Oxygen reduction reactions on pure and nitrogen-doped graphene: a first-principles modeling

TL;DR

This study uses first-principles calculations to compare oxygen reduction reactions on pure and nitrogen-doped graphene, showing that lightly doped graphene can have lower energy barriers than platinum, with coverage affected by surface structure.

Contribution

It provides new insights into the energetics and catalytic potential of nitrogen-doped graphene for oxygen reduction, highlighting effects of doping level and surface morphology.

Findings

Lightly nitrogen-doped graphene has lower energy barriers than platinum.

Maximum coverage on doped graphene depends on surface corrugation.

Energy barriers vary with oxygen load and surface structure.

Abstract

Based on first principles density functional theory calculations we explored energetics of oxygen reduction reaction over pristine and nitrogen-doped graphene with different amounts of nitrogen doping. The process of oxygen reduction requires one more step then same reaction catalyzed by metals. Results of calculations evidence that for the case of light doped graphene (about 4% of nitrogen) energy barrier for each step is lower than for the same process on Pt surface. In contrast to the catalysis on metal surface the maximal coverage of doped graphene is lower and depends on the corrugation of graphene. Changes of the energy barriers caused by oxygen load and corrugation are also discussed.