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

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基思教授正致力于开发更可持续的方法，通过设计耐用、高活性的金属催化剂，特别是用于氢化反应的催化剂，来实现同样的结果。在为这些反应开发下一代改进的催化剂时，必须了解催化剂在分子水平上如何工作。因此，该项目的一个重要组成部分是结合实验和理论知识，对这些催化剂及其反应进行全面而详细的了解。该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。参与本科研究，特别是在学生职业生涯的早期，越来越多地认识到其对学生的积极影响。PI Chianese和他的研究小组的学生每年夏天都会花一天时间为参加Camp Fiver的高中生举办一次外展活动，Camp Fiver是一个寄宿夏令营，接待一群纽约市和纽约州北部农村的高危学生。Colgate大学的Anthony Chianese教授和Jason基思教授正在开发用于酯的氢化的新催化剂。最近，已经开发了用于氢化多种极性底物的高效催化剂，这受到Milstein的PNN-钳-钌体系的公开的刺激，该体系对酯氢化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。Chianese和基思最近发现了一种基于CC-螯合配体的酯氢化催化剂，其结构表明非合作机制可能起作用。该项目的目标是通过改变催化剂结构来开发和优化这种催化剂系统，同时通过实验和计算来建立彻底的机理理解。该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。参与本科研究，特别是在学生职业生涯的早期，越来越多地认识到其对学生的积极影响。PI Chianese和他的研究小组的学生每年夏天都会花一天时间为参加Camp Fiver的学校学生举办一次外展活动，Camp Fiver是一个寄宿夏令营，接待一群纽约市和纽约北部农村的高危学生。

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.