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RUI: Development of a Non-Cooperative Ruthenium Catalyst for Ester Hydrogenation

RUI：开发用于酯加氢的非合作性钌催化剂

基本信息

批准号：
1665144
负责人：
Anthony Chianese
金额：
$ 29.46万
依托单位：
Colgate University
依托单位国家：
美国
项目类别：
Continuing Grant
财政年份：
2017
资助国家：
美国
起止时间：
2017-09-01 至 2020-08-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1665144&HistoricalAwards=false
关键词：
RUI Development Non Cooperative Ruthenium

项目摘要

Many of the current methods for carrying out chemical reactions rely on the use of expensive and/or toxic reagents, and often produce large amounts of chemical waste. In this project, Professors Anthony Chianese and Jason Keith are working to develop more sustainable methods to achieve the same results by designing robust, highly active metal catalysts, in particular for hydrogenation reactions. In developing the next generation of improved catalysts for these reactions, it is essential to understand how the catalysts work at the molecular level. Therefore, an important part of this project involves combining experimental and theoretical knowledge to build a comprehensive and detailed understanding of these catalysts and their reactions. All of the research for this project is being conducted by undergraduate students in the PIs' laboratories at Colgate. Participation in undergraduate research, especially early in a student's career, is increasingly recognized for its positive impacts on students. PI Chianese and the students working in his research group devote a day each summer to running an outreach activity for high school students attending Camp Fiver, a residential summer camp that hosts a group of at-risk students New York City and rural upstate New York.With funding from the Chemical Catalysis Program of the Chemistry Division, Professors Anthony Chianese and Jason Keith of Colgate University are developing new catalysts for the hydrogenation of esters. Recently, highly efficient catalysts have been developed for the hydrogenation of a wide array of polar substrates, spurred by the disclosure of Milstein's PNN-pincer-ruthenium system that is active for the hydrogenation of esters to alcohols and the reverse reaction. Currently, all of the most efficient catalysts for this class of transformation are developed based on an expected metal-ligand cooperative mechanism. Chianese and Keith have recently discovered a catalyst for ester hydrogenation based on a CC-chelating ligand whose structure suggests that a non-cooperative mechanism is likely operative. The goal of the project is to develop and optimize this catalyst system through modification of the catalyst structure, while devoting significant effort to building a thorough mechanistic understanding through experiment and computation. All of the research for this project is being conducted by undergraduate students in the PIs' laboratories at Colgate. Participation in undergraduate research, especially early in a student's career, is increasingly recognized for its positive impacts on students. PI Chianese and the students working in his research group devote a day each summer to running an outreach activity for school students attending Camp Fiver, a residential summer camp that hosts a group of at-risk students New York City and rural upstate New York.

目前进行化学反应的许多方法依赖于使用昂贵和/或有毒的试剂，并且经常产生大量的化学废物。在这个项目中，Anthony Chianese教授和Jason Keith教授正致力于开发更可持续的方法，通过设计坚固、高活性的金属催化剂，特别是用于氢化反应，来实现同样的结果。在开发用于这些反应的下一代改进催化剂时，了解催化剂在分子水平上的工作原理是至关重要的。因此，本项目的一个重要部分是将实验和理论知识结合起来，对这些催化剂及其反应进行全面而详细的了解。这个项目的所有研究都是由本科生在高露洁的pi实验室进行的。参与本科生研究，特别是在学生职业生涯的早期，对学生的积极影响越来越得到认可。每年夏天，PI china和他研究小组的学生们都会抽出一天的时间，为参加Camp five夏令营的高中生开展一项拓展活动。Camp five是一个寄宿夏令营，接待了一群来自纽约市和纽约州北部农村地区的高危学生。在化学部化学催化项目的资助下，高露洁大学的Anthony Chianese教授和Jason Keith教授正在开发用于酯类氢化的新型催化剂。最近，由于Milstein的pnn -钳子-钌体系的发现，人们已经开发出了用于多种极性底物加氢的高效催化剂，该体系对酯类加氢成醇和逆反应具有活性。目前，这类转化的所有最有效的催化剂都是基于预期的金属-配体合作机制开发的。中国和Keith最近发现了一种基于cc螯合配体的酯加氢催化剂，其结构表明非合作机制可能有效。该项目的目标是通过对催化剂结构的修改来开发和优化该催化剂体系，同时通过实验和计算，努力建立一个全面的机理认识。这个项目的所有研究都是由本科生在高露洁的pi实验室进行的。参与本科生研究，特别是在学生职业生涯的早期，对学生的积极影响越来越得到认可。每年夏天，PI chinanese和他研究小组的学生都会抽出一天时间，为参加Camp five夏令营的学生开展一项拓展活动。Camp five是一个住宿夏令营，接待了一群来自纽约市和纽约州北部农村地区的高危学生。