Based on first-principles DFT calculations, copper-nitrogen embedded graphene (CuN₃-Gra) is introduced as an efficient electrocatalyst for oxygen reduction reaction (ORR) in fuel cells. The possible reaction mechanisms as well as the corresponding stationary points on potential energy surfaces are studied in acidic media. Our results indicate that dissociation of O₂ over CuN₃-Gra cannot occur at normal condition due to its large energy barrier. In contrast, the O₂ hydrogenation into OOH, followed by the hydrogenation of OOH into O and H₂O species is the most favorable pathway for the ORR process. The energy barrier for rate-determining step of this reaction is calculated to be 1.00 eV which is related to the formation of first H₂O molecule. The free energy diagrams reveal that for OOH hydrogenation pathway, all of the elementary steps are exothermic at potentials 0.0–0.8 V.

基于第一性原理DFT计算，铜氮嵌入石墨烯（CuN ₃ -Gra）被引入作为燃料电池中氧还原反应（ORR）的有效电催化剂。在酸性介质中研究了可能的反应机理以及势能表面上的相应固定点。我们的结果表明，由于其较大的能垒，在正常条件下O ₂不会在CuN ₃ -Gra上发生解离。相反，O ₂氢化为OOH，然后OOH氢化为O和H ₂O种是ORR过程中最有利的途径。该反应的速率确定步骤的能垒经计算为1.00 eV，与第一H ₂ O分子的形成有关。自由能图显示，对于OOH氢化途径，所有基本步骤在0.0-0.8 V的电势下都放热。