Synergistically engineered PVDF/CNT/GnP hierarchical nanocomposites via scalable solution spinning for ultradurable, superhydrophobic EMI shielding wearables

Abstract

The rapid proliferation of next-generation wearable electronics and mission-critical smart textile systems has intensified the demand for ultra-adaptive electromagnetic interference (EMI) shielding materials that simultaneously satisfy extreme flexibility, mechanical robustness, and industrial-scale processability. 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 nanotubes (CNTs) and graphene nanoplatelets (GnPs). The multiscale architecture design ingeniously leverages CNT's 1D ballistic electron highways and GnP's 2D charge polarization interfaces, establishing dual-phase electromagnetic synergy through 3D percolated conductive networks and oriented heterointerfaces enabling multi-scale EMW scattering. Remarkably, the optimized PVDF/CNT/GnP ternary composite achieves an EMI shielding effectiveness (SE) of 23.4 dB in the X-band (18–26.5 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 CNTs and GnPs, 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. This solvent-free nanomanufacturing paradigm provides a scalable pathway toward high-throughput production of environmentally stable smart textiles, circumventing traditional vacuum-deposition and high-temperature sintering constraints.