High Performance Analysis of Complex Organic Mixtures

我们研究计划的主要重点是设计高度自动化、小型化和集成化的仪器，用于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、鉴定和定量。发展新的分析分离方法以快速有效地测定痕量有机物质对当代分析化学家提出了重大挑战，不仅对化学，而且对生物和环境科学以及医学都具有重大意义。传统上，痕量方法的一个关键组成部分是缓慢的、劳动密集型的采样和样品准备步骤。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。这项工作将导致高通量的实验室测定，以及方便的现场和体内分析。我们努力的长期目标是将分析化学“现场”转移到样品所在的位置，以促进低成本、快速和准确的测量和监测。为此，我们正在研究膜、针和纤维的配置。我们研究的一个重要的基本组成部分是通过研究主要的传质步骤，建立数学模型，并使用实验数据验证所述模型，从而增加我们对萃取过程的理解。这种方法使我们能够开发方便的提取设备、有效的方法和适当的校准程序。在发现基金支持的下一个五年研究计划中，我们建议对直接SPME采样中的置换现象有一个基本的了解，以将其应用范围扩大到更具挑战性的任务，包括不稳定癌症生物标记物的代谢组学研究、微生物学中的代谢组学研究、唾液的体内和体外最小侵入性SPME采样，以及水下SPME对生物重要分子的浓缩。我们还将开发冷纤维纳米颗粒收集和带有吸附界面的膜提取(MESI)用于呼气分析的应用。研究的另一个主要方向是设计高效的短毛细管分离技术的全柱成像检测方法。成像工作的扩展将导致纹影显微镜技术，其中信号与浓度梯度成正比，而不是浓度水平，这将强调所研究的生命系统中的动力学。这种方法可能会成为生命系统微观研究的标准特征。该计划将涉及研究合作，无论何时，它都有助于实现我们的研究目标。例如，与新加坡南洋理工大学的Newman Sze教授共同研究黑色素瘤生物标记物的发现，将有助于我们与多伦多综合医院的Marcelo Cypel教授的团队合作，在那里，外科医生开发独特的原位癌症治疗方法。我们在水下SPME采样方面的基础工作将与滑铁卢大学的Mark Seros教授在Grand River生态系统调查中、维多利亚大学的Verena TunNicliffe教授在使用遥控潜水器进行水下发现方面以及来自梅西纳大学的Luigi Mondello教授在地中海大型蛤累积污染物调查方面进行务实合作。一名本科生、四名研究生、三名博士后和一名研究助理将接受突破性分析技术开发和应用方面的培训。

The primary focus of our research program is to design highly automated miniaturized and integrated instrumentation for the isolation of organic materials from complex matrices, as well as the subsequent separation, identification and quantification of these species. The development of new analytical separation methodology for rapid and efficient determination of organic substances in trace amounts poses a significant challenge to the contemporary analytical chemist, and has major implications not only for chemistry, but also for the biological and environmental sciences as well as medicine. Traditionally, a key component of trace methodology has been slow, labour-intensive sampling and sample preparation steps. We are actively pursuing solvent-free, “green” approaches that can integrate both sampling and sample preparation steps. This effort will lead to high throughput laboratory determination, as well as convenient field and in-vivo analysis. Long-term objective of our efforts is to move analytical chemistry "on-site", where the sample is located to facilitate low cost, rapid and accurate measurement and monitoring. We are investigating membrane, needle, and fibre configurations for this purpose. A significant, fundamental component of our research is to increase our understanding of the extraction processes by investigating primary mass transfer steps, developing mathematical models, and verifying said models by using experimental data. This approach allows us to develop convenient extraction devices, effective methods, and appropriate calibration procedures. In the next 5-year research program supported by the Discovery grant, we propose to develop a fundamental understanding of displacement phenomenon in direct SPME sampling to broaden the scope of its application to more challenging tasks, including metabolomics investigation of unstable cancer biomarkers, metabolomics investigations in microbiology, in-vivo and ex-vivo minimum invasive SPME sampling of saliva, and underwater SPME enrichment of biologically significant molecules. We will also develop an application of cold-fibre nanoparticle collection and Membrane Extraction with Sorbent Interface (MESI) for breath analysis. The other major direction of the research is to design whole column imaging detection methods for high efficiency short capillary separation techniques. The extension of the imaging work will result in the Schlieren Microscope technique, where the signal is proportional to concentration gradient rather than concentration level, which will emphasize the dynamics in the investigated living system. This approach could become a standard feature of microscopic investigation of living systems. The program will involve research collaboration whenever it assists in achieving our research objective. For example, the joint research effort with Professor Newman Sze from Nanyang Technological University from Singapore on melanoma biomarker discovery will assist our work with Professor Marcelo Cypel’s group at Toronto General Hospital, where surgeons develop unique in situ cancer treatment. Our fundamental work on underwater SPME sampling will be explored practically in collaboration with Professor Mark Servos from University of Waterloo in the Grand River ecosystem investigation, Professor Verena Tunnicliffe, from the University of Victoria in underwater discovery using remotely operated underwater vehicle, and Professor Luigi Mondello, from the University of Messina in investigation of accumulation of contaminants by large clams in Mediterranean Sea. One undergraduate, four graduate, three postdoctoral students and a research associate will be trained in the development and application of groundbreaking analytical technologies.