Photodissociation and Ion Trap Mass Spectrometry

在这个由化学部化学测量和成像项目资助的奖项中，Brodbelt教授和她的学生将开发光解与化学衍生化方法相结合的方法，这些方法可以向分子添加发色团和/或电荷位点，以改变离子碎片模式。质谱已成为生物分子结构表征最通用的方法之一，提高质谱策略的选择性仍然是一个优先考虑的问题。这项工作将遵循一个主题，旨在通过使用结合靶向选择性的离子激活方法来表征生物分子的结构，同时也为理解位点特异性发色团对离子激活的影响建立一个框架。主要目标包括电荷状态对解离效率的评估，发色团的附着以提高解离效率，选择性可切割键与分子的结合，以及用于蛋白质高通量分析的光解离的发展。除了这项建议的重要科学目标之外，未来科学家的教育也是具有长期影响的同样重要的成果。需要发展更好的分析工具，包括在提议的工作中所追求的质谱策略，来阐明负责许多生物功能的分子结构，例如对抗病毒和心脏肌肉收缩的抗体。这项工作的预期收益包括：1)对分析化学和生物质谱领域未来科学家的培训和教育，以及2)开发创新的基于激光的生物分子结构表征策略，如肽、蛋白质、碳水化合物和核酸。

In this award, funded by the Chemical Measurement and Imaging Program of the Chemistry Division, Professor Brodbelt and her students will develop photodissociation in conjunction with chemical derivatization methods that add chromophores and/or charge sites to molecules in order to modify ion fragmentation patterns. Mass spectrometry has become one of the most versatile methods for structural characterization of biological molecules, and enhancing the selectivity of mass spectrometric strategies remains a priority. This work will follow a theme aimed at the structural characterization of biological molecules by using ion activation methods that incorporate targeted selectivity, while also building a framework for understanding the impact of site-specific chromophores on ion activation. The primary goals include the evaluation of charge state on dissociation efficiency, the attachment of chromophores to enhance dissociation efficiencies, the incorporation of selectively cleavable bonds into molecules, and the development of photodissociation for high throughput analysis of proteins. In addition to the important scientific goals of this proposal, the education of future scientists is an equally significant outcome with long-term impact. The development of better analytical tools, including the mass spectrometric strategies pursued in the proposed work, is needed to elucidate the structures of molecules responsible for many biological functions, such as antibodies that fight viruses and muscle contraction in the heart. The anticipated benefits arising from the proposed work include: 1) the training and education of future scientists in the area of analytical chemistry and biological mass spectrometry, and 2) the development of innovative laser-based strategies for structural characterization of biological molecules such as peptides, proteins, carbohydrates, and nucleic acids.