In this study, we report a novel, one-step synthesis method to fabricate multilayer graphene (MLG)-wrapped copper nanoparticles (CuNPs) directly on various substrates (e.g., polyimide film (PI), carbon cloth (CC), or Si wafer (Si)). The electrical resistivities of the pristine MLG-CuNPs/PI and MLG-CuNPs/Si were measured 1.7 × 10-6 and 1.4 × 10-6 ω·m, respectively, of which both values are ∼100-fold lower than earlier reports. The MLG shell could remarkably prevent the Cu nanocore from serious damages after MLG-CuNPs being exposed to various harsh conditions. Both MLG-CuNPs/PI and MLG-CuNPs/Si retained almost their conductivities after ambient annealing at 150 °C. Furthermore, the flexible MLG-CuNPs/PI exhibits excellent mechanical durability after 1000 bending cycles. We also demonstrate that the MLG-CuNPs/PI can be used as promising source-drain electrodes in fabricating flexible graphene-based field-effect transistor (G-FET) devices. Finally, the MLG-CuNPs/CC was shown to possess high performance and durability toward hydrogen evolution reaction (HER).
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