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

密西西比州立大学的Virginia Montiel-Palma在化学系化学合成项目和促进竞争研究的既定项目（EPSCoR）的支持下，正在研究从汽油和石油原料中常见的芳香族化合物中去除氮的催化剂。芳香族含n化合物，其中一些会对环境和健康产生负面影响，在目前的工业条件下很难从石油中去除。因此，开发促进这些化合物中C-N键断裂的催化剂是一个巨大的挑战。在这个项目中，设计了包含两种金属的催化剂候选物，在温和的条件下与芳香含n化合物中的C-N键反应并破坏它们。就更广泛的影响而言，PI将继续积极参与密西西比移民教育中心，在那里她参与了为移民工人子女的K-12学生提供科学教育的努力。这些努力的目的是通过解决丰富教育途径并激励学生完成和继续中学以上教育的科学课题，来消除教育不公平现象。该项目将包括系统地研究由晚期过渡金属和13族金属制成的杂双金属配合物对含氮芳香化合物的加氢作用。在某些配合物中，过渡金属与芳香环结合，而N原子直接与主基团金属结合。这种特殊的排列可以在低氢压力下使碳氮键断裂。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精确作用，以及它发生的机制。这些活动有望提供催化剂系统的基础概况，并有助于设计更有效和更坚固的加氢脱氮催化剂。参与该项目的研究生和本科生将在从事这项研究的过程中获得综合、机械和计算方法方面的经验。该奖项反映了美国国家科学基金会的法定使命，并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。

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.