Abstract
Water scarcity is a pressing global issue, requiring innovative solutions such as atmospheric water harvesting (AWH), which captures moisture from the air to provide potable water to many water-stressed areas. Thermoresponsive hydrogels, a class of temperature-sensitive polymers, demonstrate potential for AWH as matrices for hygroscopic components like salts predominantly due to their relatively energy-efficient desorption properties compared to other sorbents. However, challenges such as limited swelling capacity due to the salting-out effect and difficulty in more complete water release hinder the effectiveness of conventional hydrogel sorbents. To overcome these limitations, we introduce molecularly confined hydration in thermoresponsive hydrogels by employing a bifunctional polymeric network composed of hygroscopic zwitterionic moieties and thermoresponsive moieties. Here, we show that this approach ensures stable water uptake, enables water release at relatively low temperatures, and exhibits rapid sorption-desorption kinetics. Furthermore, by incorporating photothermal absorbers, the sorbent can achieve solar-driven AWH with comparable water release performance. This work advances the design of AWH sorbents by introducing molecularly confined hydration in thermoresponsive hydrogels, leading to a more efficient and sustainable approach to water harvesting. Our findings offer a potential solution for advanced sorbent design with comprehensive performance to mitigate the freshwater crisis.