Synergistically Engineered PVDF/CNT/GnP Hierarchical Nanocomposites via Scalable Solution Spinning for Ultradurable, Superhydrophobic EMI Shielding Wearables

Abstract

The rapid proliferation of wearable electronics and smart textile systems has intensified the demand for high-performance electromagnetic interference (EMI) shielding materials that combine exceptional flexibility, durability, and scalable manufacturability. Despite recent advances, conventional wearable EMI shielding fabrics still suffer from critical limitations, including moderate shielding efficiency (<20 dB), intricate fabrication protocols, and compromised mechanical stability under prolonged environmental exposure. To address these challenges, we propose a facile and scalable solution spinning strategy to fabricate lightweight polyvinylidene fluoride (PVDF)-based nanocomposites synergistically reinforced with carbon nanotube (CNT) and graphene nanoplatelet (GnP). The hierarchical architecture of these composites capitalizes on the complementary advantages of CNT and GnP: The three-dimensional conductive network formed by CNT ensures efficient electron transport, while the two-dimensional GnP with ultrahigh aspect ratio enhances interfacial polarization and provide exceptional electromagnetic wave (EMW) attenuation through multiple- reflection mechanisms. Remarkably, the optimized PVDF/CNT/GnP ternary composite achieves an EMI shielding effectiveness (SE) of 23.4 dB in the X-band (8.2-12.4 GHz), outperforming its binary counterparts (PVDF/CNT: 21.1 dB; PVDF/GnP: 22.3 dB) and surpassing many conventional metal-based shielding materials. This enhancement is attributed to the synergistic interplay between CNT and GnP, which establishes a percolated conductive pathway while optimizing impedance matching characteristics. Furthermore, the composites exhibit exceptional hydrophobicity (water contact angle >135°) and retain over 95% of initial EMI SE after 500 bending cycles or 240-hour humidity exposure, demonstrating unparalleled environmental stability for practical wearable applications. The proposed solution-processable methodology, requiring neither toxic solvents nor energy-intensive processes, enables environmental stability for wearable applications.