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的和/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 Chianes教授和Jason Keith教授正在努力开发更可持续的方法，通过设计坚固、高活性的金属催化剂来实现同样的结果，特别是在加氢反应中。在开发下一代用于这些反应的改进型催化剂时，了解这些催化剂在分子水平上的工作方式是至关重要的。因此，这个项目的一个重要部分是将实验和理论知识结合起来，以建立对这些催化剂及其反应的全面和详细的了解。这个项目的所有研究都是由高露洁PI实验室的本科生进行的。参与本科生的研究，特别是在学生职业生涯的早期，越来越多地认识到它对学生的积极影响。皮奇亚尼斯和他的研究小组的学生每年夏天都会花一天时间为参加第五营的高中生举办一项外展活动，这是一个寄宿夏令营，接待了一群高危学生，包括纽约市和纽约州北部的农村。在化学系化学催化项目的资助下，高露洁大学的安东尼·奇亚尼斯和杰森·基思教授正在开发用于酯加氢的新催化剂。最近，在Milstein的PNN-Pincer-Ru体系的揭示的推动下，人们已经开发出用于各种极性底物加氢的高效催化剂，该体系对酯加氢为醇和反向反应具有活性。目前，用于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。Chianes和Keith最近发现了一种基于CC-螯合配体的酯加氢催化剂，其结构表明可能存在非合作机制。该项目的目标是通过修改催化剂结构来开发和优化该催化剂系统，同时致力于通过实验和计算建立全面的机理理解。这个项目的所有研究都是由高露洁PI实验室的本科生进行的。参与本科生的研究，特别是在学生职业生涯的早期，越来越多地认识到它对学生的积极影响。皮奇亚尼斯和他的研究小组的学生每年夏天都会花一天时间为参加第五营的学生举办一项外联活动，这是一个寄宿夏令营，接待了一群高危学生，包括纽约市和纽约州北部的农村地区。

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.