Catalysis, Adsorption and Charge Transfer Kinetics in Reactions at Electrodes

这个项目属于分析化学和表面化学的一般领域以及电化学的子领域。在这项为期五年的持续资助期间，Anson教授和他的学生将设计、合成和评估新的表面限制电催化剂，用于直接将二氧还原为水，并用于甲醇、乙醇、甲醛和甲酸等有机底物的电氧化。还将探讨吸附电活性配体及其金属配合物的电催化的一般适用性。由于许多电催化物质使用聚合物基质进行表面限制，因此还将研究溶液组成控制的热力学驱动力对聚合物-电解质界面电子转移动力学的影响。最后，亚稳过渡金属-双氧配合物的电化学行为，长期以来被认为是电催化还原双氧的关键中间体，将被探讨，以提供这些过渡金属促进过程的机制见解。高效、经济的燃料电池和电池的合理设计是建立在对所涉及的电化学过程的基本理解的基础上的。本研究旨在通过电催化促进廉价底物分子的电化学转化，以用于这些技术上和社会上重要的设备。＊＊＊

9312091 Anson This project is in the general area of analytical and surface chemistry and in the subfield of electrochemistry. During the tenure of this five-year continuing grant, Professor Anson and his students will design, synthesize, and evaluate new surface confined electrocatalysts for the direct, four-electron reduction of dioxygen to water and for the electrooxidation of organic substrates such as methanol, ethanol, formaldehyde, and formic acid. The general applicability of electrocatalysis by adsorbed electroactive ligands and their metal complexes will also be explored. Because many electrocatalytic species are surface confined using polymeric matrices, the impact of solution composition-controlled thermodynamic driving forces on the kinetics of electron transfer across polymer-electrolyte interfaces will also be investigated. Finally, the electrochemical behavior of metastable transition metal-dioxygen complexes, long believed to be key intermediates in the electrocatalytic reduction of dioxygen, will be probed to afford insights into the mechanisms of these transition metal-promoted processes. %%% The rational design of efficient, economical fuel cells and batteries is predicated on a fundamental understanding of the electrochemical processes involved. This research is aimed at enhancing knowledge of how electrochemical transformations of inexpensive substrate molecules can be facilitated through electrocatalysis for use in these technologically and societally important devices. ***