Hierarchical Modeling of the Local Reaction Environment in Electrocatalysis,Accounts of Chemical Research

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Hierarchical Modeling of the Local Reaction Environment in Electrocatalysis
Accounts of Chemical Research ( IF 16.4 ) Pub Date : 2024-07-20 , DOI: 10.1021/acs.accounts.4c00234
Xinwei Zhu _{1,

2} , Jun Huang _{1,

3} , Michael Eikerling _{1,

2}

Affiliation

Electrocatalytic reactions, such as oxygen reduction/evolution reactions and CO₂ reduction reaction that are pivotal for the energy transition, are multistep processes that occur in a nanoscale electric double layer (EDL) at a solid–liquid interface. Conventional analyses based on the Sabatier principle, using binding energies or effective electronic structure properties such as the d-band center as descriptors, are able to grasp overall trends in catalytic activity in specific groups of catalysts. However, thermodynamic approaches often fail to account for electrolyte effects that arise in the EDL, including pH, cation, and anion effects. These effects exert strong impacts on electrocatalytic reactions. There is growing consensus that the local reaction environment (LRE) prevailing in the EDL is the key to deciphering these complex and hitherto perplexing electrolyte effects. Increasing attention is thus paid to designing electrolyte properties, positioning the LRE at center stage. To this end, unraveling the LRE is becoming essential for designing electrocatalysts with specifically tailored properties, which could enable much needed breakthroughs in electrochemical energy science.

中文翻译：

电催化局部反应环境的分层建模

电催化反应，例如对于能量转换至关重要的氧还原/放出反应和CO ₂还原反应，是在固液界面的纳米级双电层（EDL）中发生的多步骤过程。基于萨巴蒂尔原理的传统分析，使用结合能或有效电子结构特性（例如 d 带中心）作为描述符，能够掌握特定催化剂组催化活性的总体趋势。然而，热力学方法通常无法解释 EDL 中出现的电解质效应，包括 pH、阳离子和阴离子效应。这些效应对电催化反应产生强烈影响。人们越来越一致认为，EDL 中普遍存在的局部反应环境 (LRE) 是破译这些复杂且迄今为止令人困惑的电解质效应的关键。因此，人们越来越关注电解质特性的设计，并将 LRE 置于中心舞台。为此，解开 LRE 对于设计具有专门定制特性的电催化剂至关重要，这可以实现电化学能源科学急需的突破。

更新日期：2024-07-20

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