Amylose-Derived Macrohollow Core and Microporous Shell Carbon Spheres as Sulfur Host for Superior Lithium–Sulfur Battery Cathodes

Porous carbon can be tailored to great effect for electrochemical energy storage. In this study, we propose a novel structured spherical carbon with a macrohollow core and a microporous shell derived from a sustainable biomass, amylose, by a multistep pyrolysis route without chemical etching. This hierarchically porous carbon shows a particle distribution of 2–10 μm and a surface area of 672 m2 g–1. The structure is an effective host of sulfur for lithium–sulfur battery cathodes, which reduces the dissolution of polysulfides in the electrolyte and offers high electrical conductivity during discharge/charge cycling. The hierarchically porous carbon can hold 48 wt % sulfur in its porous structure. The S@C hybrid shows an initial capacity of 1490 mAh g–1 and retains a capacity of 798 mAh g–1 after 200 cycles at a discharge/charge rate of 0.1 C. A capacity of 487 mAh g–1 is obtained at a rate of 3 C. Both a one-step pyrolysis and a chemical-reagent-assisted pyrolysis are also assessed to obtain porous carbon from amylose, but the obtained carbon shows structures inferior for sulfur cathodes. The multistep pyrolysis and the resulting hierarchically porous carbon offer an effective approach to the engineering of biomass for energy storage. The micrometer-sized spherical S@C hybrid with different sizes is also favorable for high-tap density and hence the volumetric density of the batteries, opening up a wide scope for practical applications.