Fluffy and Ordered Graphene Multilayer Films with Improved Electromagnetic Interference Shielding over X-Band

Highly ordered nitrogen-doped graphene multilayer films with large interlayer void are successfully fabricated by thermal annealing of the compact stacking graphene oxide/copper phthalocyanine (GO/CuPc) multilayer films. Scanning electron microscopic (SEM), X-ray diffraction (XRD), Raman, X-ray photoelectron spectroscopic (XPS), and electrical conductivity measurements indicate that the breakaway of oxygen functional groups on/in the GO sheets at high temperature and the in situ pyrolysis of CuPc molecules in the interlayer of graphene sheets synergistically facilitate the restoration of GO in graphitization, the effective nitrogen doping by replacing carbon atoms in graphene frameworks, the retention of layer-by-layer stacking structure of graphene sheets in plane, and the formation of interlayer voids, leading to the enhancement in the electrical conductivity (3.64 × 10 3 S/m). In addition, due to the formation of a Fabry–Pérot resonance cavity in the unique layer-by-layer stacking structure with larger interlayer voids, constructive interference of internal reflections aligned between parallel reflecting planes endows the fluffy graphene multilayer films with excellent electromagnetic interference (EMI) shielding effectiveness (exceeds 25 dB in all X-bands). The optimal shielding effectiveness is up to 55.2 dB with a smaller thickness of 0.47 mm, which makes it possible to become a practical EMI shielding material with a distinct competitive advantage.