Regeneration of single-atom catalysts deactivated under acid oxygen reduction reaction conditions

Abstract

Single-atom catalysts serve as a promising candidate to realize noble-metal-free electrocatalytic oxygen reduction in acid media. However, their poor stability under working conditions strictly restrains their practical applications. Therefore, regeneration of their electrocatalytic activity is of great significance. Herein, the regeneration of a Fe–N–C single-atom catalyst is demonstrated to be feasible by a facile annealing regeneration strategy. The activity after regeneration recovers to that of the pristine electrocatalyst and surpasses the deactivated electrocatalyst. The regeneration mechanism is identified to be self-etching of the surface carbon layer and consequent exposure of the previously buried single-atom sites. Furthermore, the regeneration strategy is applicable to other single-atom catalysts. This work demonstrates the feasibility of regenerating oxygen reduction electrocatalysts and affords a pioneering approach to deal with rapid deactivation under working conditions.