Aluminum and Nitrogen Codoped Graphene: Highly Active and Durable Electrocatalyst for Oxygen Reduction Reaction

The development of a highly active and exceedingly durable electrocatalyst at low cost for the oxygen reduction reaction (ORR) is extremely desirable but remains to be a grand challenge. Over the past decade, the transitional-metal (e.g., Fe, Co, Ni) and N codoped graphene materials have attracted most attention as the state-of-the-art nonprecious-metal-based effective electrocatalyst for ORR but still entail unsatisfactory issues such as moderate activity and life. Herein, the main-group-metal Al and N codoped graphene (ANG) is successfully fabricated via thermal annealing treatment of N-doped graphene with aluminum tri-(8-hydroxyquinoline). As a highly effective electrocatalyst for ORR, the as-prepared ANG exhibits not only high electrocatalytic activity that even outperforms the commercial Pt/C but also good durability in both three-electrode cell and Zn-air battery. Theoretical calculations show that the inhomogeneous charge density distribution and the interaction between Al and N are mainly responsible for the marked enhancement of ORR activity. The designed ANG electrocatalysts will provide a perspective application in energy storage and promote further exploration of main-group-element-based inexpensive, active, and durable electrocatalysts.