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.

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Despite the high specific capacity of silicon as a promising anode material for the next-generation high-capacity Li-ion batteries (LIBs), its practical applications are impeded by the rapid capacity decay during cycling. To tackle the issue, herein, a bindergrafting strategy is proposed to construct a covalently cross-linked binder [carboxymethyl cellulose/phytic acid (CMC/PA)], which builds a robust branched network with more contact points, allowing stronger bonds with Si nanoparticles by hydrogen bonding. Benefitting from the enhanced mechanical reliability, the resulting Si-CMC/PA electrodes exhibit a high reversible capacity with improved long-term cycling stability. Moreover, an assembled full cell consisting of the as-obtained Si-CMC/PA anode and commercial LiFePO 4 cathode also exhibits excellent cycling performance (120.4 mA h g −1 at 1 C for over 100 cycles with 88.4% capacity retention). In situ transmission electron microscopy was employed to visualize the binding effect of CMC/PA, which, unlike the conventional CMC binder, can effectively prevent the lithiated Si anodes from cracking. Furthermore, the combined ex situ microscopy and X-ray photoelectron spectroscopy analysis unveils the origin of the superior Li-ion storage performance of the Si-CMC/PA electrode, which arises from its excellent structural integrity and the stabilized solid−electrolyte interphase films during cycling. This work presents a facile and efficient binder-engineering strategy for significantly improving the performance of Si anodes for next-generation LIBs.

Lithium (Li) metal batteries with high energy density are of great promise for next-generation energy storage; however, they suffer from severe Li dendritic growth and an unstable solid electrolyte interphase. In this study, a mixed ionic and electronic conductive (MIEC) interphase layer with an adjustable ratio assembled by ZnO and Zn nanoparticles is developed. During the initial cycle, the in situ formed Li2O with high ionic conductivity and a lithiophilic LiZn alloy with high electronic conductivity enable fast Li+ transportation in the interlayer and charge transfer at the ion/electron conductive junction, respectively. The optimized interface kinetics is achieved by balancing the ion migration and charge transfer in the MIEC Li2O–LiZn interphase. As a result, the symmetric cell with MIEC interphase delivers superior cycling stability of over 1200 h. Also, Li||Zn-ZnO@PP||LFP (LFP = LiFePO4) full cells exhibit long cyclic life for 2000 cycles with a very high capacity retention of 91.5% at a high rate of 5 C and stable cycling for 350 cycles at a high LFP loading mass of 13.27 mg cm–2.

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As promising conversion‐type anode materials for potassium‐ion storage, transition metal chalcogenides (TMCs) exhibit high energy density but suffer severe capacity fading, which is generally ascribed to their large volume expansion and the associated structural degradation. Instead, this study emphasizes that the aggregation of nanosized TMCs during conversion reaction is a more crucial reason for the following serious electrode failures. This issue has not received enough attention, and especially the detailed aggregation mechanism and its relationship to electrode failures remains unclear. Thus, by combining in situ and ex‐situ electron microscopies, the aggregation evolution of nanosized CoS2 is systematically investigated from micro to macro scale. The aggregation originates from the coalescence of the K2S matrix during potassiation, which constantly develops into larger‐scale agglomerates as the cycling continues, eventually leading to electrode fragmentation, etc. To address this issue, an anti‐aggregation strategy is proposed through isolating CoS2 nanoparticles inside individual carbon nanoshells. Impressively, the CoS2 aggregation is strictly confined within each nanoshell, which prevents their extensive aggregation across the electrode, resulting in the superior structural and electrochemical stability. This work reveals the mechanism of aggregation‐induced electrode failures and proposes the necessity of anti‐aggregation of nanosized active materials for the design of high‐capacity electrodes.

Carbonaceous anode holds great promise for potassium-ion batteries (PIBs), however, the electrochemical performance is still unsatisfactory to meet the practical requirement due to low capacities and sluggish insertion of large...

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