The role of synthesis pathway on the microstructural characteristics of sulfur-carbon composites: X-ray imaging and electrochemistry in lithium battery

Abstract

Two synthesis pathways are adopted to tune the microstructural characteristics of sulfur-carbon (S-C) composites for application in lithium-sulfur (Li-S) batteries. Both methods include intimate mixing of either carbon black or multiwalled carbon nanotubes with elemental sulfur, molten according to the first approach while dispersed in alcohol and heated according to the second one. Nano- and micro-scale X-ray computed tomography supported by X-ray diffraction and electron microscopy shows materials consisting of crystalline sulfur clusters (70 wt%) with size ranging from about 5 to 50 μm, surrounded by carbon. The sulfur cluster size appears limited by direct mixing of molten sulfur and carbons, in particular when carbon black is employed, whilst it is increased by exploiting the alcohol dispersion. Electrochemistry reveals that small sulfur particles lead to an improved rate capability in Li-S cells, whereas large active material domains may favor the capacity retention. The composites using carbon black nanoparticles exhibit the highest reversible capacity, with a maximum value exceeding 1500 mAh gS−1, whereas the composites involving multiwalled carbon nanotubes show the best capacity retention, with values approaching 70% over 150 cycles. Our multi-disciplinary approach will shed light on significant aspects aiming to enhance the Li-S battery and favor a practical application.