Endowed with intrinsic redox-rich features and superior electronic conductivities, mixed-metallic sulphides offer high prospects in electrochemical charge storage, especially in supercapacitors. Hence, their rational design and scalable preparation are of great scientific significance. Herein, we report the in-situ growth of nanostructured hybrids of NiMnS directly embedded into graphene sheets by a straightforward, scalable solid-state synthesis method. In this environment-friendly approach, the metal precursors, elemental sulphur, and graphene oxide (GO) are homogeneously mixed under ball-milling, followed by controlled thermal treatment. Incited from their unique synergistic contribution, the resulting NiMnS/G hybrids exhibit impressive electrochemical performance as a battery-type electrode in an aqueous electrolyte. The NiMnS/G hybrid electrode displayed a high specific capacity of 871.7C g−1 at 2 A g−1 with superior rate capability. Moreover, the asymmetric supercapacitor (ASC) device assembled based on the surface-enhanced NiMnS/G nanohybrid as the positive electrode and activated carbon (AC) as the negative electrode achieves an intriguing performance, delivering a maximum energy density of 53.4 Wh kg−1 at a power density of 500 W kg−1. The ASCs were successfully cycled over 10,000 cycles with 87 % capacitance retention and around 99 % Coulombic efficiency. This simple yet scalable strategy holds high promise and may pave the way for preparing other multimetallic sulphide-based hybrid electrode materials for electrochemical energy storage applications.
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