Facile and Green Process to Synthesize a Three-Dimensional Network Few-Layer Graphene/Carbon Nanotube Composite for Electromagnetic Interference Shielding

We propose an environmentally friendly liquid exfoliation approach and subsequent freeze-drying process for constructing a three-dimensional (3D) carbon-based network by using few-layer graphene (FLG) and carbon nanotubes (CNTs) for electromagnetic interference (EMI) shielding applications. Systematic characterizations—such as X-ray diffraction, scanning electron microscopy, and transmission electron microscopy—as well as Raman characterization and EMI shielding tests were performed. The results indicated that the as-synthesized 3D-FLG/CNT composite obtained through the freeze-drying process exhibited excellent electromagnetic interference shielding. The shielding effect of FLG could be improved from 15 to 22 dB by introducing CNTs. The CNTs inhibited restacking of FLG in the structure. We also compared two drying processes: oven drying and freeze-drying. The freeze-drying technique markedly improved the shielding effect of FLG/CNTs from 22 to 36 dB. The composition-optimized 3D-FLG/CNT composite could be a candidate material for use in EMI shielding.