Directing the Electrode-Electrolyte Interface Towards Active Nickel-Based Electrocatalysts for Oxygen Evolution Reaction

TL;DR

This study combines theoretical modeling and quantum simulations to understand and optimize the electrode-electrolyte interface in nickel-based electrocatalysts, revealing how solvation tuning can improve oxygen evolution reaction efficiency.

Contribution

It introduces a hybrid theoretical approach that accounts for realistic catalyst structure, doping, and solvation effects to enhance OER activity on nickel-iron oxyhydroxides.

Findings

Solvation effects linearly influence overpotential predictions.

Tuning local solvation environments can significantly boost OER activity.

Quantum chemical simulations combined with kinetic modeling provide new insights into OER processes.

Abstract

A comprehensive understanding of the electrode-electrolyte interface in energy conversion systems remains challenging due to the complex and multifaceted nature of interfacial processes. This complexity hinders the development of more efficient electrocatalysts. In this work, we propose a hybrid approach to the theoretical description of the OER process on nickel-iron-based oxyhydroxides ($\gamma$-Ni$_{1-x}$Fe$_x$OOH) electrodes in alkaline media as a model system. Multiple reaction pathways represented by the single- and dual-site mechanisms were investigated by taking into account the realistic structure of the catalyst, the doping, and the solvation effects using a simple and computationally feasible strategy. Accounting for the variable solvation effects considerably affects the predicted overpotential in a roughly linear relationship between overpotential and dielectric constant. By incorporating quantum chemical simulations with kinetic modeling, we demonstrate that tuning the local solvation environment can significantly enhance the OER activity, opening new routine ways for elucidation of the emerging issues of OER processes on transition metal oxide surfaces and design of cost-effective, efficient electrocatalytic systems.