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

具有 E 取代膦 (E = Si、Ge、Sn) 的高鲁棒过渡金属配合物接枝到金属有机框架上用于脱氢功能化

• 批准号: 2102689
• 负责人: Virginia Montiel-Palma
• 金额: $ 41.12万
• 依托单位: Mississippi State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-05-01 至 2024-04-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2102689&HistoricalAwards=false
• 关键词: Highly; Robust; Transition; Metal; Complexes

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.

在化学系化学催化计划的支持下，密西西比州立大学的弗吉尼亚·蒙蒂尔-帕尔马博士正在研究以脱氢方式将硅添加到烯烃基质中的催化剂，以形成用于制药应用、医疗和牙科植入物以及许多日常材料的有价值的积木。将催化剂从研究实验室转化为工业是一个巨大的挑战。催化剂不仅经常需要固定在固体载体上，而且材料还需要坚固耐用并保持所需的性质。通过使用最先进的方法在分子水平上研究这些催化剂的工作原理，蒙蒂埃尔-帕尔马博士和她的研究小组正在应用这一基本见解来设计更具活性和成本效益的新型改进型催化剂。还对催化剂进行了特定的分子变化，以确定它们对反应活性和稳定性的影响。蒙蒂埃尔-帕尔马博士还与密西西比州移民教育中心合作，为K-12年级的学生提供了一系列非正式的STEM课程和活动。这些学生是移民工人的子女，他们的收入来源是农业、渔业和其他主要活动。他们构成了我们社会最脆弱的群体之一。Montiel-Palma博士正在利用这一活动来解决旨在激励这些学生完成中学教育并丰富他们的教育途径的科学主题。维吉尼亚·蒙蒂埃尔·帕尔马和她的研究小组将对嫁接到金属有机骨架(MOF)载体上的脱氢硅化催化剂进行系统研究。催化剂在其钳状配体位置以及MOF的孔大小、化学性质和结构稳定性方面进行了调整。一个多方面的表征计划正被用来询问催化材料和使用这些材料的脱氢硅烷反应机理。从这些研究中获得的见解将被用来进一步告知迭代催化剂开发过程中的结构变化。综上所述，这些活性有望提供催化剂体系的基本概况，并有助于设计更有效和更强大的脱氢硅烷化系统。这些研究将与一组研究生和本科生一起进行，他们利用最先进的技术进行这个项目的合成、机械和计算方面的工作。这些经验将提供多方面的培训，以支持不同的劳动力。这一奖项反映了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。

项目成果

SO 2 capture enhancement in NU-1000 by the incorporation of a ruthenium gallate organometallic complex

通过掺入没食子酸钌有机金属络合物增强 NU-1000 中的 SO 2 捕获

• DOI: 10.1039/d1ce01076j
• 发表时间: 2021
• 期刊: CrystEngComm
• 影响因子: 3.1
• 作者: García Ponce, Jorge;Díaz-Ramírez, Mariana L.;Gorla, Saidulu;Navarathna, Chanaka;Sanchez-Lecuona, Gabriela;Donnadieu, Bruno;Ibarra, Ilich A.;Montiel-Palma, Virginia
• 通讯作者: Montiel-Palma, Virginia