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和化学研究仪器计划支持。来自耶鲁大学的Mark约翰逊教授和他的同事James Mayer、Scott米勒、帕特里克霍兰德和Nilay Hazari建造了一种新型的混合质谱仪。在离子在具有不含氧或水的惰性气氛的腔室中冷却之后，光谱仪能够实现用于光学光谱表征的离子的质量选择性隔离。该提案的目的是使用一种混合方法，其中高分辨率质谱法与光学光谱法（如红外光谱法）相结合。这一创新的关键在于在通常的离子操作（例如串联质谱）和允许收集光谱的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入的封闭惰性环境，包括手套箱中的样品操作和低温样品制备，以延长离子稳定性。它被设计为一个惰性样品轨道阱质谱仪与离子光谱（ISOMSIS）。一般来说，质谱（MS）是用于识别和表征嵌入复杂基质中的少量化学物质的关键分析方法之一。在典型的实验中，组分流入质谱仪，在那里它们被电离成母离子及其碎片离子，并测量它们的质量。这种高灵敏度的技术可以检测和确定复杂混合物中分子的结构。添加一个腔室，其中离子可以在分离后冷却，然后插入测量光（如红外光）如何与感兴趣的物质相互作用的光谱仪中，这大大增加了未知化合物和中间体表征的结构特异性。建立一个新的仪器是必不可少的，以促进经济发展和准备新一代的乐器演奏家。学生参与和建设过程，并使用外展活动，如耶鲁大学科学之路的仪器。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，包括与当地社区的联系和与当地化学工业的联系。建造这个混合质谱仪的奖项旨在加强各级的研究和教育。它特别影响了针对研究的研究是针对固氮酶模型化合物的过程中，将氮在植物中。该仪器还用于研究氧还原反应。此外，该奖项还有助于发现催化对映体选择性反应的小肽，以及利用地球上丰富的金属制备催化剂，以制造更环保的材料，从而促进经济发展。该奖项反映了NSF的法定使命，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。

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.