CAS: Electrochemical Ionic Hydrogenation: Promoting Carbonyl and Imine Reduction through Electrocatalysis

在化学系化学催化项目的支持下，Kate M.新泽西的州立大学罗格斯大学的Waldie正在研究利用电化学制备有价值的化学产品的策略。该项目的目标是开发更可持续的方法，使用可再生的可持续能源生产化学品。拟议的研究将涉及实验，以了解催化剂结构和反应条件如何结合联合收割机，以实现高反应效率和选择性。这些知识将在可持续化学制造的电催化剂设计中具有重要的应用。该项目还将为学生提供合成化学、催化和电化学方面的培训。沃尔迪集团将继续从事推广活动，促进公平和包容传统上代表性不足的人口的学生，包括一个经常性的专题讨论会系列题为多样性化学，突出了来自不同背景的化学家的职业和观点。Waldie博士还将为电化学教育开发新的讲座和实验室教学资源。本项目将在布朗斯台德酸或刘易斯酸促进剂存在下，使用过渡金属氢化物络合物开发羰基和亚胺底物的电化学离子氢化。这种加氢的电催化方法避免了对氢气或化学计量还原剂的需要。然而，避免竞争性析氢反应（HER）是电化学还原反应的重大挑战。该研究将利用详细的电化学，动力学和机理研究，以检查如何与酸的底物活化可以直接反应的金属氢化物络合物对电化学氢化超过HER.This项目的目的是建立一个热力学框架中的金属氢化物电催化剂和酸促进剂的性能进行优化，以实现高选择性和高法拉第效率的底物还原。其目标是研究大范围的反应性，并建立原则和方法，以促进羰基和亚胺氢化的电气化，以实现可持续的有机合成。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，被认为值得支持。

With the support of the Chemical Catalysis program in the Division of Chemistry, Kate M. Waldie of Rutgers, The State University of New Jersey is studying strategies to prepare valuable chemical products using electrochemistry. The goal of this project is to develop more sustainable methods for producing chemicals using renewable, sustainable energy. The proposed research will involve experiments to understand how catalyst structure and reaction conditions combine to achieve high reaction efficiency and selectivity. This knowledge will have important applications in electrocatalyst design for sustainable chemical manufacturing. The project will also provide training for students in synthetic chemistry, catalysis, and electrochemistry. The Waldie group will continue to engage in outreach activities that promote the equity and inclusion of students from traditionally underrepresented populations, including a recurring symposium series entitled Diversity in Chemistry that highlights the careers and perspectives of chemists from diverse backgrounds. Dr. Waldie will also develop new lecture and laboratory teaching resources for electrochemistry education. This project will develop the electrochemical ionic hydrogenation of carbonyl and imine substrates using transition metal-hydride complexes in the presence of Brønsted or Lewis acid promotors. This electrocatalytic approach to hydrogenation circumvents the need for hydrogen gas or stoichiometric reductants. However, avoiding the competitive hydrogen evolution reaction (HER) is a significant challenge for electrochemical reduction reactions. The proposed research will utilize detailed electrochemical, kinetic, and mechanistic studies to examine how substrate activation with an acid can direct the reactivity of metal-hydride complexes toward electrochemical hydrogenation over HER. This project aims to establish a thermodynamic framework in which the properties of the metal-hydride electrocatalyst and acid promoter are optimized to achieve high selectivity and high faradaic efficiency for substrate reduction. The goal is to investigate a large reactivity scope and establish principles and methods to advance the electrification of carbonyl and imine hydrogenation for sustainable organic synthesis.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.