Capillary Force-Induced Graphene Spontaneous Transfer and Encapsulation of Silver Nanowires for Highly-Stable Transparent Electrodes

Silver nanowires (NWs) (AgNWs) have emerged as the most promising conductive materials in flexible optoelectronic devices owing to their excellent photoelectric properties and mechanical flexibility. It is widely acknowledged that the practical application of AgNW networks faces challenges, such as high surface roughness, poor substrate adhesion, and limited stability. Encapsulating AgNW networks with graphene has been recognized as a viable strategy to tackle these issues. However, conventional methods like self-assembly reduction-oxidation or chemical vapor deposition often yield graphene protective layers with inherent defects. Here, we propose a novel one-step hot-pressing method containing ethanol solution that combines the spontaneous transfer and encapsulation process of rGO films onto the surface of the AgNWs network, enabling the preparation of flexible rGO/AgNWs/PET (reduced graphene oxide/silver NWs/polyethylene terephthalate) electrodes. The composite electrode exhibits outstanding photoelectric properties (T ≈ 88%, R ≈ 6 Ω sq-1) and possesses a smooth surface, primarily attributed to the capillary force generated by ethanol evaporation, ensuring the integrity of the rGO delamination process on the original substrate. The capillary force simultaneously promotes the tight encapsulation of rGO and AgNWs, as well as the welding of the AgNWs junction, thereby enhancing the mechanical stability (20,000 bending cycles and 100 cycles of taping tests), thermal stability (∼30 °C and ∼25% humidity for 150 days), and environmental adaptability (100 days of chemical attack) of the electrode. The electrode's practical feasibility has been validated by its exceptional flexibility and cycle stability (95 and 98% retention after 5000 bending cycles and 12,000 s long-term cycles) in flexible electrochromic devices.