Paper-like N-doped graphene films prepared by hydroxylamine diffusion induced assembly and their ultrahigh-rate capacitive properties

An approach as “hydroxylamine diffusion induced assembly” has been developed to fabricate N-doped graphene paper-like films (NG-P) and composite films containing multiwalled carbon nanotubes (NG-MWCNT-P). The obtained films have been characterized by using X-ray photoelectron spectroscopy, X-ray diffraction spectroscopy and scanning electron microscopy. The results indicate that the N atoms have doped into the graphene sheets and the interplanar distance between the graphene sheets decreases with the increment of the thermally treated temperature. The films of NG-P prepared at 100 °C are flexible and exhibit a maximum tensile stress of about 70.5 MPa and a Young's modulus of about 17.7 GPa, and the films of NG-P thermally treated at 300 °C (NG-P300) have high thermal conductivity of about 3403 W m-1 K−1. However, the NG-MWCNT-P film exhibits a relatively weaker tensile stress compared with NG-P. The electrochemical measurements show that the NG-P300 possesses excellent ultrahigh-rate capacitive properties, and that the specific capacitance and the impedance phase angle of the capacitor can reach to about 318 μF cm−2 and -77.1° respectively at frequency of 120 Hz. Simple measurements on NG-MWCNT-P show that it has specific capacitance of about 90 F g−1 based on one electrode and the capacitor possesses the high-rate capability.