Instrumental Innovations for Membrane Introduction Mass Spectrometry

识别和测量现实世界样品中的痕量分子水平是分析化学的最终目标。不幸的是，在复杂的真实世界样本(城市废水、血液、尿液、组织液等)中进行的痕量水平测量。可能会被样品的其他主要成分(干扰物)混淆，对成功的结果产生不利影响。直接测定是可取的，因为它们简单，可以减少因污染或稀释而改变结果的风险。在真实样品(杀虫剂、激素、药物、代谢物等)中成功测量环境和人类健康的关键决定因素这是具有挑战性的，因为许多当前的分析需要样品清理、浓缩和其他准备步骤，增加了时间和成本，以及样品的潜在污染或稀释的风险。*我的研究计划旨在开发新的方法，用于直接、在线、实时地测量复杂的真实样品中的痕量分子(分析物)，在环境、生物分析(医学、制药)和材料科学中具有重要的应用。这项工作的基础是使用聚合物(或其他)膜作为复杂的空气或水基样品和质谱仪(MS)之间的直接桥梁，质谱仪用于随后识别和测量痕量分析物。这项技术被称为膜引入质谱仪(MIMS)，是直接和连续的，省去了样品前处理步骤：定量、分子特异性测量是可能的。通过膜从样品转移的分析物是以混合物的形式进行的，在那里它们被转化为离子，并由MS进行分析。由于从样品转移的分析物是通过膜连续转移的，所以MIMS还可以确定浓度随时间的变化，从而提供关键信息(例如，实时空气质量测量、工业废物流监测、医疗诊断等)。在分析单个样本时可能会遗漏这一点。*MIMS对分析物的选择性来自于膜的选择、离子发生方法和质量测量步骤。我的研究将探索开发改进的、微型的膜-样品界面，实现对小样品的快速、低成本、选择性、直接测量，研究选择性和灵敏的离子产生方法及其后续的MS检测，并逐步开发紧凑型、便携式MIMS系统，从长远来看，这些系统将能够在需要时随时随地进行直接、实时的测量，提供高精度的实验室外结果，对于严重事件(环境泄漏)以及提供及时的医疗诊断、实现更高质量的医疗保健、提高所有加拿大人的生活质量至关重要。

The identification and measurement of trace levels of molecules in real world samples is the end goal of analytical chemistry. Unfortunately, trace level measurements made in complicated, real-world samples (municipal waste water, blood, urine, tissue fluids, etc.) can be confounded by the other, major components of the samples (interferents), adversely affecting successful results. Direct determinations are desirable, because they are simple, and can reduce the risk of altering the results through contamination or dilution. The successful measurement of key determinants of environmental and human health in real samples (pesticides, hormones, drugs, metabolites, etc.) is challenging because many current analyses require sample cleanup, concentration and other preparation steps, adding both time and cost, as well as the risk of potential contamination or dilution of the samples.***My research program is aimed at developing new approaches for the direct, online, ‘real-time' measurement of trace level molecules (analytes) in complex, real samples, with important applications in environmental, bioanalytical (medical, pharmaceutical) and material sciences. The basis for this work is to use polymer (or other) membranes as a direct bridge between complex air or water based samples and mass spectrometers (MS), which are used for the subsequent identification and measurement of trace level analytes. The technique, called membrane introduction mass spectrometry (MIMS), is direct and continuous, eliminating sample pretreatment steps: quantitative, molecularly specific measurements are possible. Analytes that transfer from the sample across the membrane do so as a mixture, where they are converted into ions, and analyzed by the MS. Because analyte transfer from a sample is continuous across the membrane, MIMS can also determine concentration changes over time, providing key information (e.g. real-time air quality measurements, industrial waste stream monitoring, point-of-care medical diagnostics, etc.) that can be missed when analyzing single samples. ***MIMS' selectivity for analytes arises from the membrane choice, the ion generation approach and the mass measurement steps. My research will explore the development of improved, miniaturized membrane-sample interfaces, enabling rapid, low-cost, selective, direct measurements for small samples, investigate selective and sensitive ion generation approaches and their subsequent MS detection, and the evolutionary development of compact, portable MIMS based systems, that in the long term will enable direct, real-time measurements when and where they are needed, providing high precision results out-of-the-lab, crucial in events such as critical incidents (environmental spills) as well as in providing timely medical diagnostics, enabling better quality health care, improving the quality of life for all Canadians.