Spatially coupled adsorption and catalysis for sustainable lithium–sulfur batteries

Lithium–sulfur batteries have been considered a promising energy storage technology for maximizing sustainability, owing to their ultrahigh theoretical energy density and the abundant supply of low-cost sulfur. However, their high-energy advantage is often compromised in practice by the heavy, voluminous host materials and catalysts required to mitigate the polysulfide shuttle effect and sluggish redox kinetics. Here we address this dilemma by spatially coupling adsorption and catalytic sites within an sp-nitrogen-doped graphdiyne multishelled architecture. This design enables an exceptional sulfur loading of 93.9%, achieving a close-to-theoretical capacity of 1,462 mAh g_(S+host)⁻¹ and a pouch-cell energy density of ~457 Wh kg⁻¹. Even at a high rate of 10C, the system maintains an energy density of 1,384.5 Wh kg_(S+host)⁻¹ over 600 cycles. In situ spectroscopic characterizations and theoretical calculations reveal that the favourable orbital overlapping between sp-nitrogen and neighbouring carbon facilitates rapid electron transfer and optimized charge redistribution, thus simultaneously promoting the adsorption and redox reaction of polysulfides. By minimizing inactive mass, this work provides a scalable blueprint for high-performance, resource-efficient battery chemistries.