Multifunctional Metal-Organic Frameworks for Cooperative Catalysis

用于协同催化的多功能金属有机框架

• 批准号: 2102554
• 负责人: Wenbin Lin
• 金额: $ 50万
• 依托单位: University of Chicago
• 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: 2021-08-01 至 2024-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2102554&HistoricalAwards=false
• 关键词: Multifunctional; Metal; Organic; Frameworks; Cooperative

With the support of the Chemical Catalysis Program in the Division of Chemistry, Professor Wenbin Lin of the University of Chicago is developing new metal-organic frameworks (MOFs) as cooperative catalysts for chemical synthesis. Cooperative catalysts accelerate two or more steps in concert, which increases the efficiency of chemical bond construction and thereby facilitates multi-step processes. Although solid catalysts are used in many catalytic reactions, they are difficult to precisely engineer for cooperative catalysis due to the inability to install spatially-controlled catalytic sites. Professor Lin and his research group are addressing this problem by using recent advances in MOFs to build multifunctional MOFs for cooperative catalysis. A bottom-up approach is being used to build recyclable and reusable multifunctional MOFs with cooperative catalytic sites and to optimize these structures for important chemical synthesis applications in the pharmaceutical, agrochemical, and fine-chemical industries. The structure-function relationships between the MOFs and the targeted catalytic processes are being studied to support continued design improvements. These activities are further being used to support research opportunities for undergraduate and high school students to improve engagement in STEM disciplines.Many natural enzymes possess multiple precisely engineered active sites to cooperatively catalyze multiple transformations of simple molecules, such as carbon dioxide, to complex molecules, such as carbohydrates, with high efficiency and selectivity. Despite the importance of solid catalysts in the production of commodity chemicals, they cannot be used for cooperative catalysis because of the lack of methods to precisely engineer uniform and synergistic catalytic centers in a spatially controlled manner in these solids. Professor Lin and his research group will utilize synthetic strategies to prepare new MOFs with large open channels/pores and multifunctional active sites for cooperative catalyst combinations including: (ii) Lewis acid and transition metal catalysts, (ii) photoredox and transition metal catalysts, or (iii) photoredox and Lewis/Bronsted acid catalysts. These MOFs will then being examined for C-C and C-heteroatom cross-coupling, olefin metathesis, and olefin oligomerization reactions. The intrinsic MOF properties are being leveraged with the aim of discovering viable new catalytic systems and developing biomimetic materials with cooperative functions. This research program will also provide important training for a diverse group of postdoctoral researchers and graduate students in the development of sustainable chemical processes for environmental stewardship.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，芝加哥大学的林文斌教授正在开发新的金属有机框架（MOFs）作为化学合成的协同催化剂。协同催化剂协同加速两个或更多个步骤，这增加了化学键构建的效率，从而促进多步骤过程。虽然固体催化剂被用于许多催化反应中，但由于不能安装空间控制的催化位点，它们难以精确地设计用于协同催化。林教授和他的研究小组正在利用MOFs的最新进展来解决这个问题，以构建用于协同催化的多功能MOFs。一种自下而上的方法正在被用来构建可回收和可重复使用的多功能MOFs与合作催化位点，并优化这些结构的重要化学合成应用在制药，农业化学品和精细化工行业。正在研究MOFs和目标催化过程之间的结构-功能关系，以支持持续的设计改进。许多天然酶具有多个精确设计的活性位点，可以协同催化简单分子（如二氧化碳）向复杂分子（如碳水化合物）的多种转化，具有高效率和高选择性。尽管固体催化剂在商品化学品生产中很重要，但它们不能用于协同催化，因为缺乏方法以空间控制的方式在这些固体中精确设计均匀且协同的催化中心。林教授及其研究小组将利用合成策略制备具有大开放通道/孔和多功能活性位点的新型MOFs，用于协同催化剂组合，包括：（ii）刘易斯酸和过渡金属催化剂，（ii）光氧化还原和过渡金属催化剂，或（iii）光氧化还原和刘易斯/布朗斯台德酸催化剂。然后将检查这些MOF的C-C和C-杂原子交叉偶联、烯烃复分解和烯烃低聚反应。利用固有的MOF特性，目的是发现可行的新催化体系和开发具有协同功能的仿生材料。该研究项目还将为不同的博士后研究人员和研究生提供重要的培训，以开发可持续的化学过程，促进环境管理。该奖项反映了NSF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。