Large-scale synthesis of N-doped carbon capsules supporting atomically dispersed iron for efficient oxygen reduction reaction electrocatalysis
Hui Yang, Yanfang Liu, Xiaolu Liu, Xiangke Wang, He Tian, Geoffrey I. N. Waterhouse, Paul E. Kruger, Shane G. Telfer, Shengqian Ma
Abstract
The large-scale synthesis of platinum-free electrocatalysts for the oxygen reduction reaction (ORR) remains a grand challenge. We report the large-scale production of stable and active ORR electrocatalysts based on iron, an earth-abundant element. A core–shell zeolitic imidazolate framework–tannic acid coordination polymer composite ([email protected]) was utilized as the catalyst precursor, which was transformed into iron atoms dispersed in hollow porous nitrogen-doped carbon capsules (H-Fe-Nx-C) through ion exchange and pyrolysis. H-Fe-Nx-C features site-isolated single-atom iron centers coordinated to nitrogen in graphitic layers, high levels of nitrogen doping, and high permeability to incoming gases. Benefiting from these characteristics, H-Fe-Nx-C demonstrated efficient electrocatalytic activity (E1/2 = 0.92 V, vs. RHE) and stability towards the ORR in both alkaline and acidic media. In ORR performance, it surpassed the majority of recently reported Fe-N-C catalysts and the standard Pt/C catalyst. In addition, H-Fe-Nx-C showed outstanding tolerance to methanol.