High Performance Analysis of Complex Organic Mixtures

我们的研究计划的主要重点是通过设计高度自动化的小型化和集成仪器来促进实验室自动化和现场部署，用于从复杂基质中分离有机材料，以及随后的分离，鉴定和定量这些物种。我们正在积极追求无溶剂的“绿色”方法，可以整合采样和样品制备步骤，从而方便现场部署和体内测定。我们努力的长期目标是将分析化学“现场化”，即样品所在的位置，作为降低分析成本的一种手段，同时仍然提供快速准确的测量、筛选和监测。作为这项持续努力的一部分，我们的研究团队目前正在研究各种聚合物膜、吸附剂填充针和范围-吸附剂涂层支撑结构，包括纤维、尖端、颗粒和叶片。在未来5年的研究计划中，我们计划继续扩大我们对SPME取样过程中组织传质的基本理解，以扩大其应用范围，包括蛋白质提取，活系统代谢组学研究等更具挑战性的任务。本研究将有助于开发方便的提取装置、有效的方法和适当的校准程序，从而通过应用微提取原理实现高灵敏度的检测。主要重点将是利用现场仪器开发水和空气监测方法。我们之前的研究清楚地表明，体内SPME技术，“化学活检”，可以有效地从各种研究系统中分离代谢物组成，包括不稳定的化合物，这一壮举有助于正确表征生命系统。SPME还为微透析提供了补充的体内信息，因为它提供了更好的亲脂化合物覆盖范围。鉴于上述情况，鉴于许多脂质是良好的疾病生物标志物，我们一直在扩大体内脂质组学领域的研究。虽然大多数样品制备设备通常与色谱耦合，但我们最近考虑了设备与质谱和/或离子迁移率谱的直接耦合，利用这些设备的分离能力。为了促进这方面的研究，我们一直在开发一种通过离子在分离通道中的聚焦来实现离子迁移的新方法。这种独特的方法不仅由于聚焦而具有更高的灵敏度，而且还促进了选择性的增强，因为它可以通过向漂移气体中添加适当的化合物（“调节剂”）来有效地探索簇的形成。基于这一原理的系统将被设计得足够便携和紧凑，甚至可以放置在手机设备上

The primary focus of our research program is to facilitate lab automation and on-site deployment via design of highly automated miniaturized and integrated instrumentation for isolation of organic materials from complex matrices, as well as subsequent separation, identification, and quantification of these species. We are actively pursuing solvent-free, "green" approaches that can integrate both sampling and sample preparation steps and therefore facilitate convenient field deployment and in-vivo determinations. The long-term objective of our efforts is to move analytical chemistry "on-site", where the sample is located, as a means to decrease the cost of analysis, while still delivering rapid and accurate measurement, screening, and monitoring. As part of this ongoing effort, our research team is currently investigating various polymer membrane, sorbent packed needle, and range-sorbent coated support configurations, including fibers, tips, particles, and blades. In the next 5-year research program supported by the Discovery grant, we propose to continue expanding our fundamental understanding of mass transfer in tissue during SPME sampling so as to broaden the scope of its application to more challenging tasks, including protein extraction, metabolomics investigations of live systems. The proposed research will facilitate development of convenient extraction devices, effective methods, and appropriate calibration procedures, resulting in the enablement of highly sensitive detection through application of microextraction principles. The main focus will be development of water and air monitoring methods using on-site instrumentation. Our previous research clearly demonstrated that in-vivo SPME technology, "chemical biopsy", can effectively isolate metabolite composition, including unstable compounds, from various investigated systems, a feat which facilitates correct characterization of living systems. SPME also provides complementary in-vivo information to microdialysis, as it provides better coverage of lipophilic compounds. Considering the above, we have been expanding our research in the area of in-vivo lipidomics, given that many lipids are good disease biomarkers. While most sample preparation devices are typically coupled to chromatography, we have recently considered direct coupling of devices to mass spectrometry and/or ion mobility spectrometry, taking advantage of the separation power of these devices. To facilitate this line of research, we have been developing a new approach to ion mobility via focusing of ions in the separation channel. This unique approach not only results in higher sensitivity due to focusing, but also facilitates enhancement in selectivity, as it enables effective exploration of cluster formation by addition of appropriate compounds ("modifiers") to the drift gas. System based on such principle will be designed to be portable and compact enough so as to even allow for their placement onto a cellphone device