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Cationic gold-antimony complexes: Synthesis and electrophilic properties.

阳离子金锑配合物：合成和亲电子特性。

基本信息

批准号：
1856453
负责人：
Francois Gabbai
金额：
$ 54.25万
依托单位：
Texas A&M University
依托单位国家：
美国
项目类别：
Continuing Grant
财政年份：
2019
资助国家：
美国
起止时间：
2019-08-01 至 2023-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1856453&HistoricalAwards=false
关键词：
Cationic gold antimony complexes Synthesis

项目摘要

A catalyst is a substance that speeds or otherwise facilitates a chemical reaction. Catalysts are critical to the chemical and pharmaceutical industries, where they are used to reduce the energy required for chemical reactions and to guide the details of precise chemical transformations. While gold is an expensive element, many catalysts incorporate it. Improving gold catalysts is an important area of investigation. In this project, funded by the Chemical Synthesis Program of the Chemistry Division, Professor Francois Gabbai of the Department of Chemistry at Texas A&M University seeks to improve the catalytic properties of gold by combining it with antimony, a non-metallic element. The antimony is able to combine with gold in a way that enhances gold's reactivity. The gold-antimony compounds that are isolated are developed into catalysts for the activation of alkenes, which are major chemical industry feedstocks. Professor Gabbai participates in outreach programs to K-6 students in Spanish/English dual language programs in order to interest young students in science and technology.This research project investigates the chemistry of gold (Au) complexes featuring ambiphilic ligands comprised of two phosphine donors and an antimony moiety. The central objective is to determine if the charge of the antimony (Sb) ligand can be used to modulate the electrophilic character and catalytic properties of the gold center. A series of dinuclear complexes with a gold atom held in close proximity to a pentavalent antimony center are synthesized and ligand abstraction reactions generate complexes in which the pentavalent antimony center is either monocationic or dicationic. Structural, spectroscopic and computational studies indicate if the accumulation of positive character on the antimony ligand promotes a donor-acceptor Au-Sb interaction. A correlation between the charge of the antimony ligand and the electrophilic reactivity of the gold center is indicated by the catalytic activation of alkenes in polymerization and hydroamination reactions.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.

催化剂是一种加速或促进化学反应的物质。催化剂对化学和制药行业至关重要，它们用于减少化学反应所需的能量，并指导精确化学转化的细节。虽然金是一种昂贵的元素，但许多催化剂都含有它。改进金催化剂是一个重要的研究领域。在这个由化学系化学合成计划资助的项目中，德克萨斯州农工大学化学系的Francois Gabbai教授试图通过将金与锑（一种非金属元素）结合来改善金的催化性能。锑能够以增强金的反应性的方式与金联合收割机结合。分离出的金锑化合物被开发成用于活化烯烃的催化剂，烯烃是主要的化学工业原料。 Gabbai教授参加了西班牙语/英语双语课程中K-6学生的外展计划，以培养年轻学生对科学和技术的兴趣。本研究项目研究了由两个膦供体和一个锑部分组成的具有两亲性配体的金（Au）配合物的化学。中心目标是确定锑（Sb）配体的电荷是否可用于调节金中心的亲电特性和催化性能。一系列的双核配合物与金原子保持在接近五价锑中心的合成和配体提取反应生成的配合物，其中五价锑中心是单阳离子或双阳离子。结构，光谱和计算研究表明，如果锑配体上的积极字符的积累，促进了施主-受主Au-Sb相互作用。锑配位体的电荷和金中心的亲电反应性之间的相关性通过烯烃在聚合和氢化胺化反应中的催化活化来表示。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而被认为值得支持。