Powder metallurgy template growth of 3D N-doped graphene foam as binder-free cathode for high-performance lithium/sulfur battery

Abstract

Here, we present a facile technique to design self-supported 3D N-doped graphene foam (NGF) via simply annealing in chemical vapor deposition furnace which used powder metallurgy nickel template and melamine as both carbon and nitrogen source. The NGF possesses highly conductive and interconnected mesoporous network. Particularly nitrogen-doping provided strong polysulfide immobilization ability, significantly suppressing the shuttle effect. The NGF was directly used as binder-free electrode which delivered a high initial discharge capacity of 987 mA h g−1 and maintains at 819 mA h g−1 after 200 cycles at 0.2 C, corresponding to 82.9% capacity retention. Specifically, even at high current density of 2 C, it still possesses a good long life cycle performance (from 633.8 mA h g−1 to 440.3 mA h g−1 after 500 cycles, with ultralow capacity fading rate of 0.061% per cycle). 7Li nuclear magnetic resonance (7Li NMR) suggested strong interaction between NGF and polysulfide. Moreover, X-ray photoelectron spectroscopy and density function theory calculation further revealed the strong interaction mostly ascribed to chemisorption and physisorption of polysulfide by pyridinic and pyrrolic nitrogen, respectively. As we know this method-based NGF as binder free electrode was first reported, which provided an effective strategy for developing high-performance Li/S batteries.