Ion/ion Chemistry and Ion Trap Approaches for the Structural Characterization of the Lipidome

用于脂质组结构表征的离子/离子化学和离子阱方法

• 批准号: 2304386
• 负责人: Scott McLuckey
• 金额: $ 49.5万
• 依托单位: Purdue 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: 2023-08-15 至 2026-07-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2304386&HistoricalAwards=false
• 关键词: Ion; ion; Chemistry; Trap; Approaches

With support from the Chemical Measurement and Imaging Program in the Division of Chemistry, Professor Scott McLuckey and his group at Purdue University are developing novel approaches for the structural characterization of lipid molecules. The reactivities of molecules and the roles that they play are intimately tied to their structures. Molecules comprised of the same atoms but with different linkages between atoms (i.e., isomers) can have markedly different reactivities. The chemistries associated with all forms of life are replete with examples in which isomeric molecules play key and unique roles. As a class of biomolecules, lipids are emerging as highly informative markers of the biological state of an organism. The lipid complement of an organism is referred to as its ‘lipidome’. Many examples of isomerism have been identified in lipidomes, many of which are already known to be biologically significant. However, tools to characterize the structural diversity of the lipidome are lacking. Professor McLuckey and his students are inventing new tools and approaches to characterize the lipidome, which will enable the scientific community to generate a deeper understanding of the chemistry of life.This project seeks to develop novel ion/ion reaction and electrodynamic ion trap approaches for the structural characterization of ions derived from lipids present in complex mixtures. An underlying theme of the work is to employ the most sensitive approach to ionization while using gas-phase ion/ion reactions to convert the initially formed ion-type to alternate ion-types that yield structural details that a single ion-type alone cannot provide. Collision-induced dissociation under a range of conditions will be used to probe the ion-types generated using various reagents. Isomer distinction, for example, will be based on differences in product ion identities and/or abundances and differences in dissociation rates. The even-electron lipid ions generated directly by electrospray ionization will be subjected to reactions that will lead multiple alternate ion-types that include odd-electron ions, metal-containing ions, and combinations thereof. This work has the potential to yield a flexible means for the structural characterization of a variety of lipids present in complex mixtures and, as such, could provide valuable enabling analytical technology for the study of frontline questions in lipidomics and lipid biology.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，普渡大学的Scott McLuckey教授和他的团队正在开发用于脂质分子结构表征的新方法。 分子的反应性和它们所起的作用与它们的结构密切相关。 由相同的原子组成但原子之间具有不同键的分子（即，异构体）可具有显著不同的反应性。 在与所有生命形式相关的化学反应中，同分异构分子扮演着关键而独特的角色。 作为一类生物分子，脂质正在成为生物体生物学状态的高度信息标记。 生物体的脂质补体被称为其“脂质体”。 已在脂质体中鉴定出许多异构现象的实例，其中许多已知具有生物学意义。 然而，缺乏表征脂质体结构多样性的工具。 McLuckey教授和他的学生正在发明新的工具和方法来表征脂质体，这将使科学界对生命的化学有更深入的了解。该项目旨在开发新的离子/离子反应和电动离子阱方法，用于复杂混合物中脂质衍生的离子的结构表征。 这项工作的一个基本主题是采用最敏感的电离方法，同时使用气相离子/离子反应将最初形成的离子类型转换为替代离子类型，从而产生单一离子类型无法单独提供的结构细节。 在一系列条件下的碰撞诱导解离将用于探测使用各种试剂产生的离子类型。 例如，异构体区分将基于产物离子身份和/或丰度的差异以及解离速率的差异。 通过电喷雾电离直接产生的偶电子脂质离子将经历反应，该反应将产生包括奇电子离子、含金属离子及其组合的多种交替离子类型。 这项工作有可能产生一种灵活的手段，用于复杂混合物中存在的各种脂质的结构表征，因此，可以为脂质组学和脂质生物学前沿问题的研究提供有价值的分析技术。该奖项反映了NSF的法定使命，并被认为值得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来支持。