REDEEM-electrocat: Rethinking Electrode Design - Emergent Electronic and Magnetic effects in electrocatalysis

REDEEM-electriccat：重新思考电极设计 - 电催化中出现的电子和磁效应

• 批准号: EP/V048279/1
• 负责人: Gilberto Teobaldi
• 金额: $ 1.06万
• 依托单位: Science and Technology Facilities Council
• 依托单位国家: 英国
• 项目类别: Research Grant
• 财政年份: 2021
• 资助国家: 英国
• 起止时间: 2021 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FV048279%2F1
• 关键词: REDEEM; electrocat; Rethinking; Electrode; Design

Electrocatalysis (EC) lies at the heart of most of the emerging technologies for a sustainable future. Enormous efforts are being directed towards designing and modifying catalysts for a range of reactions relevant to fuel generation and use, energy storage, and bulk chemical production. Within EC, and the wider field of heterogeneous catalysis, catalysts achieve changes in rate, and hence selectivity, of a particular pathway through modification of the energy of adsorbed intermediates and transition states (TS) of the elementary steps along a reaction pathway. Unfortunately, binding energies of intermediates and TS are usually strongly correlated. As a result, modifications in the structure or composition of the catalysts are often ineffective in breaking these correlations (scaling relationships). Reactive surfaces that bind an initial state more strongly often also bind the TS and final state more strongly too, leading to minimal change in the energy-barrier (rate) of the step.Scaling relationships have been long known in catalysis but research in new strategies to deliberately circumvent them is far newer. Approaches are emerging in EC such as the isolated or combined use of strained structures, high dilution alloys, and ligand modified surfaces. These require a fundamental redesign of the catalysts. Currently overlooked is the potential of in-situ generated magnetic fields to break scaling relationships for intermediates and transition states with different spin-multiplicity, which are inevitably present in multi-electron processes. This proposal aims to explore the potential of established solutions in spintronics to generate local magnetic fields for breaking scaling relationships in EC.

电催化（EC）是可持续未来的大多数新兴技术的核心。巨大的努力是针对设计和修饰催化剂的一系列反应，与燃料产生和使用相关，能源储能和大量化学生产。在EC中，以及异质催化的更广泛的领域，催化剂通过修改沿反应途径的基本步骤的吸附中间体和过渡状态（TS）的能量来实现特定途径的变化，从而实现了特定途径的变化。不幸的是，中间体和TS的结合能通常密切相关。结果，催化剂的结构或组成的修改通常在打破这些相关性（缩放关系）时无效。反应性的表面更加强烈地结合初始状态也经常结合TS和最终状态，从而使步骤的能量阻控制器（速率）的变化最小。尺度关系在催化中备受闻名，但是在新策略中，有意构成它们的新策略进行了研究，这是更新的。在EC中出现了方法，例如隔离或联合使用应变结构，高稀释合金和配体修饰的表面。这些需要重新设计催化剂。当前被忽略的是原位生成的磁场的潜力，即具有不同自旋多性性的中间体和过渡状态的缩放关系，这在多电子过程中不可避免地存在。该建议旨在探索旋转三位型固定解决方案的潜力，以生成局部磁场，以破坏EC中的缩放关系。