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

电催化（EC）是大多数可持续未来新兴技术的核心。人们正致力于设计和改性用于与燃料产生和使用、能量储存和大宗化学品生产相关的一系列反应的催化剂。在EC和更广泛的多相催化领域中，催化剂通过改变吸附的中间体和沿着反应途径的基本步骤的过渡态（TS）的能量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，中间体和TS的结合能通常是强烈相关的。因此，催化剂的结构或组成的改变通常不能有效地打破这些相关性（比例关系）。反应性表面与初始状态的结合更强，也往往与TS和最终状态的结合更强，导致步骤的能量势垒（速率）变化最小。标度关系在催化中早已为人所知，但有意规避它们的新策略的研究要新得多。在EC中出现的方法，如单独或组合使用应变结构，高稀释合金，和配体修饰的表面。这就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的潜力，以打破不同的自旋多重性，这是不可避免地存在于多电子过程中的中间体和过渡态的标度关系。这个建议的目的是探索潜在的自旋电子学中建立的解决方案，以产生局部磁场打破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.