One‑step spray‑coated self-stratified PDMS/P(VDF‑TrFE) hybrid fibrous composite-based Triboelectric Nanogenerators

Abstract

Fibrous architectures have emerged as highly promising platforms for triboelectric nanogenerators (TENGs) due to their large surface area, mechanical flexibility, and enhanced mechanical-to-electrical energy conversion efficiency. However, conventional fabrication strategies for fiber-based triboelectric layers typically require high-voltage processing such as electrospinning, which limits scalable manufacturing. Here, we introduce a one-step spray-coating strategy that simultaneously induces fiber formation, hierarchical micro/nanostructuring, and spontaneous phase separation, producing self-stratified polydimethylsiloxane/poly(vinylidene fluoride-co-trifluoroethylene) [PDMS/P(VDF-TrFE)] hybrid fibrous composites without the need for high-voltage equipment. Rapid solvent evaporation drives surface energy-mediated spontaneous self-stratification, resulting in a compositionally graded architecture with a PDMS-enriched exterior and a P(VDF-TrFE)-rich interior. The resulting self-stratified hybrid fibrous networks promote β -phase crystallization within the P(VDF-TrFE)-rich interior, strengthen charge retention through the PDMS-enriched sheath, and enlarge the effective contact area, collectively leading to synergistically enhanced triboelectric performance. Consequently, the optimized material composition yields an open-circuit voltage ( V oc ) of 290 V, a short-circuit current ( I sc ) of 7.5 µA, and a maximum power density of 1.23 W m −2 . The fabricated devices maintain stable output over 30,000 mechanical cycles and demonstrate practical utility in handwritten letter recognition systems and smart door lock devices. This scalable spray-coating approach provides a simple and effective strategy for fabricating fibrous triboelectric layers with strong potential for self-powered sensing systems, human–machine interfaces, and large-area energy harvesting applications.