Laser-Derived Interfacial Confinement Enables Planar Growth of 2D SnS(2) on Graphene for High-Flux Electron/Ion Bridging in Sodium Storage

Establishing covalent heterointerfaces with face-to-face contact is promising for advanced energy storage, while challenge remains on how to inhibit the anisotropic growth of nucleated crystals on the matrix. Herein, face-to-face covalent bridging in-between the 2D-nanosheets/graphene heterostructure is constructed by intentionally prebonding of laser-manufactured amorphous and metastable nanoparticles on graphene, where the amorphous nanoparticles were designed via the competitive oxidation of Sn-O and Sn-S bonds, and metastable feature was employed to facilitate the formation of the C-S-Sn covalent bonding in-between the heterostructure. The face-to-face bridging of ultrathin SnS(2) nanosheets on graphene enables the heterostructure huge covalent coupling area and high loading and thus renders unimpeded electron/ion transfer pathways and indestructible electrode structure, and impressive reversible capacity and rate capability for sodium-ion batteries, which rank among the top in records of the SnS(2)-based anodes. Present work thus provides an alternative of constructing heterostructures with planar interfaces for electrochemical energy storage and even beyond. [Image: see text] SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40820-022-00829-1.