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
Affiliations
Hui Yang
College of Environmental Science and Engineering, North China Electric Power University, Beijing, 102206, PR China
Yanfang Liu
College of Environmental Science and Engineering, North China Electric Power University, Beijing, 102206, PR China
Xiaolu Liu
College of Environmental Science and Engineering, North China Electric Power University, Beijing, 102206, PR China
Xiangke Wang
College of Environmental Science and Engineering, North China Electric Power University, Beijing, 102206, PR China
He Tian
State Key Laboratory of Silicon Materials, Center of Electron Microscopy, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, PR China
Geoffrey I.N. Waterhouse
MacDiarmid Institute for Advanced Materials and Nanotechnology, School of Chemical Sciences, The University of Auckland, Auckland, 1142, New Zealand
Paul E. Kruger
MacDiarmid Institute for Advanced Materials and Nanotechnology, School of Physical and Chemical Sciences, University of Canterbury, Christchurch, 8140, New Zealand
Shane G. Telfer
MacDiarmid Institute for Advanced Materials and Nanotechnology, School of Fundamental Sciences, Massey University, Palmerston North, 4442, New Zealand
Shengqian Ma
Department of Chemistry, University of North Texas, Denton, TX, 76201, United States; Corresponding author.
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 (ZIF-8@K-TA) 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.
