Enhancement of Electrocatalytic Oxygen Reduction Reaction and Oxygen Evolution Reaction by Introducing Lanthanum Species in the Carbon Shell.

Abstract

The development of cost-effective non-noble metal electrocatalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) opens up the possibility for sustainable energy systems. Herein, we report a surface overcoating strategy with lanthanum organic complex (La-OC) as the precursor to prepare lanthanum species (La-SPc) encapsulated in nitrogen, fluorine, and sulfur self-doped porous carbon (NFS-PC) composites (La-SPc@NFS-PC) for efficient ORR and OER. The La-SPc is introduced not only as a promoter to increase the electrochemical stability of the La-SPc@NFS-PC catalysts but also to tailor the electronic structure of NFS-PC due to the unique electrochemical properties of La-SPc. In addition, the integration of La-SPc and NFS-PC can improve the electronic conductivity of composites by inducing electron redistribution and lowering the band gap, which is advantageous in enhancing the kinetics of charge transfer. Simultaneously, benefiting from the optimized porous structure and positive cooperation of La-SPc with NFS-PC shells, the obtained La-SPc@NFS-PC-3 delivers robust bifunctional ORR/OER activities and stabilities. More importantly, the Zn-air battery (ZAB) assembled with La-SPc@NFS-PC-3 demonstrates an outstanding power density (181.1 mW cm-2) and long cycling life, outperforming the commercial Pt/C. This work offers a rational approach to preparing high-efficiency rare-earth-based catalysts and provides potential applications in ZABs.