High thermal conductivity and stretchability of layer-by-layer assembled silicone rubber/graphene nanosheets multilayered films

Thermally conductive silicone rubber composites used for heat removal from electronic devices have attracted great attention. A facile spin-assisted layer-by-layer assembly approach was used to fabricate highly thermally conductive multilayered silicone rubber/graphene films. The films exhibit highly ordered lamellar structure with the high orientation of graphene which provides continuous thermally conductive pathways in horizontal direction. A multilayered film with 40 assembly cycles has the thermal conductivity of 2.03 W/(m·K) in in-plane direction. Moreover, the film can be highly twisted to any angle and has the elongation at break of 325%, which is rarely achieved in previously reported graphene-based multilayered films. Even up to 500 stretch-recovery cycles at 50% strain, the change of the thermal conductivity was negligible, indicating the high durability, excellent flexibility and stretchability of the film. The films with high thermal conductivity and stretchability have potential applications in flexible electronics, wearable devices and electronic skin.