Drastically-enlarged interlayer-spacing MoS2 nanocages by inserted carbon motifs as high performance cathodes for aqueous zinc-ion batteries

• Preparation of unique MoS 2 nanocages with 3D hollow structure. • The preparation method from bottom to top is used to introduce N-doped carbon motifs between the layers of MoS 2 to ensure the uniformity and stability of the electrode material. • The novel MoS 2 exhibit excellent high rate performance and excellent cycling stability when applied as cathodes for AZIBs. • The energy storage mechanism regarding highly reversible of zinc ion (de)insertion is elucidated through in-situ XRD and ex-situ Raman technology. • The calculation of density functional theory further reveals the reduction of the ion diffusion barrier accelerates the electrochemical kinetics. Two dimensional (2D) layered nanomaterials have emerged as a promising energy storage material due to inherent 2D channels. Nevertheless, low capacity and poor cycling stability limit their practical applications in aqueous zinc ion batteries (AZIBs). The article innovatively introduces N-doped carbon motifs between the layers of MoS 2 to produce the interlayer spacing enlarged MoS 2 nanocages with multistage structures, via a strategy combining interlayer polymerization with template assistance. NC motifs provided abundant channels for substance transport and electron transfer. Cage-shaped structure inhibits stacking of nanosheets during synthesis and application, and alleviates volume changes caused by ion migration during (dis)charging. Therefore, this novel MoS 2 exhibit excellent high rate performance (247.8 mA h g −1 at 0.1 A g −1 and 100.9 mA h g −1 at 8.0 A g −1 ) and excellent cycling stability (85.6 % capacity retention after 3200 cycles at 1.0 A g −1 ) when applied as cathodes for AZIBs. The flexible quasi-solid batteries based on C-MoS 2 -NC cathode exhibit excellent electrochemical performance under different bending conditions. The energy storage mechanism regarding highly reversible of zinc ion (de)insertion is elucidated through in-situ XRD and ex-situ Raman technology. The calculation of density functional theory further reveals the reduction of the ion diffusion barrier accelerates the electrochemical kinetics. As an attractive candidate battery for smart grid and large energy storage systems (ESS), aqueous zinc ion batteries (AZIBs) have been extensively researched due to high security and high specific capacity. Here, the authors report a strategy of combining in-situ interlayer polymerization and template method for bottom-up constructing 2D MoS 2 nanosheets with nitrogen-doped carbon interlayer modification into 3D hollow nanocages, exhibiting excellent zinc ion storage performance.