Abstract
In recent years, a growing interest in “beyond-Li-ion“ batteries has caused a speedy development of alternative battery technologies based on other alkali metals. Room temperature sodium sulfur (RT Na-S) batteries are potential candidate for sustainable large-scale energy storage systems. They offer low cost, nontoxicity and natural abundance of both cathode and anode materials combined with high theoretical energy density. However, rapid capacity fading related to the irreversible shuttling of soluble polysulfides, poor reaction kinetics and low sulfur utilisation in the cathode materials significantly limit their practical application.In this work, a microporous sulfur-carbon complex is produced from sustainable natural precursors in a one-pot synthesis via stepwise thermally-induced inverse vulcanisation and condensation. The material exhibits a unique structure, with sulfur chains covalently anchored to the conductive carbon matrix and physically confined in ultra-micropores. An increase in sulfur content in the sulfur-copolymer alters the morphology and chemical composition of the final sulfur-carbon material, enhancing the amount of long-chain sulfur. The combination of optimal microstructure, good electrical conductivity and high content of electrochemically active sulfur translates to an unprecedented ~99% utilisation of sulfur and the highest reported capacity for a room temperature Na-S cathode, along with high rate capability, coulombic efficiency and long-term stability. This study offers an innovative approach towards the understanding of the key chemico-physical properties of the sulfur-carbon composite materials for the development of high-performance cathodes in RT Na-S batteries with an atom-efficient utilisation of sulfur.
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