), is capable of direct analysis of solids just by aiming the source at the solid surface and sampling the produced ions into a mass spectrometer. However, direct introduction of significant volumes of liquid samples into this source has not been possible, as solvent loads can quench the afterglow and, thus, the formation of reagent ions. As a result, the analysis of liquid samples is preferably carried out by analyzing dried residues or by desorbing small amounts of liquid samples directly from the liquid surface. In the former case, reproducibility of sample introduction is crucial if quantitative results are desired. In the present study, introduction of liquid samples as very small droplets helps overcome the issues of sample positioning and reduced levels of solvent intake. A recently developed “drop-on-demand” (DOD) aerosol generator is capable of reproducibly producing very small volumes of liquid (~17 pL). In this paper, the coupling of FAPA-MS and DOD is reported and applications are suggested. Analytes representing different classes of substances were tested and limits of detections were determined. Matrix tolerance was investigated for drugs of abuse and their metabolites by analyzing raw urine samples and quantification without the use of internal standards. Limits of detection below 2 µg/mL, without sample pretreatment, were obtained.
机译：近年来，分析光谱化学中发展最快的领域之一是环境解吸/电离质谱（ADI-MS）。这种迅速增长的兴趣归因于该方法的优势：简单的质谱，很少或没有样品制备，以及适用于固态，液态或气态样品。一种这样的ADI-MS源，即流动的大气压余辉（FAPA），仅通过将源对准固体表面并将产生的离子采样到质谱仪中就能够直接分析固体。但是，不可能将大量的液体样品直接引入该源中，因为溶剂负载会淬灭余辉，从而终止试剂离子的形成。结果，优选通过分析干燥的残留物或通过直接从液体表面解吸少量液体样品来进行液体样品的分析。在前一种情况下，如果需要定量结果，样品引入的可重复性至关重要。在本研究中，以非常小的液滴形式引入液体样品有助于克服样品定位和减少溶剂摄入量的问题。最近开发的“按需滴落”（DOD）气雾发生器能够可重复生产非常少量的液体（〜17 pL）。本文报道了FAPA-MS和DOD的耦合并提出了应用建议。测试了代表不同类别物质的分析物，并确定了检出限。通过分析未加工尿液样本和定量分析，不使用内标物，对滥用药物及其代谢物的基质耐受性进行了研究。未经样品预处理，检出限低于2 µg / mL。

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