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

界面电化学和电催化：在分子水平上理解和指导电化学现象

• 批准号: 121968-2012
• 负责人: Jerkiewicz, Gregory
• 金额: $ 4.01万
• 依托单位: Queen's University
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2013
• 资助国家: 加拿大
• 起止时间: 2013-01-01 至 2014-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=522240
• 关键词: Interfacial; Electrochemistry; Electrocatalysis; Understanding; Directing

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.

我们在界面电化学和电催化方面的研究项目包括四个创新和相互关联的重点，这些重点将同时进行，目的是获得对电化学现象的分子水平的理解。我们将研究Pt电催化活性的起源，并将确定关键特征，这些特征将用于开发一套具有类似电催化性能的非Pt电催化剂的合成指南。这将通过详细的实验研究来实现，其中包括开发变温电化学石英晶体纳米平衡。我们将通过研究H在具有精心定制尺寸的球形Pt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电吸附的临界尺寸，从而产生独特的界面行为。我们将对Pt（hkl）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效应。由于用于聚合物电解质膜燃料电池的铂纳米颗粒主要包含（111）和（100）个面以及棱角，因此本研究将有助于理解其降解过程。我们还将研究温度对形成亚纳米厚度的金属层的影响，这些金属层具有定制的化学成分和与衬底的精细粘附性；我们将评估温度变化对其物理性质的影响。该研究计划包括四个主题，为突破创造了机会，如果不是发现的话。这是一个雄心勃勃的挑战，但我们成功承担困难项目的能力和我们过去的成就证明，通过训练有素的HQP可以实现所提出的研究。虽然这项研究是基础性质的，但它将通过创造新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，并将培养一套独特的跨学科技能，这将有助于他们未来的职业发展。