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.

在化学分区化学测量和成像计划的支持下，斯科特·麦克卢基（Scott McLuckey）教授及其在普渡大学（Purdue University）的小组正在开发脂质分子结构表征的新方法。分子的反应性及其扮演的角色与它们的结构密切相关。包括相同原子的分子，但在原子（即异构体）之间具有不同的联系可能具有明显不同的反应性。与所有形式的生命相关的化学作品被替换为异构分子扮演关键和独特角色的例子。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。生物体的脂质完成称为其“脂质术”。许多异构体的例子已经在脂质组中鉴定出来，其中许多已经众所周知具有生物学意义。但是，缺乏表征脂质仪的结构多样性的工具。麦克卢基（McLuckey）教授和他的学生正在发明新的工具和方法来表征脂质组，这将使科学界能够对生命的化学产生更深入的了解。该项目旨在开发新的离子/离子反应和电动力学离子陷阱方法，以使其从复杂混合物中产生的脂质产生的离子衍生而成。这项工作的一个基本主题是使用最敏感的方法进行电离，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，从而产生单个离子型单独的结构细节，而单一离子类型则无法提供。在一系列条件下碰撞诱导的解离将用于探测使用各种试剂产生的离子类型。例如，异构体的区别将基于产品离子身份和/或抽象和解离率差异的差异。电喷雾离子化直接产生的均匀的脂质离子将受到反应，该反应将导致多种替代离子类型，包括奇异电子离子，含金属的离子及其组合。这项工作有可能产生一种灵活的手段，用于复杂混合物中各种脂质的结构表征，因此，可以为研究脂质组学和脂质生物学的一线问题提供有价值的分析技术，以反映NSF的法定任务，反映了通过评估基金会的诚实评估和广泛的crtial and crowia and crowia and tocriatial and tocriatial and tocriatial and tocriatial and tocrit和广泛的支持。