First-Principles investigation of H2O2 electrosynthesis on Cu-C24N24 single-atom catalyst

Abstract

Hydrogen peroxide (H₂O₂) is an important chemical. The direct synthesis of H₂O₂ has been identified as an environmentally friendly process through the two-electron oxygen reduction reaction (2e^- ORR) under acidic conditions. Nevertheless, the reliance of this technique on expensive electrocatalysts derived from precious metals significantly impedes its practicality for large-scale industrial application. In our study, based on density functional theory calculations, we prove that Cu-modified C₂₄N₂₄ (Cu-C₂₄N₂₄) single-atom catalyst (SAC) is an efficient electrocatalyst based on non-noble metals for 2e^- ORR. The results show that Cu-C₂₄N₂₄, Pd-C₂₄N₂₄, Pt-C₂₄N₂₄, and Rh-C₂₄N₂₄ possess good stability. In addition, the Cu-C₂₄N₂₄ SAC exhibits an ideal OOH* binding energy of 4.26 eV, leading to a notably optimal catalytic activity for 2e^- ORR. What is more, the Cu-C₂₄N₂₄ SAC shows a preference for aiding in H₂O₂ production over the rival 4e^- ORR with an overpotential of merely 0.04 V. Given these desirable properties, the Cu-C₂₄N₂₄ SAC emerges as a promising option for facilitating 2e^- ORR.