ABSTRACT Silicon anodes offer high theoretical capacity for lithium‐ion batteries but suffer from volume‐change‐induced instability and degradation. Conventional van der Waals coatings yield unstable interfaces and poor ion/electron transport, while thermal transport remains underexplored. Here, we propose heterointerface‐engineered Si@MoSe 2 @C anodes with chemically bonded interfaces, where lattice‐matched MoSe 2 covalently bridges porous Si and carbon coating, forming robust Si─Se─Mo linkages that stabilize the structure and optimize transport pathways. The Si@MoSe 2 @C anode delivers 1054 mAh g −1 after 100 cycles at 0.2 A g −1 —exceeding most Si anodes—and 99.5% Coulombic efficiency over 400 cycles at 1.0 A g −1 , with high cycling efficiency demonstrated in both liquid and all‐solid‐state lithium‐ion batteries (ASSLIBs). In situ X‐ray diffraction, Raman spectroscopy, and electron microscopy/spectroscopy, together with first‐principles calculations, confirm that this MoSe 2 ‐mediated covalent bridging enables reversible reactions with favorable kinetics and structural integrity by strengthening and delocalizing Se─Si bonding and reducing Li + migration barriers by 24%. Critically, we present the first measurements of the effective thermal conductivity of a silicon‐anode composite, showing that Si@MoSe 2 @C exhibits a 27% higher value than Si, addressing long‐overlooked cell‐level thermal‐management requirements and improving elevated‐temperature cell performance. This heterointerface design provides a synergistic strategy for engineering high‐performance Si anodes across batteries with enhanced safety.
Zhu et al. (Sat,) studied this question.
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