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

在化学系化学合成计划和既定的刺激竞争研究计划(EPSCoR)的支持下，密西西比州立大学的弗吉尼亚·蒙蒂埃尔-帕尔马正在研究从汽油和石油原料中常见的芳香族化合物中脱除氮的催化剂。在目前的工业条件下，芳香族含氮化合物很难从石油中去除，其中一些化合物可能会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键断裂的催化剂是一个巨大的挑战。在这个项目中，包含两种金属的候选催化剂被设计成在温和的条件下与芳香族含氮化合物中的C-N键反应并断裂。在更广泛的影响方面，国际移民联合会将继续积极参与密西西比州移民教育中心的工作，在那里她参与努力，接触作为移民工人子女的K-12学生，并向他们提供科学教育。这些努力的目的是解决教育不平等问题，解决丰富教育途径的科学问题，并激励学生完成和继续中学以后的教育。该项目将涉及系统地研究由后过渡金属和13族金属组成的异双金属络合物对含氮芳香族化合物的氢化作用。在其中一些配合物中，过渡金属与芳环结合，而N原子直接与主族金属结合。这种特殊的安排有望在低氢压下允许C-N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确切作用，以及它发生的机理。这些活动预计将提供催化剂系统的基本概况，并有助于设计更有效和更坚固的加氢脱氮催化剂。参与该项目的不同的研究生和本科生将在从事这项研究的过程中获得合成、机械和计算方法方面的经验。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。

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.