Monolayer Amorphous Carbon-Bridged Nanosheet Mesocrystal: Facile Preparation, Morphosynthetic Transformation, and...

Self-assembly of nanoscale building units into mesoscopically ordered superstructures opens the possibility for tailored applications. Nonetheless, the realization of precise controllability related specifically to the atomic scale has been challenging. Here, first, we explore the key role of a molecular surfactant in adjusting the growth kinetics of two-dimensional (2D) layered SnS₂. Experimentally, we show that high pressure both enhances the adsorption energy of the surfactant sodium dodecylbenzene sulfonate (SDBS) on the SnS₂(001) surface at the initial nucleation stage and induces the subsequent oriented attachment (OA) growth of 2D crystallites with monolayer thickness, leading to the formation of a monolayer amorphous carbon-bridged nanosheet mesocrystal. It is notable that such a nanosheet-coalesced mesocrystal is metastable with a flowerlike morphology and can be turned into a single crystal via crystallographic fusion. Subsequently, direct encapsulation of the mesocrystal via FeCl₃-induced pyrrole monomer self-polymerization generates conformal polypyrrole (PPy) coating, and carbonization of the resulting nanocomposites generates Fe-N-S-co-doped carbons that are embedded with well-dispersed SnS/FeCl₃ quantum sheets; this process skillfully integrated structural phase transformation, pyrolysis graphitization, and self-doping. Interestingly, such an integrated design not only guarantees the flowerlike morphology of the final nanohybrids but also, more importantly, allows the thickness of petalous carbon and the size of the nanoconfined particles to be controlled. Benefiting from the unique structural features, the resultant nanohybrids exhibited the brilliant electrochemical performance while simultaneously acting as a reliable platform for exploring the structure-performance correlation of a Li-ion battery (LIB).