Li‐rich Mn‐based cathode materials (LRMs) are potential cathode materials for high energy density lithium‐ion batteries. However, low initial Coulombic efficiency (ICE) severely hinders the commercialization of LRM. Herein, a facile oleic acid‐assisted interface engineering is put forward to precisely control the ICE, enhance reversible capacity and rate performance of LRM effectively. As a result, the ICE of LRM can be precisely adjusted from 84.1% to 100.7%, and a very high specific capacity of 330 mAh g−1 at 0.1 C, as well as outstanding rate capability with a fascinating specific capacity of 250 mAh g−1 at 5 C, are harvested. Theoretical calculations reveal that the introduced cation/anion double defects can reduce the diffusion barrier of Li+ ions, and in situ surface reconstruction layer can induce a self‐built‐in electric field to stabilize the surface lattice oxygen. Moreover, this facile interface engineering is universal and can enhance the ICEs of other kinds of LRM effectively. This work provides a valuable new idea for improving the comprehensive electrochemical performance of LRM through multistrategy collaborative interface engineering technology.
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.
Li-rich layered oxide cathodes (LLOs) are widely researched since the first discovery by Thackeray et al., [1] and they are considered as promising cathode candidates for next-generation Li-ion batteries due to their extraordinary specific capacity of
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