Highly Robust Transition Metal Complexes with E-Substituted Phosphines (E = Si, Ge, Sn) Grafted onto Metal-Organic Frameworks for Dehydrogenative Functionalization

在化学系化学催化项目的支持下，密西西比州立大学的Virginia Montiel-Palma博士正在研究将硅以脱氢方式添加到烯烃底物上的催化剂，以形成用于制药、医疗和牙科植入物以及许多日常材料的有价值的构建块。将催化剂从研究实验室转化为工业是一个巨大的挑战。催化剂不仅通常必须固定在固体载体上，而且材料需要坚固并保持所需的性能。通过使用最先进的方法来研究这些催化剂在分子水平上是如何工作的，Montiel-Palma博士和她的研究小组正在应用这一基本见解来设计更有效、更经济的新型催化剂。还对催化剂进行了特定的分子变化，以确定其对反应性和稳定性的影响。与密西西比移民教育中心合作，蒙蒂埃尔-帕尔马博士还为K-12年级的学生提供了一系列非正式的STEM课程和活动。这些学生是农民工的子女，他们的收入来源是农业、渔业和其他主要活动。他们是我们社会中最脆弱的群体之一。Montiel-Palma博士利用这个活动来讨论科学话题，旨在激励这些学生完成中学教育，丰富他们的教育途径。Virginia Montiel-Palma和她的研究小组将对接枝到金属有机骨架（MOF）载体上的脱氢硅基化催化剂进行系统研究。催化剂的钳状配体位点以及MOF的孔径、化学性质和结构稳定性都得到了调整。一个多方面的表征计划被用来询问催化材料和利用这些材料脱氢硅氧烷化的机制。从这些调查中获得的见解将用于进一步告知迭代催化剂开发过程中的结构变化。综上所述，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稳健的脱氢硅基化系统。这些研究将由研究生和本科生组成的团队进行，他们将利用最先进的技术进行该项目的综合、机械和计算方面的研究。这些经验将提供多方面的培训，以支持多元化的员工队伍。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 Catalysis Program in the Division of Chemistry, Dr. Virginia Montiel-Palma of Mississippi State University is investigating catalysts that add silicon to alkene substrates in a dehydrogenative fashion to form valuable building blocks for pharmaceutical application, medical and dental implants, and many everyday materials. Translating catalysts from the research laboratory to industry is a huge challenge. Not only do catalysts often have to be immobilized onto a solid support, but the material needs to be robust and retain the desired properties. By using state-of-the-art methods to study how these catalysts work at the molecular level, Dr. Montiel-Palma and her research group are applying this fundamental insight to design new improved catalysts that are more active and cost-efficient. Specific molecular changes are also being made to the catalysts to determine their effect on their reactivity and stability. In partnership with the Mississippi Migrant Education Center, Dr. Montiel-Palma is also giving a series of informal STEM lessons and activities for students K-12. These students are children of migratory workers with income sources in agriculture, fisheries, and other primary activities. They constitute one of the most vulnerable sectors of our society. Dr. Montiel-Palma is using this activity to address scientific topics aimed at motivating these students to finish secondary education and enrich their educational pathways.Dr. Virginia Montiel-Palma and her research group will conduct a systematic study of dehydrosilylation catalysts grafted to metal-organic framework (MOF) supports. The catalysts are being tuned at both their pincer-like ligand sites as well as in the pore size, chemical properties, and structural stability of the MOF. A multifaceted characterization plan is being used to interrogate the catalytic materials and the mechanism of dehydrosilylation using these materials. The insights gained from these investigations are to be used to further inform structural changes in an iterative catalyst development process. Taken together, these activities are expected to provide a foundational profile of the catalyst system and help design more efficient and robust dehydrosilylation systems. These studies will be conducted with a team of graduate and undergraduate students carrying out the synthetic, mechanistic, and computational aspects of this project utilizing state-of-the-art technologies. These experiences will provide multi-faceted training in support of a diverse workforce.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.