Ultra-Stretchable, Adhesive, Conductive, and Antifreezing Multinetwork Borate Ester-Based Hydrogel for Wearable Strain Sensor and VOC Absorption

Abstract

Hydrogels based on borate ester bonds exhibit remarkable tensile strength and self-healing ability, which make them a promising material for various biological research and strain sensor applications. However, in order to meet the practical application of hydrogel strain sensors, they must also show high conductivity, frost resistance, and proper adhesion, which is still a continuous challenge. Herein, a triple network hydrogel was prepared using poly(vinyl alcohol) (PVA) as the first network, ethylene imine polymer (PEI) as the second network, and poly(acrylamide-co-acrylic acid) copolymer (denoted as P(AM-Co-AA)) as the third network. 3-Carboxy-4-fluorophenylboronic acid (CFBS) was used as the cross-linking agent, glycerol (GL) was added to improve low-temperature resistance, and sodium chloride (NaCl) was incorporated to enhance electrical conductivity. The resulting PVA-CFBS@PEI@P(AM-Co-AA) triple network hydrogel exhibited impressive mechanical properties, including ultra tensile strength (4100%, 266.8 kPa), high toughness (6.5 MJ/m³), and low-temperature resistance (-60 °C). Additionally, it demonstrated high conductivity (σ = 1.83 mS/cm). The incorporation of CFBS endowed the hydrogel with excellent self-healing ability, while GL improved low-temperature resistance and strain sensing sensitivity (gauge factor (GF) = 2.8 (0-300%), GF = 5.6 (300-600%), GF = 8.7 (600-1000%)). The prepared hydrogel sensor can repetitively detect and differentiate between a wide range of human activities such as joint movements, frowning, and smiling. Additionally, the hydrogel demonstrated favorable mechanical properties at -20 °C (good adhesion, tensile strength: 1169.8%, 1.2 MPa; conductivity: 0.71 mS/cm, and strain sensing coefficient: GF = 1.3), making it suitable for applications in low-temperature environments. Furthermore, it also functions as an exceptional adsorbent, capable of selectively absorbing volatile organic compounds at high capacity (e.g., methanol: 1.80 g/g; acetone: 1.50 g/g).