Graphene exhibits properties of atomic thickness, high transparency, and high carrier mobility, which is highly desirable for a flexible transparent conductive material. However, the electronic properties of large-area chemical vapor deposition grown graphene film suffer from insulated polymer contaminations introduced by the transfer process and the easily cracked nature. Here, we report a preparation method of a transfermedium-free large-area nanofiber-reinforced graphene (a-PAN/G) film simply by annealing the electrostatically spun polyacrylonitrile (PAN) nanofibers on the graphene film. The film could be free-standing on water and suspended in air with high transparency and enhanced electrical and mechanical properties compared to that of a monolayer graphene film. The flexible transparent a-PAN/G films were demonstrated as active materials for sensitive pressure sensors. The obtained pressure sensors demonstrate high sensitivity (44.5 kPa −1 within 1.2 kPa), low operating voltage (0.01−0.5 V), and excellent stability for 5500 loading− unloading cycles, revealing promising potential applications in wearable electronics.

Plasma-enhanced chemical vapor deposition (PECVD) is an applicable route to achieve low-temperature growth of graphene, typically shaped like vertical nanowalls. However, for transparent electronic applications, the rich exposed edges and high specific surface area of vertical graphene (VG) nanowalls can enhance the carrier scattering and light absorption, resulting in high sheet resistance and low transmittance. Thus, the synthesis of laid-down graphene (LG) is imperative. Here, a Faraday cage is designed to switch graphene growth in PECVD from the vertical to the horizontal direction by weakening ion bombardment and shielding electric field. Consequently, laid-down graphene is synthesized on low-softening-point soda-lime glass (6 cm × 10 cm) at ≈580 °C. This is hardly realized through the conventional PECVD or the thermal chemical vapor deposition methods with the necessity of high growth temperature (1000 °C-1600 °C). Laid-down graphene glass has higher transparency, lower sheet resistance, and much improved macroscopic uniformity when compare to its vertical graphene counterpart and it performs better in transparent heating devices. This will inspire the next-generation applications in low-cost transparent electronics.

High-quality graphene film grown on dielectric substrates by a direct chemical vapor deposition (CVD) method promotes the application of high-performance graphene-based devices in large scale. However, due to the noncatalytic feature of insulating substrates, the production of graphene film on them always has a low growth rate and is time-consuming (typically hours to days), which restricts real potential applications. Here, by employing a local-fluorine-supply method, we have pushed the massive fabrication of a graphene film on a wafer-scale insulating substrate to a short time of just 5 min without involving any metal catalyst. The highly enhanced domain growth rate (∼37 nm min −1 ) and the quick nucleation rate (∼1200 nuclei min −1 cm −2 ) both account for this high productivity of graphene film. Further first-principles calculation demonstrates that the released fluorine from the fluoride substrate at high temperature can rapidly react with CH 4 to form a more active carbon feedstock, CH 3 F, and the presence of CH 3 F molecules in the gas phase much lowers the barrier of carbon attachment, providing sufficient carbon feedstock for graphene CVD growth. Our approach presents a potential route to accomplish exceptionally large-scale and high-quality graphene films on insulating substrates, i.e., SiO 2 , SiO 2 /Si, fiber, etc., at low cost for industry-level applications.