Effect of Different N/C Coordination Electronic Structures on the Activity of Bifunctional Rare-Earth Ytterbium Electrocatalysts for Oxygen Electrodes.

The research and development of bifunctional electrocatalysts for the oxygen electrode is of great significance to solve the problem of electrochemical energy. Herein, the effect of different structure-activity relationships on the performance of YbNC-gra catalysts was explored. The bifunctional activity of graphene with a vacancy defect supported by single-atom rare-earth ytterbium was studied by density functional theory (DFT) calculations. We systematically analyzed the stability, electronic properties, and catalytic performance of potential bifunctional catalysts. The results showed that all catalysts were thermodynamically and kinetically stable. Under acidic conditions, YbNC-oppo-gra and YbNC-pen-gra showed good ORR activity, and their overpotentials were 0.53 and 0.65 V, respectively. In an alkaline environment, most of the YbNC-gra catalysts showed excellent ORR and OER bifunctional catalytic activity. Their overpotentials were all below 0.6 V. In particular, the η and η of the YbNC-gra electrocatalyst were as low as 0.33 and 0.42 V. This verified the practicability and feasibility of hydroxyl-modified catalysts to enhance activity. This research provides theoretical insights into the further design and development of high-efficiency rare-earth-supported bifunctional catalysts.