Direct Mass Spectrometry Innovations for Trace Level Measurements in Complex Samples

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(非法街头毒品、城市废水、食品、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。此外，进行这些测定的传统方法可能既昂贵又耗时。直接测定是可取的，因为它们简单快速，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由于目前的许多分析方法需要样品清理、浓缩和其他准备步骤，增加了时间和成本，并存在样品潜在污染或稀释的风险，因此具有挑战性。我的研究计划旨在开发新的方法，用于直接、在线、“实时”测量复杂的真实样品中的痕量分子(分析物)，具有重要的环境、生物分析(临床、药物)、执法、法医、减害药物测试和食品安全应用。本研究的基础是使用直接采样接口作为复杂样品和质谱仪之间的桥梁，用于后续痕量水平分析物的鉴定和测量。我们研究组正在探索和开发的膜引入质谱仪(MIMS)和纸喷雾质谱仪(PS-MS)的直接质谱学技术使用简单，无需样品前处理步骤：这两种方法都可以进行快速、定量和分子特异性的测量。这些方法非常适合在现场或现场使用紧凑型质谱仪。潜在的应用将从医疗诊断到环境紧急反应，我们目前正在开发有效的下一代减少伤害药物测试策略，用于阿片类药物过量危机。从长远来看，我们的研究成果将有助于开发直接测量技术，在需要时随时随地进行实时测量，提供实验室外的高精度结果，在严重事件(环境泄漏)等事件中以及在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方面至关重要。

The identification and measurement of trace levels of molecules in real world samples is the ultimate goal of analytical chemistry. Unfortunately, trace level measurements made in complicated, real-world samples (illicit street drugs, municipal waste water, foodstuffs, blood, urine, tissue fluids, etc.) can be confounded by the other, major components of the samples (interferents), adversely affecting successful results. Further, conventional methods to make these determinations can be both costly and time consuming. Direct determinations are desirable because they are simple and fast, 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 analysis methods require sample cleanup, concentration and other preparation steps, adding 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 environmental, bioanalytical (clinical, pharmaceutical), enforcement, forensic, harm reduction drug testing and food security applications. The basis for my research is to use direct sampling interfaces as a bridge between complex samples and mass spectrometers, which are used for the subsequent identification and measurement of trace level analytes. The direct mass spectrometry techniques of membrane introduction mass spectrometry (MIMS) and paper spray mass spectrometry (PS-MS) being explored and developed in our research group are simple to use and eliminate sample pretreatment steps: rapid, quantitative, molecularly specific measurements are possible with both. These methods are ideally suited for use with compact mass spectrometers at the point-of-care or on-site in the field. Potential applications will span from medical diagnostics to environmental emergency responses, and we are currently developing effective, next generation harm reduction drug testing strategies for use in the opioid overdose crisis. In the long term our research outcomes will enable the development of direct measurement technologies that produce 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.