关键字：TOTAL-ENERGY CALCULATIONS; RECENT PROGRESS; CATALYSTS; CARBON

摘要：In recent years, non-precious-metal-doped single-atom catalysts have emerged as promising alternatives to Pt- based catalysts due to their high active site density and excellent oxygen reduction reaction (ORR) activity. However, challenges arise in precisely controlling the doping precision of metal atoms during experimental preparation, often resulting in clustering of metal atoms. The impact of these metal clusters on catalytic activity remains unclear. Here employing density functional theory, we investigated a series of N-doped graphene based catalysts, including MN4, MN4@M4-Py, MN4@M4-Qu (M = Cr, Mn, Fe, Co, Ni, Cu, Zn, Ru, Rh, Pd, Ag, Ir, Pt), to elucidate changes in catalyst properties upon metal cluster loading and assess how different configurations of metal clusters influence ORR activity. Our findings reveal synergistic interactions between metal clusters and single atoms, which can either enhance or inhibit catalytic activity depending on elemental types and cluster configurations. Remarkably, the CoN4@Co4-Py catalyst exhibits superior ORR catalytic performance, with an overpotential of 0.277 V. This study not only sheds light on the synergistic effects between metal clusters and catalysts, but also offers theoretical insights for the experimental preparation of catalysts.

卷号：233

期号：-

是否译文：否