Abstract
We demonstrate a sustainable and efficient approach to produce high performance sulfur/carbon composite cathodes via a bottom-up catalytic approach. The selective oxidation of H2S by a nitrogen-enriched mesoporous carbon catalyst can produce elemental sulfur as a by-product which in-situ deposit onto the carbon framework. Due to the metal-free catalytic characteristic and high catalytic selectivity, the resulting sulfur/carbon composites have almost no impurities that thus can be used as cathode materials with compromising battery performance. The layer-by-layer sulfur deposition allows atomic sulfur binding strongly with carbon framework, providing efficient immobilization of sulfur. The nitrogen atoms doped on the carbon framework can increase the surface interactions with polysulfides, leading to the improvement in the trapping of polysulfides. Thus, the composites exhibit a reversible capacity of 939 mAh g−1 after 100 cycles at 0.2 C and an excellent rate capability of 527 mAh g−1 at 5 C after 70 cycles.
Highlights
We demonstrate a sustainable and efficient approach to produce high performance sulfur/carbon composite cathodes via a bottom-up catalytic approach
We recently found that the nitrogen-enriched mesoporous carbons (NMCs) can act as metal-free catalysts in their own right to directly oxidize H2S to elemental sulfur at the room temperature via the reaction H2S 1 1/2O2 R S 1 H2O27
Relative to the conventional top-down impregnation, bottom-up catalytic synthesis of NMC/S composites allows sulfur atoms being layer-by-layer deposited on the carbon framework
Summary
We demonstrate a sustainable and efficient approach to produce high performance sulfur/carbon composite cathodes via a bottom-up catalytic approach. Relative to the conventional top-down impregnation, bottom-up catalytic synthesis of NMC/S composites allows sulfur atoms being layer-by-layer deposited on the carbon framework In this way, the NMC/S composites where sulfur atoms is located very close to the conductive carbon, provide efficient immobilization of sulfur and the enhancement of electronic contacts with sulfur, as a direct consequence to improved electrochemical properties. The basic nitrogen functionalities may increase the surface interactions with polysulfide anions, leading to the improvement in the trapping of polysulfides These structural and surface chemistry features are expected to work co-operatively and lead to the NMC/S composites with high electrochemical performances
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