Synergistic Engineering of Heterointerface and Architecture in New-Type ZnS/Sn Heterostructures In Situ Encapsulated in Nitrogen-Doped Carbon Toward High-Efficient Lithium-Ion Storage

Engineering heterogeneous composite electrodes consisting of multiple active components for meeting various electrochemical and structural demands have proven indispensable for significantly boosting the performance of lithium-ion batteries (LIBs). Here, a novel design of ZnS/Sn heterostructures with rich phase boundaries concurrently encapsulated into hierarchical interconnected porous nitrogen-doped carbon frameworks (ZnS/Sn@NPC) working as superior anode for LIBs, is showcased. These ZnS/Sn@NPC heterostructures with abundant heterointerfaces, a unique interconnected porous architecture, as well as a highly conductive N-doped C matrix can provide plentiful Li⁺-storage active sites, facilitate charge transfer, and reinforce the structural stability. Accordingly, the as-fabricated ZnS/Sn@NPC anode for LIBs has achieved a high reversible capacity (769 mAh g⁻¹, 150 cycles at 0.1 A g⁻¹), high-rate capability and long cycling stability (600 cycles, 645.3 mAh g⁻¹ at 1 A g⁻¹, 92.3% capacity retention). By integrating in situ/ex situ microscopic and spectroscopic characterizations with theoretical simulations, a multiscale and in-depth fundamental understanding of underlying reaction mechanisms and origins of enhanced performance of ZnS/Sn@NPC is explicitly elucidated. Furthermore, a full cell assembled with prelithiated ZnS/Sn@NPC anode and LiFePO₄ cathode displays superior rate and cycling performance. This work highlights the significance of chemical heterointerface engineering in rationally designing high-performance electrodes for LIBs.