Influence of morphology of monolithic sulfur-poly(acrylonitrile) composites used as cathode materials in lithium-sulfur batteries on electrochemical performance

Solvent-induced phase separation (SIPS) and thermally-induced phase separation (TIPS) derived poly(acrylonitrile) (PAN) based monoliths with different morphology and specific surface area were prepared and thermally converted into monolithic sulfur-poly(acrylonitrile) (SPAN) materials for use as active cathode materials in lithium-sulfur batteries. During thermal processing, the macroscopic monolithic structure fully prevailed while significant changes in porosity were observed. Both the monomer content in the precursor PAN-based monoliths and the tortuosity of the final monolithic SPAN materials correlate with the electrochemical performance of the SPAN-based cathodes. Overall, percolation issues predominate. In percolating SPAN-based cathode materials, the specific capacity of the SPAN-based cells increases with decreasing tortuosity. All monolithic SPAN materials provided highly reversible and cycle stable cathodes reaching reversible discharge capacities up to 1330 mA h g_sulfur ^-1 @ 0.25C, 900 mA h g_sulfur ^-1 @ 2C and 420 mA h g_sulfur ^-1 @ 8C.