High Performance Analysis of Complex Organic Mixtures

我们研究计划的主要重点是通过设计高度自动化、小型化和集成化的仪器来从复杂的基质中分离有机物质，以及随后对这些物种进行分离、鉴定和量化，从而促进实验室自动化和现场部署。我们正在积极寻求无溶剂的“绿色”方法，这种方法可以将采样和样品制备步骤结合在一起，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”转移到样品所在的地方，作为一种降低分析成本的手段，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、吸着剂填充针和范围吸着剂涂层支撑配置，包括纤维、尖端、颗粒和刀片。在发现基金支持的下一个五年研究计划中，我们建议继续扩大我们对SPME采样过程中组织中质量传递的基本了解，以便将其应用范围扩大到更具挑战性的任务，包括蛋白质提取、肝脏系统的代谢组学研究。拟议的研究将有助于开发方便的提取设备、有效的方法和适当的校准程序，从而通过应用微萃取原理实现高灵敏度的检测。主要重点将是开发使用现场仪器的水和空气监测方法。我们之前的研究清楚地表明，活体固相微萃取技术，即“化学活组织检查”，可以有效地从各种研究系统中分离代谢物成分，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还为微透析提供了体内补充信息，因为它更好地覆盖了亲脂化合物。考虑到上述情况，我们一直在扩大我们在体内脂类组学领域的研究，因为许多脂类是良好的疾病生物标志物。虽然大多数样品制备设备通常与色谱耦合，但我们最近考虑将设备直接耦合到质谱仪和/或离子迁移谱，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聚焦分离通道中的离子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导致更高的灵敏度，而且还有助于提高选择性，因为它能够通过向漂移气体中添加适当的化合物(“修饰剂”)来有效地探索团簇的形成。基于这种原理的系统将被设计成足够轻便和紧凑，甚至可以将它们放置在移动电话设备上

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