Simulation of Potential-Dependent Activation Energies in Electrocatalysis: Mechanism of O–O Bond Formation on RuO2

电催化剂 化学 化学物理 电子转移 电子 计算化学 电化学 物理 物理化学 量子力学 电极
作者
Zhiyao Duan,Penghao Xiao
出处
期刊:Journal of Physical Chemistry C [American Chemical Society]
卷期号:125 (28): 15243-15250 被引量:61
标识
DOI:10.1021/acs.jpcc.1c02998
摘要

Theoretical assessment of potential-dependent activation energies of electrochemical reactions is of critical importance but remains challenging. In this work, we present two computational tools to tackle this long-standing challenge. First, we implement a general computational framework for constant-potential saddle searches including both atomic positions and number of electrons as variables. Second, we develop a novel correction method to determine potential-dependent activation energies based on conventional zero-charge calculations. Different from existing capacitance-only schemes, our correction method takes into account the potential-dependent structural relaxation. This correction allows a significant reduction in computational overhead, but is still quite accurate, supplementing the direct constant-potential simulation. With these tools, we study the O–O bond formation reaction on the RuO2(110) surface. A number of new mechanistic insights are developed from the constant-potential calculations. The proton-coupled electron transfer pathway for the O–O bond formation has been determined to be favorable over the water dissociation mechanism. It is found that both H atoms strip from H2O successively to directly form adsorbed O2 without forming a stable intermediate OOH. With this example, we also demonstrate that the charge-structure coupling effect is not always negligible and can be captured by the full-Hessian correction. We expect the methods developed here to become useful tools in electrocatalysis.
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