Experimental and Computational Studies of Bifunctional Organometallic Catalysis

双功能有机金属催化的实验和计算研究

• 批准号: 2102623
• 负责人: Yong Yan
• 金额: $ 55万
• 依托单位: San Diego State University Foundation
• 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: 2021-11-01 至 2024-10-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2102623&HistoricalAwards=false
• 关键词: Experimental; Computational; Studies; Bifunctional; Organometallic

With the support of the Chemical Catalysis Program in the Division of Chemistry, Professors Douglas B. Grotjahn and Andrew L. Cooksy of San Diego State University are performing research aimed at determining the best catalysts for new reactions that can be used to make organic compounds of interest for a variety of applications, including pharmaceuticals, materials, and biology. To accomplish this, many catalysts that contain a metal and a larger non-metal portion (ligand) will be made and tested, to determine what combinations of metals and ligands will yield the best performing catalysts. In addition, fundamental studies of how the catalysts operate on the molecular level will be performed. This grant will support the training of several young investigators in the field of catalysis. Because catalysis accounts for a third of global GDP and a majority of chemical products and chemical processes, the discovery of new or improved catalysts for organic reactions and new mechanisms has great practical importance, contributing to economic development and recovery. As in the previous grant period, practical catalysts will be developed and improved. Also, to broaden public understanding of catalysis, the PIs and the graduate students will introduce the concept into an existing and highly successful high school outreach program.With the support of the Chemical Catalysis Program in the Division of Chemistry, Professors Douglas B. Grotjahn and Andrew L. Cooksy of San Diego State University will employ design principles of Nature’s enzymes, particularly hydrogen bonding and proton transfer, to accelerate (often by more than 1000-fold) organometallic catalysis and reactions by new mechanisms. Ligands containing proton-donating or hydrogen-bonding groups will be synthesized and combined with a variety of metal precursors to form their metal derivatives for catalysis. Interactions of these pendant groups with nonpolar and polar reactants, intermediates, or transition states are expected to create faster catalysts. The focus will be mostly on waste-free addition or isomerization reactions, with several goals: (1) integrate the use of computer-based molecular predictions before and after catalyst discovery; (2) build and apply a toolbox of alkene isomerization catalysts; (3) use ligands to enable X-H activation; and (4) develop catalysts for addition reactions. The project will include significant one-on-one training in modern techniques of organic and organometallic chemistry, including NMR spectroscopy, catalysis screening, and computation. The proposed research will add new mechanistic insight to our picture of bifunctional catalysis, using complementary experimental and computational studies to allow the design of better catalysts and chemical processes.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.

在化学催化计划的支持下，圣地亚哥州立大学的Douglas B. Grotjahn和Andrew L. Cooksy教授正在进行研究，旨在确定可用于新反应的最佳催化剂，这些催化剂可用于使有机化合物用于使各种应用的有机化合物，包括药物，材料，材料，材料，材料，和生物学。为此，将制造和测试许多含有金属和较大非金属部分（配体）的催化剂，以确定哪种金属和配体的组合将产生最佳的性能催化剂。此外，将如何在分子水平上进行催化剂的基础研究。该赠款将支持对催化领域的几名年轻调查员的培训。由于催化占全球GDP的三分之一以及大多数化学产品和化学过程，因此发现有机反应的新的或改进的催化剂和新机制具有非常实际的重要性，这有助于经济发展和恢复。与上一个赠款期一样，将开发和改进实用的催化剂。 Also, to broaden public understanding of catalysis, the PIs and the graduate students will introduce the concept into an existing and highly successful high school outreach program.With the support of the Chemical Catalysis Program in the Division of Chemistry, Professors Douglas B. Grotjahn and Andrew L. Cooksy of San Diego State University will employ design principles of Nature’s enzymes, particularly hydrogen bonding and proton transfer, to accelerate (often by more than 1000-fold)有机催化和新机制的反应。将合成含有质子或氢键基的配体含有质子或氢键组的配体，并与多种金属前体合成，以形成其金属衍生物进行催化。这些吊坠基团与非极性和极性反应物，中间体或过渡状态的相互作用有望产生更快的催化剂。重点将主要放在无废物的添加或异构化反应上，其目标是多个目标：（1）在发现催化剂之前和之后整合了基于计算机的分子预测； （2）构建并应用一个烯烃同组化催化剂的工具箱； （3）使用配体启用X-H激活； （4）开发催化剂以进行添加反应。该项目将包括有机和有机化学现代技术的一对一培训，包括NMR光谱，催化筛查和计算。拟议的研究将使用互补的实验和计算研究为我们的双功能催化的情况增添新的机械见解，从而允许设计更好的催化剂和化学过程。该奖项反映了NSF的法定任务，并被认为是通过基金会的知识分子优点和更广泛的影响审查标准来通过评估来获得的支持。

项目成果

Synthesis and crystal structure of an iridium complex containing the novel electron-poor hybrid monoanionic ligand Ph2PCF2PO2(OiPr)

• DOI: 10.1016/j.poly.2022.116162
• 发表时间: 2022-12
• 期刊: Polyhedron
• 影响因子: 2.6
• 作者: D. Sattler;J. Bailey;D. Grotjahn