Kinetic Properties of Oxygen Evolution Reaction Catalysis in Hematite,Advanced Theory and Simulations

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Kinetic Properties of Oxygen Evolution Reaction Catalysis in Hematite
Advanced Theory and Simulations ( IF 2.9 ) Pub Date : 2023-05-05 , DOI: 10.1002/adts.202300182
Nadav Snir ₁ , Maytal Caspary Toroker _{1,

2}

Affiliation

Water splitting is a promising method for hydrogen generation, but current catalytic reactions suffer from low efficiency. One possible reason for such inefficiency is a high kinetic barrier for water oxidation, and there is a lack of direct and efficient method to calculate the barrier for each reaction. In this paper, the inner sphere component of the reorganization energy that contributed to the activation energies is calculated. A novel algorithm is used for calculating the reorganization energy based on Marcus theory combined with the climbing image nudged elastic band method used to find transition states and activation energies of the oxygen evolution reaction steps, which allows the calculation of the activation energy at different potentials and without simulating solvation in order to obtain the inner sphere component alone arising from the reorganization of the ionic surface. The new method is tested in both acidic and basic conditions and with explicit water molecules, as well as implicit solvation. It is discovered that the reaction involving the transition of the *O intermediate into *OOH has the highest activation energy of all steps, thus explaining the high coverage of the *O intermediate found by experiments.

中文翻译：

赤铁矿中析氧反应催化动力学性质

水分解是一种很有前景的制氢方法，但目前的催化反应效率较低。这种低效率的一个可能原因是水氧化的动力学势垒较高，并且缺乏直接有效的方法来计算每个反应的势垒。本文计算了对活化能有贡献的重组能的内球部分。基于马库斯理论，结合用于寻找析氧反应步骤的过渡态和活化能的爬升图像微移弹性带方法，采用一种新颖的算法来计算重组能，从而可以计算不同电位和活化能。无需模拟溶剂化以获得因离子表面重组而单独产生的内球成分。新方法在酸性和碱性条件下以及显式水分子和隐式溶剂化下进行了测试。结果发现，涉及*O中间体转变为*OOH的反应具有所有步骤中最高的活化能，从而解释了实验发现的*O中间体的高覆盖率。

更新日期：2023-05-05

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