CAREER: Heterobimetallic Complexes for Facile Hydrodenitrogenation Processes with Low Hydrogen Intake

在化学系化学合成计划和刺激竞争研究既定计划（EPSCoR）的支持下，密西西比州立大学的Virginia Montiel-Palma正在研究从汽油和石油原料中常见的芳族化合物中去除氮的催化剂。在目前的工业条件下，很难从石油中除去含芳族氮化合物，其中一些化合物可能对环境和健康产生负面影响。因此，开发促进这些化合物中C-N键裂解的催化剂是一个巨大的挑战。在这个项目中，催化剂的候选人，包括两种金属的设计反应，并打破芳香族含N化合物中的C-N键在温和的条件下。就更广泛的影响而言，PI将继续积极与密西西比移民教育中心合作，参与为移民工人子女的K-12学生提供科学教育的努力。这些努力的目的是消除教育不公平现象，解决科学问题，丰富教育途径，激励学生完成并继续接受中学以上教育，该项目将包括系统研究用后过渡金属和第13族金属制成的杂环化合物氢化含氮芳族化合物。在这些络合物中的一些中，过渡金属结合到芳环，而N原子直接结合到主族金属。这种特殊的安排预计将允许在低氢压力下的C-N键的断裂。一个多方面的表征计划将被用来询问金属配位模式在氢解反应中的确切作用，以及它发生的机制。这些活动预计将提供一个基本的催化剂系统的配置文件，并在更有效和强大的加氢脱氮催化剂的设计援助。 参与该项目的研究生和本科生将获得合成，机械和计算方法学方面的经验，以进行这项研究。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智力价值和更广泛的影响审查标准进行评估。

With the support of the Chemical Synthesis Program in the Division of Chemistry and the the Established Program to Stimulate Competitive Research (EPSCoR), Virginia Montiel-Palma of Mississippi State University is investigating catalysts that remove nitrogen from aromatic compounds commonly present in gasolines and petroleum feedstocks. Aromatic N-containing compounds, some of which can have a negative environmental and health impact, are difficult to remove from petroleum under current industry conditions. Thus, developing catalysts that facilitate the cleavage of C-N bonds in these compounds is a huge challenge. In this project, catalyst candidates that incorporate two metals are designed to react with and break the C-N bonds in aromatic N-containing compounds under mild conditions. In terms of broader impacts, the PI will continue to be actively engaged with the Mississippi Migrant Education Center where she participates in efforts to reach and provide science education to K-12 students who are children of migratory workers. These efforts are aimed at fighting educational inequities by addressing scientific topics that enrich the educational pathways and motivate students to complete and continue their education beyond the secondary level.This project will involve a systematic study of the hydrogenation of nitrogen-containing aromatic compounds by heterobimetallic complexes made of a late transition metal and a group-13 metal. In some of these complexes, the transition metal binds to an aromatic ring, while the N atom binds directly to the main group metal. This particular arrangement is expected to allow for the scission of the C-N bonds at low hydrogen pressures. A multifaceted characterization plan will be used to interrogate the precise role of the metal coordination modes in the hydrogenolysis reaction, as well as the mechanism by which it occurs. These activities are expected to provide a foundational profile of the catalyst system and aid in the design of more efficient and robust hydrodenitrogenation catalysts. A diverse group of graduate and undergraduate students involved in the project will gain experience in synthetic, mechanistic, and computational methodologies in pursuing this research.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.