Instrumental Innovations for Membrane Introduction Mass Spectrometry

在真实的世界样品中痕量水平的分子的鉴定和测量是分析化学的最终目标。不幸的是，在复杂的、真实世界的样品（城市废水、血液、尿液、组织液等）中进行的痕量水平测量是不可能的。可能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，并且可以降低由于污染或稀释而改变结果的风险。成功测量真实的样品中环境和人类健康的关键决定因素（农药、激素、药物、代谢物等）这是具有挑战性的，因为许多当前的分析需要样品净化、浓缩和其他制备步骤，增加了时间和成本，以及潜在的污染或稀释样品的风险。 我的研究项目旨在开发新的方法，用于直接，在线，“实时”测量复杂，真实的样品中的痕量分子（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，用于随后的痕量水平分析物的识别和测量。该技术被称为膜引入质谱法（MIMS），是直接和连续的，消除了样品预处理步骤：定量，分子特异性测量是可能的。从样品转移穿过膜的分析物以混合物的形式进行，在那里它们被转化成离子，并由MS进行分析。由于从样品转移的分析物是连续穿过膜的，因此MIMS还可以确定浓度随时间的变化，提供关键信息（例如，实时空气质量测量、工业废物流监测、护理点医疗诊断等）。在分析单个样品时可能会遗漏。 MIMS对分析物的选择性来自膜的选择、离子产生方法和质量测量步骤。我的研究将探索改进的，小型化的膜样品接口的发展，使快速，低成本，选择性，直接测量小样品，研究选择性和敏感的离子产生方法及其随后的MS检测，以及紧凑型，便携式MIMS基于系统的进化发展，从长远来看，这将使直接，实时测量时，他们需要的地方，在实验室外提供高精度的结果，这在重大事件（环境泄漏）以及提供及时的医疗诊断等事件中至关重要，从而实现更高质量的医疗保健，提高所有加拿大人的生活质量。

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.