Yolk–Shell Nanoreactors With Dual Confinement and Catalysis for High-Performance Lithium−Sulfur Batteries

Abstract

The practical application of lithium−sulfur (Li−S) batteries is hindered by the shuttle effect of soluble lithium polysulfides and sluggish sulfur redox kinetics, resulting in rapid capacity fading and limited cycle life. Here, we present a rationally engineered yolk–shell nanoreactor architecture that integrates dual confinement and catalytic functionality to address these challenges. The nanoreactor comprises a polar, catalytically active core encapsulated within a conductive nitrogen-doped carbon shell, offering synergistic physical restriction of polysulfides and accelerated multistep sulfur conversion. Density functional theory calculations reveal uniformly low-energy barriers along the Li₂S₈-to-Li₂S pathway, with no evident rate-limiting step. Benefiting from this cooperative design, the sulfur host achieves a ultralow capacity decay (0.028% per cycle over 1000 cycles at 2 C) and enables a high areal capacity (493 mAh g⁻¹ at 4.3 mg cm⁻² sulfur loading) with 76.3% retention after 100 cycles at 0.3 C. This work offers a versatile strategy for constructing catalysis-integrated sulfur hosts and highlights the potential of yolk–shell nanoreactors in advancing practical Li−S energy storage systems.

Keywords

dual confinement and catalysis / high sulfur loading / lithium−sulfur batteries / polysulfide conversion kinetics / yolk–shell nanoreactors

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2025 The Author(s). Carbon Neutralization published by Wenzhou University and John Wiley & Sons Australia, Ltd.