The facile fabrication of functionally graded all-graphene films using a single-step casting process is reported. The films consist of a self-assembled graphene oxide (GO) precursor that can be reduced to different levels on an active metal substrate. Control of processing conditions such as the underlying substrate metal and the film-drying environment results in an ability to tailor the internal architecture of the films as well as to functionally grade the reduction of GO. A gradient arrangement within each film, where one side is electrically conductive reduced GO (rGO) and the other side is insulating GO, was confirmed by scanning electron microscopy, Raman, X-ray diffraction, Fourier transform infrared, and X-ray photoelectron spectroscopy characterization studies. All-graphene-based freestanding films with selectively reduced GO were used in transient electronic applications such as flexible circuitry and RFID tag antennas, where their decommissioning is easily achieved by capitalizing on GO's ability to readily dissociate and create a stable suspension in water. Furthermore, the functionally graded structure was found to exhibit differential swelling behavior, and its potential applications in graphene-based actuators are outlined.
Keywords: functionally graded; graphene; graphene oxide; self-assembly; transient electronics.