Thermoresponsive Water Transportation in Dually Electrostatically Crosslinked Nanocomposite Hydrogels.

Controlling water transportation within hydrogels makes hydrogels attractive for diverse applications, but it is still a very challenging task. Herein, a novel type of dually electrostatically crosslinked nanocomposite hydrogel showing thermoresponsive water absorption, distribution, and dehydration processes are developed. The nanocomposite hydrogels are stabilized via electrostatic interactions between negatively charged poly(acrylic acid) and positively charged layered double hydroxide (LDH) nanosheets as well as poly(3-acrylamidopropyltrimethylammonium chloride). Both LDH nanosheets as crosslinkers and the surrounding temperatures played pivotal roles in tuning the water transportation within these nanocomposite hydrogels. By changing the surrounding temperature from 60 to 4 °C, these hydrogels showed widely adjustable swelling times between 2 and 45 days, while the dehydration process lasted between 7 and 27 days. A swift temperature decrease, for example, from 60 to 25 °C, generated supersaturation within these nanocomposite hydrogels, which further retarded the water transportation and distribution in hydrogel networks. Benefiting from modified water transportation and rapidly alternating water uptake capability during temperature change, pre-loaded compounds can be used to track and visualize these processes within nanocomposite hydrogels. At the same time, the discharge of water and loaded compounds from the interior of hydrogels demonstrates a thermoresponsive sustained release process.