A PVDF/MWCNTs/GO@MWCNTs/AgNWs bilayer structured composite film with ultra‐high EMI shielding and conductivity performance

Abstract Electromagnetic interference (EMI) shielding materials with easy processing, high electrical conductivity, and excellent absorption loss are urgently needed in aerospace, military stealth and portable electronic devices. In this study, a polyvinylidene fluoride/multi‐walled carbon nanotubes (PVDF/MWCNTs)‐3 wt% composite film prepared by simple solution mixing and polyethylene terephthalate (PET) nonwoven scraping method was used as the substrate, and the PVDF/MWCNTs/graphene oxide@multi‐walled carbon nanotubes (PVDF/MWCNTs/GO@MWCNTs) and PVDF/MWCNTs/GO@MWCNTs/silver nanowires (PVDF/MWCNTs/GO@MWCNTs/AgNWs) bilayer composite films were prepared by vacuum‐assisted filtration (VAF). When the amount of GO@MWCNTs was 20 mL, the conductivity of PVDF/MWCNTs/GO@MWCNTs film is 3.5 × 101 S m −1 , the total EMI shielding effectiveness (EMI SE T ) was 15.5 dB and the EMI absorption efficiency (EMI SE A ) was 10.7 dB, the specific EMI SE (SSE/T) was 539.5 dB/ dB/(cm −2 g). When the amount of AgNWs was 25 mL, the conductivity of PVDF/MWCNTs/GO@MWCNTs/AgNWs film with 0.47 mm thickness was 1.6 × 10 4 S m −1 , the EMI SE T was 69.1 dB, the EMI SE A was 61.1 dB, and the SSE/T was 2320.0 dB cm 2 g −1 . The results show that the absorption was played a dominant role in the EMI shielding mechanism of obtained films. The addition of GO@MWCNTs/AgNWs increases the electrical conductivity and EMI shielding performance of the film more than the addition of GO@MWCNTs. This is mainly because GO， MWCNTs and AgNWs formed a novel three‐dimensional conductive network structure inside the composite film due to their hydrogen bonding and van der Waals forces, which increases the carrier channels and promotes the interaction between the internal microcurrents and the electromagnetic waves, achieving the purpose of attenuating the electromagnetic waves. The obtained PVDF/MWCNTs/GO@MWCNTs/AgNWs film has good potential in EMI shielding in aerospace, military and electronic intelligence applications. Highlights Well‐dispersed and highly conductive GO@MWCNTs were prepared by hydrothermal synthesis. AgNWs with good conductivity and high aspect ratio were prepared. PVDF‐based bilayer composite films with novel 3D conductive network were prepared. The synergistic EMI shielding mechanism of the film is discussed.