MRI: Development of a hybrid mass spectrometry platform with mass-selective optical spectroscopy of cryogenic ions

该奖项由主要研究仪器项目和化学研究仪器项目支持。耶鲁大学的马克·约翰逊教授和他的同事詹姆斯·梅尔、斯科特·米勒、帕特里克·霍兰德和尼莱·哈扎里建造了一种新型的混合质谱仪。在离子在没有氧气或水的惰性大气中冷却后，光谱仪能够对离子进行质量选择性隔离，以进行光学光谱表征。该提案的目的是使用一种混合方法，将高分辨率质谱学与红外等光学光谱相结合。这一创新的关键来自于在通常的离子操作(例如串联质谱仪)和允许收集光谱的光学光谱仪之间增加了低温离子处理阶段。该仪器包括用于离子注射的封闭的惰性环境，包括在手套盒中进行样品处理和低温样品制备以延长离子稳定性。它被设计成一种惰性样品轨道离子光谱质谱仪(ISOMSIS)。通常，质谱仪是用于识别和表征嵌入在复杂基质中的少量化学物种的关键分析方法之一。在一个典型的实验中，这些组分流入质谱仪，在那里它们被电离成母离子，并测量它的碎片离子及其质量。这种高度灵敏的技术可以检测和确定复杂混合物中的分子结构。增加一个室，在那里离子可以在分离后冷却，然后插入光谱仪，该光谱仪测量光(如红外光)如何与感兴趣的物种相互作用，大大提高了未知化合物和中间体表征的结构特异性。建立一种新的乐器对于促进经济发展和培养新一代乐器演奏家至关重要。学生们参与和构建过程，并在耶鲁科学之路等外展活动中使用该仪器。研究人员还展示了这个仪器平台在各种活动中所提供的能力，从接触当地社区到与当地化学工业的联系。建造这种混合质谱仪的奖项旨在加强各级的研究和教育。它尤其影响针对研究的研究，研究针对在植物中结合氮素的过程中的酶固氮酶模型化合物。该仪器还可用于氧还原反应的研究。此外，它还有助于发现催化对映体选择性反应的小肽，以及用富含稀土的金属制备催化剂，以制造更环保的材料，促进经济发展。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

This award is supported by the Major Research Instrumentation and the Chemistry Research Instrumentation programs. Professor Mark Johnson from Yale University and colleagues James Mayer, Scott Miller, Patrick Holland and Nilay Hazari built a new type of mixed mass spectrometer. The spectrometer enables mass-selective isolation of ions for optical spectroscopic characterization after the ions are cooled in a chamber having an inert atmosphere without oxygen or water. The aim of the proposal is to use a hybrid approach in which high resolution mass spectrometry is integrated with optical spectroscopies, such as infrared. The key to this innovation derives from the addition of a cryogenic ion processing stage between the usual ion manipulations (for example, tandem mass spectrometry) and the optical spectrometers that allow the collection of spectra. The instrument includes incorporation of an enclosed, inert environment for ion injection that include sample manipulation in a glovebox and low temperature sample preparation to prolong the ion stability. It is designed as an inert sample orbitrap mass spectrometer with ion spectroscopy (ISOMSIS). In general, mass spectrometry (MS) is one of the key analytical methods used to identify and characterize small quantities of chemical species embedded in complex matrices. In a typical experiment, the components flow into a mass spectrometer where they are ionized into the parent ion and its fragment ions and their masses are measured. This highly sensitive technique allows detection and determination of the structure of molecules in a complex mixture. The addition of a chamber where the ions can be cooled after separation followed by insertion into a spectrometer that measure how light (such as infrared light) interacts with species of interest substantially increases the structural specificity in characterization of unknown compounds and intermediates. The building a new instrumentation is essential to improve economic development and to prepare the new generation of instrumentalists. Students participate and the building process and use the instrument in outreach activities such as that Yale Pathways to Science. The investigators also demonstrate the capabilities afforded by this instrumental platform in activities ranging from outreach to the local community and connections to local chemical industry.The award to build this mixed mass spectrometer is aimed at enhancing research and education at all levels. It especially impacts studies directed to study research is directed to the enzyme nitrogenase model compounds in processes that incorporate nitrogen in plants. The instrument is also used for investigations of the oxygen reduction reaction. In addition, it aids in the discovery of small peptides that catalyze enantioselective reactions, and in the preparation of catalysts with earth-abundant metals to make more environmentally friendly materials that will improve economic development.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.