Iron-Salt Thermally Emitted Strategy to Prepare Graphene-like Carbon Nanosheets with Trapped Fe Species for an Efficient Electrocatalytic Oxygen Reduction Reaction in the All-pH Range

Earth-abundant, highly active, and durable electrocatalysts toward oxygen reduction reaction (ORR) in the all-pH range are highly required for practical application of electrochemical energy conversion technologies. Here, non-noble-metal graphene-like carbon nanosheets with trapped Fe species (Fe-N/GPC) are developed by an iron-salt thermally emitted strategy, which integrates the modulation of the electronic structure for boosted intrinsic activity with the engineering of hierarchical porosity for enriched active sites. The ORR electrocatalytic performance of Fe-N/GPC-800 achieves the half-wave potentials of 0.86 and 0.77 V with limiting current densities of 6.1 and 4.7 mA cm–2 in 0.1 M KOH and 0.1 M PBS solutions, respectively, as well as respectable stability. Furthermore, Fe-N/GPC-800 also shows considerable ORR catalytic activity in acid media accompanied by stability superior to those of Pt/C catalysts. The as-prepared Fe-N/GPC-800, as a cathodic catalyst, is assessed in a Zn–air battery test and delivers an open-circuit voltage of 1.44 V with a power density of 134 mW cm–2 as well as the outstanding durability after 350 cycles at 10 mA cm–2, demonstrating appreciable promise in application of metal–air batteries. This work provides an enabling and versatile strategy for facile and scale-up preparation of high-performance non-noble-metal electrocatalysts.