Endogenous Interfacial Mo−C/N−Mo‐S Bonding Regulates the Active Mo Sites for Maximized Li+ Storage Areal Capacity

Abstract Active sites, mass loading, and Li‐ion diffusion coefficient are the benchmarks for boosting the areal capacity and storage capability of electrode materials for lithium‐ion batteries. However, simultaneously modulating these criteria to achieve high areal capacity in LIBs remains challenging. Herein, MoS 2 is considered as a suitable electroactive host material for reversible Li‐ion storage and establish an endogenous multi‐heterojunction strategy with interfacial Mo−C/N−Mo‐S coordination bonding that enables the concurrent regulation of these benchmarks. This strategy involves architecting 3D integrated conductive nanostructured frameworks composed of Mo 2 C‐MoN@MoS 2 on carbon cloth (denoted as C/MMMS) and refining the sluggish kinetics in the MoS 2 ‐based anodes. Benefiting from the rich hetero‐interface active sites, optimized Li adsorption energy, and low diffusion barrier, C/MMMS reaches a mass loading of 12.11 mg cm −2 and showcases high areal capacity and remarkable rate capability of 9.6 mAh cm −2 @0.4 mA cm −2 and 2.7 mAh cm −2 @6.0 mA cm −2 , respectively, alongside excellent stability after 500 electrochemical cycles. Moreover, this work not only affirms the outstanding performance of the optimized C/MMMS as an anode material for supercapacitors, underscoring its bifunctionality but also offers valuable insight into developing endogenous transition metal compound electrodes with high mass loading for the next‐generation high areal capacity energy storage devices.