Oxygen evolution reaction: a perspective on a decade of atomic scale simulations

Area of Science:

• Materials Science
• Computational Chemistry
• Electrochemistry

Background:

• The oxygen evolution reaction (OER) is crucial for water oxidation but suffers from intrinsic limitations, leading to inefficiency.
• Significant research efforts have focused on developing strategies to overcome these limitations and reduce the required overpotential.
• The universal scaling relationship between key intermediates (HO* and HOO*) is a known challenge in OER catalysis.

Purpose of the Study:

• To analyze published DFT calculation data for OER to understand the limited progress in reducing overpotential.
• To investigate the robustness of the HO*–HOO* scaling relationship across various computational methods and material structures.
• To identify computational challenges, particularly for doped semiconducting oxides, and propose solutions.

Main Methods:

• Systematic collection and analysis of published DFT calculation studies focused on the oxygen evolution reaction.
• Evaluation of binding energies for intermediates like HO* and HOO* to assess scaling relationships.
• Comparative analysis of trends in doped semiconducting oxides versus other oxide materials.

Main Results:

• The universal scaling relationship between HO* and HOO* intermediates was confirmed to be robust across diverse computational approaches.
• No clear trend was observed for the O* binding energy, indicating complex behavior.
• Doped semiconducting oxides exhibited distinct trends compared to other oxides, highlighting a computational description challenge.

Conclusions:

• The persistent HO*–HOO* scaling relationship remains a fundamental barrier to lowering OER overpotential.
• Accurately describing doped semiconducting oxides computationally presents a significant challenge.
• A novel computational approach is proposed to overcome these challenges for simulations of doped semiconductors.