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Thermoresponsive hydrogels have been studied intensively for creating smartdrug carriers and controlled drug delivery. Understanding the drug releasekinetics and corresponding transport mechanisms of nanoparticles (NPs) in athermoresponsive hydrogel network is the key to the successful design of asmart drug delivery system. We construct a mesoscopic model of rigid NPsentrapped in a hydrogel network in an aqueous solution, where the hydrogelnetwork is formed by cross-linked semiflexible polymers of PNIPAM. By varyingthe environmental temperature crossing the lower critical solution temperatureof PNIPAM we can significantly change the hydrogel network characteristics. Wesystematically investigate how the matrix porosity and the nanoparticle sizeaffect the NPs' transport kinetics at different temperatures. Quantitativeresults on the mean-squared displacement and the van Hove displacementdistributions of NPs show that all NPs entrapped in the smart hydrogels undergosubdiffusion at both low and high temperatures. For a coil state, thesubdiffusive exponent and the diffusion coefficient of NPs increase due to theincreased kinetic energy and the decreased confinement on NPs, while thetransport of NPs in the hydrogels can be also enhanced by decreasing the matrixporosity and NPs' size. However, when the solution temperature is increasedabove the critical temperature, the hydrogel network collapses following thecoil-to-globule transition, with the NPs tightly trapped in some local regionsinside the hydrogels. Consequently, the NP diffusion coefficient can be reducedby two orders of magnitude, or the diffusion processes can even be completelystopped. These findings provide new insights for designing controlled drugrelease from stimuli-responsive hydrogels, including autonomously switch on/offdrug release to respond to the changes of the local environment.

Controlled release of entrapped nanoparticles from thermoresponsive hydrogels with tunable network characteristics