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

电催化（EC）是大多数可持续发展的新兴技术的核心。人们正在努力设计和改进催化剂，以用于与燃料产生和使用、能源储存和大宗化学品生产有关的一系列反应。在EC和更广泛的多相催化领域中，催化剂通过改变吸附中间体的能量和反应途径基本步骤的过渡态（TS）来实现特定途径的速率变化，从而实现选择性变化。不幸的是，中间产物的结合能和TS通常是强相关的。因此，改变催化剂的结构或组成往往无法打破这些相关性（结垢关系）。结合初始态更强的活性表面通常也更强地结合TS和最终态，导致该步骤的能量势垒（速率）变化最小。在催化中，尺度关系早已为人所知，但有意规避它们的新策略的研究要晚得多。在EC中出现了一些方法，如分离或结合使用应变结构、高稀释合金和配体修饰表面。这需要对催化剂进行根本性的重新设计。目前被忽视的是，原位产生的磁场可能会破坏具有不同自旋多重性的中间体和过渡态的标度关系，而这在多电子过程中是不可避免的。本提案旨在探索自旋电子学中已建立的解决方案的潜力，以产生局部磁场来打破EC中的标度关系。

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.