Interfacial Electrochemistry and Electrocatalysis: Understanding and Directing Electrochemical Phenomena at the Molecular Level

我们在界面电化学和电催化方面的研究计划包括四个创新的和相互关联的推力，这些推力将同时进行，目的是从分子水平上了解电化学现象。我们将研究铂的电催化活性的起源，并确定关键特征，这些特征将被用来制定一套指南，用于合成具有类似电催化性能的非铂电催化剂。这将通过详细的实验研究来实现，其中将包括开发变温电化学石英晶体纳米天平。我们将通过研究H在具有合适尺寸的球形铂纳米颗粒上的电吸附来研究电催化中的尺寸依赖现象，并确定纳米颗粒尺寸开始影响H的电吸附的临界尺寸，从而产生独特的界面行为。我们将对铂电极的电氧化和电溶解进行细致的研究，目的是发现特定于表面几何形状的影响。由于用于聚合物电解质膜燃料电池的铂纳米颗粒主要含有(111)和(100)晶面以及棱角，因此本研究将有助于了解其降解过程。我们还将研究温度对金属层形成的影响，这些金属层的厚度为亚纳米，具有量身定制的化学成分和与基材的微调附着力；我们将评估温度变化对其物理性能的影响。这个由四个主题组成的研究项目创造了一个突破的机会，如果不是发现的话。这是雄心勃勃和具有挑战性的，但我们成功承担困难项目的能力和我们过去的成就证明，拟议的研究可以在训练有素的HQP的帮助下实现。虽然这项研究是基础性的，但它将通过创造新的知识而使电化学技术受益。最后，六名HQP将接受现代电化学和电催化方面的培训，并将发展一套独特的跨学科技能，这将提升他们未来的职业生涯。

Our research program in interfacial electrochemistry and electrocatalysis consist of four innovative and inter-related thrusts that will be pursued at the same time with the objective of gaining molecular-level understanding of electrochemical phenomena. We will study the origin of electrocatalytic activity of Pt and will identify key characteristics that will be used to develop a set of guidelines for the synthesis of non-Pt electrocatalysts possessing similar electrocatalytic properties. This will be achieved through detailed experimental research, which will include the development of variable-temperature electrochemical quartz-crystal nanobalance. We will investigate size-dependent phenomena in electrocatalysis by studying the electro-adsorption of H on spherical Pt nanoparticles having well-tailored dimensions and determine the critical dimension at which the size of nanoparticles begins to affect the H electro-adsorption giving rise to a unique interfacial behavior. We will carry out meticulous investigation of the electro-oxidation and electro-dissolution of Pt(hkl) electrodes with the objective of discovering effects that are specific to the surface geometry. Because Pt nanoparticles used in polymer electrolyte membrane fuel cells contain mainly (111) and (100) facets plus edges and corners, this research will contribute to the understanding of their degradation. We will also study the impact of temperature on the formation of metallic layers that are sub-nm in thickness, possess a tailored chemical composition and fine-tuned adhesion to the substrate; we will assess the influence of temperature variation on their physical properties. The research program comprising four themes creates an opportunity for a breakthrough, if not for a discovery. It is ambitious and challenging, but our ability to successfully undertake difficult projects and our past achievements prove that the proposed research can be realized with well-trained HQP. Though the research is basic in nature, it will benefit electrochemical technologies by creating new knowledge. Finally, six HQP will be trained in modern electrochemistry and electrocatalysis, and will develop a unique set of inter-disciplinary skills, which will enhance their future careers.