Fabrication and application of flexible graphene silk composite film electrodes decorated with spiky Pt nanospheres

A free-standing graphene silk composite (G/S) film was fabricated via vacuum filtration of a mixed suspension of graphene oxide and silk fibres, followed by chemical reduction. Spiky structured Pt nanospheres were grown on the film substrate by cyclic voltammetry electrodeposition. The electrical and mechanical performance of a single graphene coated silk fibre was investigated. The conductivity of a single graphene coated silk fibre is 57.9 S m(-1). During 1000 bending measurements, the conductivity was stable and showed negligible variation. The G/S film has a sheet resistivity of 90 Ω □(-1) with a porous and hierarchical structure. The spiky Pt nanosphere decorated G/S film was directly used as a H₂O₂ electrode with a sensitivity of 0.56 mA mM(-1) cm(-2), a linear range of 0-2.5 mM and an ultralow detection limit of 0.2 μM (S/N = 3). A glucose biosensor electrode was further fabricated by enzyme immobilization. The results show a sensitivity of 150.8 μA mM(-1) cm(-2) and a low detection limit of 1 μM (S/N = 3) for glucose detection. The strategy of coating graphene sheets on a silk fibre surface provides a new approach for developing electrically conductive biomaterials, tissue engineering scaffolds, bendable electrodes, and wearable biomedical devices.