Monolayer Amorphous Carbon-Bridged Nanosheet Mesocrystal: Facile Preparation, Morphosynthetic Transformation, and Energy Storage Applications

Abstract

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 SnS 2 . Experimentally, we show that high pressure both enhances the adsorption energy of the surfactant sodium dodecylbenzene sulfonate (SDBS) on the SnS 2 (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 carbonbridged nanosheet mesocrystal. It is notable that such a nanosheetcoalesced 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 FeCl 3induced 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/FeCl 3 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).

High-Performance Lithium-Ion Capacitors Based on 3D Interconnected Nitrogen-Doped Ultrathin Carbon Frameworks with Encapsulated Fe2O3 Nanoparticles

“…29 Due to the polymerization of the pyrrole monomer initiated by Fe 3+ in a pyrrole atmosphere (Figure S2), Fe 3+ @NaCl was translated into PPy@Fe 3+ @ NaCl. 30 Besides, it could be observed that the boundaries of PPy@Fe 3+ @NaCl became obscure as NaCl partially dissolved in ethanol (Figure 1c). 3DNC@ Fe 2 O 3 @NaCl-X was obtained by heating PPy@Fe 3+ @NaCl at the temperature of X (X = 650, 700, and 750 °C).…”

“…Subsequently, Fe 3+ @NaCl and pyrrole were placed in a sealed bottle at 35 °C to realize the gas coating process (Figure S1). Due to the polymerization of the pyrrole monomer initiated by Fe 3+ in a pyrrole atmosphere (Figure S2), Fe 3+ @NaCl was translated into PPy@Fe 3+ @NaCl . Besides, it could be observed that the boundaries of PPy@Fe 3+ @NaCl became obscure as NaCl partially dissolved in ethanol (Figure c).…”

Facile Synthesis of Graphene with Fast Ion/Electron Channels for High-Performance Symmetric Lithium-Ion Capacitors

“…The initial Coulombic efficiencies of MRPG and MRPG/CNT are calculated to be 39.3% and 44.9%, respectively, and MRPG/CNT shows a higher initial Coulombic efficiency. Nevertheless, the initial Coulombic efficiencies of MRPG and MRPG/CNT are lower compared with graphite and metal oxides/sulfides . This is mainly due to the large specific surface area of MRPG and MRPG/CNT, which needs to decompose a large amount of electrolyte to form the stabilized solid electrolyte interphase (SEI), resulting in low initial Coulombic efficiency.…”

“…Nevertheless, the initial Coulombic efficiencies of MRPG and MRPG/CNT are lower compared with graphite 44 and metal oxides/sulfides. 45 This is mainly due to the large specific surface area of MRPG and MRPG/CNT, which needs to decompose a large amount of electrolyte to form the stabilized solid electrolyte interphase (SEI), resulting in low initial Coulombic efficiency. In addition, we have studied the change in GO and CNT mass ratio to the electrochemical performance (Table S1).…”

Recent Progresses on Applications of Conducting Polymers for Modifying Electrode of Rechargeable Batteries

“…[34,35] Furthermore, the carbon material obtained by carbonization of CPs also have these advantages of higher stability compared with CPs precursor while inhibiting side reactions and improving electron transport brought by doping heteroatomic atoms. [36,37] To summarize, CPs and their derivatives could contribute to enhance charge transfer and inhibit parasitic reaction, which significantly improve the electrochemical performance of high specific capacity electrodes.…”