Conducting polymer hydrogels have been considered as promising materials for flexible sensors. The integrated performances of ultrasoftness, high deformation, mechanical robustness, conformal adhesion, and high sensitivity are of great importance for their applications in wearable sensors but still remains challenging. Herein, a highly deformable conducting polymer hydrogel with ultrasoftness, tear resistance, and self-adhesiveness is fabricated by incorporating poly(3, 4-ethylenedioxythiophene):poly(styrene sulfonic acid) (PEDOT:PSS) and silk sericin (SS) into a covalently cross-linked polyacrylamide (PAM) network. Owing to abundant noncovalent interactions among the folded SS chains, PAM chains, and PEDOT:PSS, the obtained hydrogel shows a low modulus (10.3 kPa), ultrastretchability (>2000%), particularly large biaxial strain (an areal strain of 1700%), high toughness (tearing energy of 2.5 kJ/m2), and good conformal adhesion. As a result, this hydrogel demonstrates superior strain-sensitivity (gauge factor = 13.8) in a broad strain range (2000%) and excellent sensing reproducibility. The hydrogel-based wearable sensor can be used for accurately monitoring large and tiny human movements in real time and serves as bioelectrodes for precise gathering of electrocardiography and electromyography signals, showing great potential for applications in flexible sensing devices.
Bingsen Wang,Fagui Dong,Xisheng Sun,Yanan Bu,Haonan Wang,Dawei Tang,Lin Li
Achieving stable bioelectronic interfaces is hindered by inherent mechanical–electrochemical mismatches, limiting long-term device functionality in dynamic tissues. Current hydrogel-based bio-ionotronic devices face a fundamental trade-off: soft hydrogels lack sufficient ionic carriers, while ionic hydrogels compromise softness due to high cross-linking density. Here, we developed a biphasic ionic hydrogel (BIH) by integrating microgel-rich ionic reservoirs (microgel phase) into a continuous hydrogel matrix (CH phase) via hydrogen bonds. The microgel phase and CH phase of BIH work synergistically, reducing cross-linking density while maintaining the ion monomer content of the hydrogel. This synergistic structure decouples ionic storage from mechanical compliance, enabling ultrasoftness (2 kPa) and high ionic conductivity (8.55 S m–1), surpassing conventional ionic hydrogels. By tuning the microgel content, we increased the polymer network’s characteristic length, facilitating ion diffusion while maintaining structural integrity and reducing interfacial impedance. Demonstrations in real-time electromyography and mechanical motion sensing validated its potential for soft bioelectronics.