Ultra-robust, high-adhesive, self-healing, and photothermal zwitterionic hydrogels for multi-sensory applications and solar-driven evaporation.

Zwitterionic hydrogels have received considerable attention owing to their characteristic structures and integrating multifunctionality. However, the superhydrophilicity-induced poor mechanical properties severely hinder their potential applications. Besides, from the perspective of wide applications, zwitterionic hydrogels with integrated high mechanical properties, conductivity and multifunctionalities including self-adhesive, self-healing, and photothermal properties are highly desirable yet challenging. Herein, a new class of high-performance and multifunctional zwitterionic hydrogels are designed based on the incorporation of polydopamine-coated liquid metal nanoparticles (LM@PDA). Due to the efficient energy dissipation endowed by the isotropically extensible deformation of LM@PDA and the multiple interactions within the hydrogel matrix, the resultant hydrogels exhibited ultrahigh robustness with tensile strength of up to 1.3 MPa, strain of up to 1555% and toughness of up to 7.3 MJ m-3 , superior or comparable to those of most zwitterionic hydrogels. The introduced LM@PDA also endows the hydrogels with high conductivity, versatile adhesion, autonomous self-healing, excellent injectability, three-dimensional printability, degradability, and photothermal conversion performance. These preferable properties enable the hydrogels promising as wearable sensors with multiple sensory capabilities for a wide range of strain values (1-500%), pressures (0.5-200 kPa) and temperatures (20-80 °C) with an impressive temperature coefficient of resistance (up to 0.15 °C-1 ). Moreover, these hydrogels can be also applied as solar evaporators with a high water evaporation rate (up to 2.42 kg m-2 h-1 ) and solar-thermal conversion efficiency (up to 90.3%) for solar desalination and wastewater purification. The present work can pave the way for the future development of zwitterionic hydrogels and beyond.