Real-time Measurements in Real-world Samples: Fate and Distribution of Trace Organic Contaminants by Direct Mass Spectrometry

真实样品中的实时测量：通过直接质谱法测定痕量有机污染物的归宿和分布

• 批准号: RGPIN-2022-05349
• 负责人: Krogh, Erik
• 金额: $ 2.62万
• 依托单位: Vancouver Island University
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2022
• 资助国家: 加拿大
• 起止时间: 2022-01-01 至 2023-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=747956
• 关键词: Real; time; Measurements; world; Samples

This research program centres on the development and application of innovative real-time mass spectrometry (MS) techniques for the direct and continuous measurement of molecular determinants of environmental and human health. Direct MS is an extremely powerful analytical platform that enables high throughput, time-resolved, and in-situ measurements. These unique capabilities address several long-standing constraints to current understanding of the fate and distribution of contaminants of emerging concern by providing molecular level information in complex samples with applications in real-time monitoring and advanced spatiotemporal analysis. This research will 1) develop novel direct sampling methods for new contaminant classes, 2) study environmental chemical processes in complex media, and 3) mobilize MS for in-field measurements in air, water, and sediments. These goals are realized by developing sensitive and selective MS methods that are fast, simple, and robust. In the absence of chromatographic separation, direct MS relies on selectivity imparted by the sample introduction method, ionization mechanism, and the mass spectrometer. In membrane introduction methods, molecules permeate into an acceptor which is continuously infused into a mass spectrometer. Understanding factors that control mass transport allow us to improve selectivity and design novel membrane-based strategies using new materials, electrical gradients, and chemical modifiers. Field asymmetric waveform ion mobility spectrometry represents an ideal pairing with direct MS applications as it provides fast, orthogonal separation (based on differential mobility). It is readily paired with high resolution, lab-based instruments and lower cost, portable MS, providing the opportunity to develop methods for subsequent in-field applications. Time-resolved MS techniques provide unique insight into the mechanisms of chemical and physical processes that affect the transformation of contaminants in the environment. Membrane introduction MS techniques are employed to follow changes in the concentration of analytes in heterogeneous samples including sorption of trace contaminants on microplastics and photochemical degradation of naphthenic acids in oil sands process waters. Proton-transfer reaction MS provides continuous on-road measurements of volatile organic compounds that yields chemical concentrations mapped at the neighborhood scale and compositional information to `finger-print' sources and apportion contributions. The research described here opens important new territory in environmental chemical analysis by developing next-generation methods to provide real-time molecular level information in real-world samples. Providing chemical information `when' and `where' it is needed enables environmental assessment and forensics at unprecedented spatiotemporal resolution. As such, this research contributes directly to environmental protection and healthy communities.

该研究项目的重点是开发和应用创新的实时质谱（MS）技术，用于直接和连续测量环境和人类健康的分子决定因素。Direct MS是一个非常强大的分析平台，可实现高通量，时间分辨和原位测量。这些独特的功能通过提供复杂样品中的分子水平信息，在实时监测和先进的时空分析中应用，解决了当前对新兴关注的污染物的命运和分布的理解的几个长期限制。这项研究将1)为新的污染物类别开发新的直接采样方法，2)研究复杂介质中的环境化学过程，以及3)利用质谱在空气、水和沉积物中进行现场测量。这些目标是通过开发快速、简单、鲁棒的灵敏、选择性的质谱方法来实现的。在没有色谱分离的情况下，直接质谱依赖于样品引入方法、电离机制和质谱仪所赋予的选择性。在膜导入方法中，分子渗透到受体中，受体连续注入质谱仪。了解控制质量传递的因素使我们能够提高选择性，并使用新材料、电梯度和化学改性剂设计新的基于膜的策略。现场不对称波形离子迁移率光谱代表了与直接MS应用的理想配对，因为它提供了快速，正交分离（基于差分迁移率）。它很容易与高分辨率的实验室仪器和低成本的便携式质谱仪配对，为后续的现场应用提供了开发方法的机会。时间分辨质谱技术为影响环境中污染物转化的化学和物理过程的机制提供了独特的见解。膜导入质谱技术用于跟踪非均质样品中分析物浓度的变化，包括微量污染物在微塑料上的吸附和油砂工艺水中环烷酸的光化学降解。质子转移反应质谱提供挥发性有机化合物的连续道路测量，产生化学浓度在邻域尺度和组成信息映射到“指纹”来源和分摊贡献。这里描述的研究通过开发下一代方法来提供真实样品的实时分子水平信息，为环境化学分析开辟了重要的新领域。提供“何时”和“何地”需要的化学信息，使环境评估和取证能够以前所未有的时空分辨率进行。因此，这项研究直接有助于环境保护和健康社区。