New Approaches to Reversible Homogeneous Electrocatalysts

可逆均相电催化剂的新方法

• 批准号: 1565947
• 负责人: Robert Waymouth
• 金额: $ 55.5万
• 依托单位: Stanford University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2016
• 资助国家: 美国
• 起止时间: 2016-09-01 至 2019-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1565947&HistoricalAwards=false
• 关键词: New; Approaches; Reversible; Homogeneous; Electrocatalysts; New; Approaches; Reversible; Homogeneous; Electrocatalysts

In this project funded by the Chemical Catalysis program of the Chemistry Division, Professor Robert Waymouth of Stanford University is developing new experimental approaches for the electrocatalytic conversion of alcohols into ketones. The conversion of chemical compounds such as alcohols into ketones can form the basis of fuel cells, which are alternatives to conventional power sources. While the alcohol/ketone fuel cells are very attractive, the chemical reaction is difficult. In this project, new catalysts that facilitate such difficult reactions are being developed. This research provides new means for the energy-efficient conversion of chemical fuels into useful forms of energy. Collaborative investigations with Professors Richard Zare and Christopher Chidsey at Stanford University enhance the experimental and educational infrastructure for energy science and provide faculty, postdoctoral, graduate, and undergraduate students with rich opportunities for education and collaborative research. This project focuses on homogeneous catalysts bearing proton and redox-active ligands. It is guided by the hypothesis that mechanistic concepts that have been developed for chemical transfer hydrogenation catalysis, such as metal-ligand bifunctional activation of substrates, can be applied to the behavior of proton- and redox-active ligands that are effective in mediating multi-electron and proton transfers. The experimental approach utilizes homogeneous coordination complexes and seeks to determine the key features of the metal/ligand coordination environments that mediate the hydrogen atom, proton and electron transfer steps in efficient electrocatalytic processes. The development and application of high resolution mass spectrometry techniques, interfaced to electrochemical cells is an innovative aspect of the experimental plan. These provide new mechanistic insights on the intermediates generated during electrocatalytic reactions. Broader impacts of this work include new approaches for the energy-efficient conversion of chemical fuels into useful forms of energy.

在该项目由化学部化学催化计划资助的项目中，斯坦福大学的罗伯特·韦茅斯教授正在开发新的实验方法，用于将酒精转化为酮的电催化转化。化合物（例如醇）转化为酮的化合物可以构成燃料电池的基础，这是传统电源的替代品。虽然酒精/酮燃料电池非常吸引人，但化学反应很困难。在这个项目中，正在开发促进这种困难反应的新催化剂。这项研究为化学燃料转化为有用的能源形式提供了新的手段。斯坦福大学与理查德·扎尔（Richard Zare）和克里斯托弗·奇德西（Christopher Chidsey）的合作调查增强了能源科学的实验和教育基础设施，并为教师，博士后，研究生和本科生提供丰富的教育机会和协作研究的机会。该项目的重点是带有质子和氧化还原活性配体的均质催化剂。它的指导下，可以将用于化学转移氢化催化的机械概念（例如底物的金属配体双功能激活）用于质子和氧化还原活性配体的行为，这些配体有效地介导多电子和蛋白质转移。 实验方法利用均匀的配位络合物，并寻求确定介导氢原子，质子和电子传递步骤中有效电催化过程的金属/配体配位环境的关键特征。 高分辨率质谱技术的开发和应用与电化学细胞相连是实验计划的创新方面。这些提供了对电催化反应过程中产生的中间体的新机械见解。 这项工作的更广泛的影响包括将化学燃料转化为有用形式的能源的新方法。