Build a Rigid–Flexible Graphene/Silicone Interface by Embedding SiO(2) for Adhesive Application

[Image: see text] An effective strategy was developed to enhance the adaptability of graphene/silicone matrices under external stimuli by embedding nanoscale SiO(2) into the graphene/silicone interfaces as a buffer layer. Chemically reduced graphene (rGE) was first covered by SiO(2) using an in situ preparation, forming sandwichlike rGE/SiO(2) (rGES). Then, rGES was integrated into methyl vinyl polysiloxane, followed by vulcanization, producing the final rGES/silicone rubber (SR) nanocomposite. Such interfacial modification actually built a rigid–flexible SiO(2) buffer layer between rGE and polysiloxane. Obvious improvements were seen in both thermal and mechanical properties due to improved interfacial interaction. In a vulcanized rGES/SR system, the addition of 30 wt % rGES (3 wt % rGE) yielded a tensile strength of 6.13 MPa (up to 25 times that of the unmodified rGE in filled SR), a tear strength of 18.08 kN/m, and an elongation at break of 267%, several times higher than those of an rGE/SR nanocomposite. Thermal analysis results indicated that the initial decomposition temperature of rGES/SR containing 5 wt % rGES (0.5 wt % rGE) increased by more than 98 and 288 °C compared to that of SiO(2)/SR and rGE/SR, respectively. The rGES/polysiloxane matrices showed a tensile shear adhesive strength of 1.78 MPa when used as an adhesive for aluminum sheets, which is higher than that of the rGE/polysiloxane matrix (0.93 MPa).