Metal Ion-Induced Rapid Gelation of PEDOT:PSS Fibers for Synergistic Optimization of Thermoelectric and Mechanical Performance.

Abstract

Conductive polymer thermoelectric fibers, featuring inherent flexibility and weavability, hold great promise for wearable generation in smart clothing. However, balancing their thermoelectric and mechanical properties remains a critical challenge, restricting operational stability under mechanical deformation in wearable scenarios. Herein, we propose a novel wet-spinning strategy involving Ca²⁺-induced rapid gelation to fabricate high-performance PEDOT:PSS thermoelectric fibers. Ca²⁺-induced structural regulation optimized carrier transport, elevating the otherwise low Seebeck coefficient of PEDOT:PSS to 47.82 ± 1.04 μV·K^-1 while retaining high electrical conductivity of 197.71 ± 7.83 S·cm^-1. More importantly, Ca²⁺ can electrostatically anchor polymer chains, increasing cross-linking to form a tough network structure that improves both mechanical strength (140.37 ± 3.82 MPa) and fracture strain (29.14 ± 0.68%). The optimized fibers achieved synergistic thermoelectric-mechanical properties and a 0.05 K high temperature sensitivity. Integrated into smart gloves, these fibers enable temperature monitoring and heat-prevention warning, demonstrating significant potential for safeguarding the health and safety of disabled persons.