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Constructing a “Pizza‐Like” MoS2/Polypyrrole/Polyaniline Ternary Architecture with High Energy Density and Superior Cycling Stability for Supercapacitors

Polypyrrole (PPy) and polyaniline (PANI) are most promising candidates for high energy and power density supercapacitors. However, their relative low surface area and poor cyclic stability greatly limit their practical applications. Morphology‐ and size‐controlled micro/nanostructure formation of such materials may lead to enhanced performance. Here, the solvent‐exchange method is proposed for the preparation of high‐concentration few‐layer MoS2 (f‐MoS2) suspension in an ethanol–water mixed solvent. PPy layers with high surface coverage are formed on the resultant dispersible f‐MoS2 by in situ polymerization of pyrrole. The MoS2/PPy hybrid is then used as the reactive layer for subsequent in situ growth and attachment of PANI, thus forming a “pizza‐like” MoS2/PPy/PANI ternary nanostructure. The rational design of such hierarchical nanostructures greatly enhances the specific capacitance up to 1273 F g−1 at 0.5 A g−1 and effectively improves the cyclic performance maintaining ≈83% after 3000 charge/discharge cycles. The excellent performances of MoS2/PPy/PANI hybrid are mainly attributed to robust interconnected frameworks for improved electrical conductivity and well‐defined porosities for enhanced electrolyte/electrode interaction. The superior electrochemical performance thus suggests a promising strategy for fabricating component adjustable, high energy density, and durable nanostructures as novel electrode materials for supercapacitors.