Panoptic Mass Spectrometry

全景质谱法

• 批准号: 2305057
• 负责人: Abraham Badu-Tawiah
• 金额: $ 48.5万
• 依托单位: Ohio State University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-07-01 至 2026-06-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2305057&HistoricalAwards=false
• 关键词: Panoptic; Mass; Spectrometry

With support from the Chemical Measurement and Imaging Program in the Division of Chemistry, Professor Abraham Badu-Tawiah and his research group at Ohio State University is developing a new mass spectrometry platform to enable the analysis of all kinds of chemical species in ultra-small sample volumes in a single experiment, a potentially significant advance in metabolomics-related technology. Mass spectrometers measure mass-to-charge ratio of chemical species, a universal parameter that should make this analytical technique widely applicable across diverse fields. Currently, this capability is realized using different ion sources for different compounds. The goal of this research is to develop a single universal (panoptic) ion source that can analyze a wide range of chemical species. The idea of universality is expanded from the detection of diverse chemicals to include the analyses of liquid-, solid-, and vapor-phase samples, all using the same panoptic ion source. The subjects of chemical instrumentation, new ionization methods, and the processing of ultra-small sample volumes are well suited for the education of scientists at all levels. Education-outreach activities are fully integrated and are designed to directly impact students in the early stages (K-12) of their educational experience. Due to the simplicity of the proposed experiments, this group is well-positioned to introduce students – particularly from groups underrepresented in the STEM (science, technology, engineering and mathematics) fields – to interdisciplinary science, build their confidence and encourage them to think of science in a broad, discovery-based manner. Challenges associated with small volume analysis include inefficient fractionation prior to analysis, leading to significant matrix effects. The intellectual merits of this research revolve around the tandem development of three novel concepts. First, a dynamic electrospray process will enable temporally distinct ionization mechanisms to be initiated from a single emitter to ionize different compounds, as well as to offer temporal separation of chemical species involved, based on solution-phase mobility. Second, the plasma ionization included in the dynamic spray process will allow analysis of polar and nonpolar compounds in all three states of matter (i.e., liquid-, solid-, and vapor-phase samples), thus establishing the first panoptic (universal) ion source. Third, the specific mechanisms of ion generation (particularly those based on ambient plasma chemistry) will enable mass spectrometer operation in four conceivable modes (four quadrant) to detect all possible ion types (M•+, M•-, [M+H]+, [M-H]+, [M-H]-, [M+nH]n+) originating from the panoptic ion source. Therefore, a new panoptic mass spectrometry platform will be created in which the universal ion source will be coupled with a four-quadrant mass analyses. We expect this research to transform direct infusion mass spectrometry into a high-performance analytical system in which low-resolution mass spectrometers can be used more effectively for complex mixture analysis. This capability is made possible by enabling online sample processing, including temporal separation and chemical reactions. The specific reactions selected (e.g., charge inversion, transesterification, and epoxidation of C=C bonds) have potential to expand the scope of lipidomics by enabling lipid analysis at multiple isomer levels.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

在化学系化学测量和成像项目的支持下，俄亥俄州州立大学的Abraham Badu-Tawiah教授和他的研究小组正在开发一种新的质谱平台，以便在一个实验中分析超小样品体积中的所有化学物质，这是代谢组学相关技术的潜在重大进步。质谱仪测量化学物质的质荷比，这是一个通用参数，应该使这种分析技术广泛适用于不同的领域。目前，这种能力是通过使用不同化合物的不同离子源来实现的。这项研究的目标是开发一个单一的通用（panoptic）离子源，可以分析范围广泛的化学物种。普适性的概念从不同化学品的检测扩展到包括液相、固相和气相样品的分析，所有这些都使用相同的全景离子源。化学仪器，新的电离方法和超小样品体积的处理的主题非常适合各级科学家的教育。教育推广活动是完全一体化的，旨在直接影响学生在早期阶段（K-12）的教育经验。由于拟议实验的简单性，该小组有能力向学生-特别是来自STEM（科学，技术，工程和数学）领域代表性不足的群体-介绍跨学科科学，建立他们的信心，并鼓励他们以广泛的，基于发现的方式思考科学。与小体积分析相关的挑战包括分析前分馏效率低下，导致显着的基质效应。这项研究的智力价值围绕着三个新概念的串联发展。首先，动态电喷雾过程将使时间上不同的电离机制，从一个单一的发射器启动，以激发不同的化合物，以及提供时间分离的化学物质的基础上，溶液相的流动性。第二，包括在动态喷雾过程中的等离子体电离将允许分析所有三种物质状态（即，液相、固相和气相样品），从而建立了第一个全景（通用）离子源。第三，离子生成的特定机制（特别是基于环境等离子体化学的那些）将使得质谱仪能够以四种可想到的模式（四象限）操作，以检测源自全景离子源的所有可能的离子类型（M·+、M·-、[M+H]+、[M-H]+、[M-H]-、[M+nH]n+）。因此，将创建一个新的泛光质谱平台，其中通用离子源将与四象限质量分析耦合。我们希望这项研究能够将直接注入质谱法转变为一种高性能的分析系统，在这种系统中，低分辨率质谱仪可以更有效地用于复杂混合物的分析。通过启用在线样品处理，包括时间分离和化学反应，这种能力成为可能。选择的具体反应（例如，该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。