Enhancing the oxygen evolution reaction by tuning the electrode-electrolyte interface in nickel-based...

Area of Science:

• Electrochemistry
• Materials Science
• Theoretical Chemistry

Background:

• Understanding electrode-electrolyte interfaces is crucial for energy conversion systems.
• Interfacial complexities impede the development of efficient electrocatalysts.
• Nickel-iron oxyhydroxides (γ-Ni1-xFexOOH) are promising electrocatalysts for oxygen evolution reactions (OER).

Purpose of the Study:

• To develop a hybrid theoretical approach for describing the OER process on γ-Ni1-xFexOOH electrodes.
• To investigate multiple reaction pathways, including single- and dual-site mechanisms.
• To elucidate the impact of catalyst structure, doping, and solvation effects on OER activity.

Main Methods:

• Utilized a hybrid approach combining quantum chemical simulations and kinetic modeling.
• Investigated realistic catalyst structures, doping effects, and variable solvation environments.
• Analyzed single- and dual-site reaction mechanisms for OER.

Main Results:

• Variable solvation effects significantly influence predicted overpotentials.
• A roughly linear relationship exists between overpotential and dielectric constant.
• Tuning the local solvation environment demonstrably enhances OER activity.

Conclusions:

• The hybrid approach provides a computationally feasible strategy for theoretical OER description.
• Optimizing the solvation environment is a viable route to enhance electrocatalyst performance.
• This work offers new insights into OER on transition metal oxides and designing efficient electrocatalytic systems.