In-Plane Coassembly Route to Atomically Thick Inorganic–Organic Hybrid Nanosheets

Control over the anisotropic assembly of small building blocks into organized structures is considered an effective way to design organic nanosheets and atomically thick inorganic nanosheets with nonlayered structure. However, there is still no available route so far to control the assembly of inorganic and organic building blocks into a flattened hybrid nanosheet with atomic thickness. Herein, we highlight for the first time a universal in-plane coassembly process for the design and synthesis of transition-metal chalcogenide–alkylamine inorganic–organic hybrid nanosheets with atomic thickness. The structure, formation mechanism, and stability of the hybrid nanosheets were investigated in detail by taking the Co₉S₈–oleylamine (Co₉S₈–OA) hybrid nanosheets as an example. Both experimental data and theoretical simulations demonstrate that the hybrid nanosheets were formed by in-plane connection of small two-dimensional (2D) Co₉S₈ nanoplates <i>via</i> oleylamine molecules adsorbed at the side surface and corner sites of the nanoplates. X-ray absorption fine structure spectroscopy study reveals the structure distortion of the small 2D Co₉S₈ nanoplates that endows structural stability of the atomically thick Co₉S₈–OA hybrid nanosheets. The brand new atomically thick nanosheets with inorganic–organic hybrid network nanostructure will not only enrich the family of atomically thick 2D nanosheets but also inspire more interest in their potential applications