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CAS: Dinuclear Metallacycles as Intermediates in Catalysis

CAS：双核金属环作为催化中间体

基本信息

批准号：
2101931
负责人：
Christopher Uyeda
金额：
$ 47.5万
依托单位：
Purdue 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：
2021-06-01 至 2024-05-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=2101931&HistoricalAwards=false
关键词：
CAS Dinuclear Metallacycles Intermediates Catalysis

项目摘要

With the support of the Chemical Catalysis program in the Division of Chemistry, Dr. Christopher Uyeda of Purdue University is studying catalytic reactions that will improve the efficiency and sustainability of chemical synthesis. There are numerous scientific and technological advances that rely on synthetic organic molecules. For example, the ability to selectively deactivate a protein using a small molecule inhibitor forms the basis for understanding and treating human diseases. Molecules can also store or convert energy, allowing them to be used in devices such as solar cells and batteries. Often, the molecules that are required for these applications have complex structures and are prepared using lengthy synthetic processes. A major challenge in modern chemical synthesis is to improve the efficiency and sustainability of these processes by reducing the number of steps that are required and the amount of waste that is generated. In this project, Dr. Uyeda will address these goals by studying transition metal catalysts that can rapidly generate complex molecules from readily available starting materials, ideally with little to no waste byproducts. A diverse group of undergraduate, graduate, and postdoctoral researchers will be involved this research project. In the process, they will gain technical and non-technical training that will prepare them for future careers in STEM and STEM-adjacent fields. Outreach activities will communicate the impact that catalysis research has on society to a broad audience of other scientists, students, and the general public. Additionally, mentorship activities are geared toward broadening the participation of underrepresented groups in STEM professions.With the support of the Chemical Catalysis program in the Division of Chemistry, Dr. Christopher Uyeda of Purdue University is studying metal–metal bonds as active sites for catalysis. Metallacycles are key catalytic intermediates in many organic transformations, including cycloadditions, bond insertions, and rearrangements. In this project, Dr. Uyeda will explore how dinuclear active sites can be used to access metallacycles with unique catalytic properties. The overarching goal is to use multiple metals to cooperatively activate substrates that are typically inert toward monometallic complexes. Furthermore, the orbital symmetry properties of metal–metal bonds will be leveraged to control chemo-, regio-, and stereoselectivity in multicomponent reactions. This project will involve synthesizing new bimetallic complexes, studying stoichiometric organometallic reactions, and developing selective catalytic transformations. Undergraduate, graduate, and postdoctoral researchers involved in this project will work at the interface of organic and inorganic chemistry. They will gain a fundamental understanding of transition metal chemistry while learning to apply this knowledge to develop useful catalytic reactions. Results from this project will be communicated to a broad audience through review articles, seminars, and podcast interviews. This project will also support outreach activities that engage high school and undergraduate students, with an emphasis on retaining underrepresented students in chemistry.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.

在化学系化学催化项目的支持下，普渡大学的Christopher Uyeda博士正在研究能够提高化学合成效率和可持续性的催化反应。许多科学技术的进步都依赖于合成有机分子。例如，使用小分子抑制剂选择性地使蛋白质失活的能力构成了理解和治疗人类疾病的基础。分子还可以储存或转换能量，使它们能够用于太阳能电池和电池等设备。通常，这些应用所需的分子具有复杂的结构，并且需要使用冗长的合成过程来制备。现代化学合成的一个主要挑战是通过减少所需步骤的数量和产生的废物量来提高这些过程的效率和可持续性。在这个项目中，Uyeda博士将通过研究过渡金属催化剂来实现这些目标，这种催化剂可以从现成的起始材料中快速生成复杂的分子，理想情况下几乎没有废物副产品。本科生、研究生和博士后研究人员将参与这项研究项目。在此过程中，他们将获得技术和非技术培训，为他们未来在STEM和STEM相关领域的职业生涯做好准备。外联活动将把催化研究对社会的影响传达给广大的其他科学家、学生和公众。此外，指导活动旨在扩大STEM专业中代表性不足群体的参与。在化学系化学催化项目的支持下，普渡大学的Christopher Uyeda博士正在研究金属-金属键作为催化的活性位点。金属环是许多有机转化的关键催化中间体，包括环加成、键插入和重排。在这个项目中，Uyeda博士将探索如何利用双核活性位点来获得具有独特催化性能的金属循环。总体目标是使用多种金属来协同激活通常对单金属配合物惰性的底物。此外，金属-金属键的轨道对称性将被用来控制多组分反应中的化学选择性、区域选择性和立体选择性。该项目将包括合成新的双金属配合物，研究化学计量有机金属反应，以及开发选择性催化转化。参与本项目的本科生、研究生和博士后研究人员将在有机和无机化学的界面工作。他们将获得过渡金属化学的基本理解，同时学习应用这些知识来开发有用的催化反应。这个项目的结果将通过评论文章、研讨会和播客采访传达给广大受众。该项目还将支持面向高中生和本科生的推广活动，重点是保留在化学领域代表性不足的学生。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。