Robust and self-healing flexible transparent electrodes based on nanocellulose-mediated dual-dynamic networks with...

Developing flexible transparent electrodes (FTEs) that reconcile mechanical toughness with autonomous self-healing remains a significant challenge for wearable electronics. We hypothesized that 2-amino-4-hydroxy-6-methylpyrimidine functionalized nanocellulose (UTCNF) could serve as a high-density dynamic hub within a disulfide-crosslinked matrix to reconcile this conflict. By co-integrating UTCNF and disulfide bonds into PDMS, we engineered a dual-dynamic substrate. Results validate that the synergistic quadruple hydrogen and reversible covalent bonding network effectively dissipates energy, yielding exceptional toughness (19.70 MJ/m³) and healing efficiency (91.30%). Building on this, a hybrid AgNW-MXene conductive network was constructed via interfacial anchoring and capillary-driven cold-welding. Benefiting from this architecture, the resulting FTE exhibits an outstanding comprehensive optoelectronic performance, balancing a remarkably low sheet resistance of 3.64 Ω/sq. with a high optical transmittance of 77.90%, which yields a highly competitive optoelectronic Figure of Merit (σ_dc/σ_op) of ∼390. The resulting FTE demonstrated remarkable electromechanical durability (>3000 bending cycles) and environmental resilience. Finally, integrated electroluminescent devices exhibited stable performance under extreme deformation, sub-zero temperatures (-20 °C), and underwater immersion. This study establishes a mechanistically grounded paradigm for leveraging functional carbohydrate polymers to develop durable, adaptive, and high-performance flexible electronics.