Cellulose-enabled dynamic crosslinking microdomains strategy inducing high strong and tough, reprocessable bio-elastomer for durable self-powered electronic textiles

Abstract

Self-powered electronic textiles undergo repeated deformation and friction, which imposes higher demands on the mechanical durability and sustainability of the dielectric polymeric substrates. However, designing the ideal polymeric substrates simultaneously possessing high strength and toughness, and excellent reprocessing performance for highly durable electronic textiles remains a rigorous challenge due to the intrinsic conflict in the mechanisms. Herein, we present a design concept that cellulose-enabled reversible chemical micro-crosslinking combination with multiple hierarchical hydrogen bonds induced dynamic crosslinking microdomains to realize the superior strength and toughness, and reprocessable bio-elastomers. The disintegration of hierarchical hydrogen bonds dissipating energy combination with the orientation arrangement of dynamic crosslinking microdomains along the stretching direction miraculously realize the superior mechanical strength (55.58 MPa) and toughness (144.25 MJ/m³). The reversible breakage and reconstruction of the dynamic crosslinking microdomains allow the bio-elastomer to be reprocessed for several cycles with extremely high mechanical strength recovery efficiency of 91.54 %. The bio-elastomers are employed as dielectric layers to laminate with the PPy-modified cotton fabric for large-scale manufacture of TENG-based electronic textiles with high stability, durability, and washability. The application scenarios are demonstrated for energy harvesting, motion monitoring, and human–computer interaction, providing a novel paradigm for environmental friendliness and durable wearable electronics.