Abstract
Polymer–nanoparticle hydrogels are a unique class of self‐assembled, shear‐thinning, yield‐stress fluids that have demonstrated potential utility in many impactful applications. Here, we present a thorough analysis of the gelation and yielding behavior of these materials with respect to the polymer and nanoparticle component stoichiometry. Through comprehensive rheological and diffusion studies, we reveal insights into the structural dynamics of the polymer nanoparticle network that identify that stoichiometry plays a key role in gelation and yielding, ultimately enabling the development of hydrogel formulations with unique shear‐thinning and yield‐stress behaviors. Access to these materials opens new doors for interesting applications in a variety of fields including tissue engineering, drug delivery, and controlled solution viscosity.
Highlights
Shear-thinning hydrogels are unique and promising tools for controlling the delivery of therapeutics and cells, controlling solution viscosity, and 3D printing[1]
The polymers are theorized to form a dynamic corona around the nanoparticles bridging between nanoparticles[2,18]
We utilized a consistent level of dodecyl modification and concentrated our efforts on understanding the effects of P-NP stoichiometry on gelation, viscoelasticity, and flow properties
Summary
Shear-thinning hydrogels are unique and promising tools for controlling the delivery of therapeutics and cells, controlling solution viscosity, and 3D printing[1]. While recent research has revealed many of the driving factors for the dynamic mechanical properties and temperature responsiveness of materials comprising mixtures of interacting polymers and nanoparticles, many of which have focused on polymeric melt systems, the exact interaction mechanisms which dominate gelation (e.g., bridging of polymers between particles or jamming of polymer-coated particles) under various formulation conditions are still poorly understood[18,19,20] For this reason, we sought to design and execute a series of rheology and diffusion studies to elucidate the dominant mechanisms occurring in gelation of the PNP hydrogel system. We use shear rheology and diffusion studies on a wide range of PNP hydrogel formulations to reveal the compositional features yielding unique and desirable properties in these materials
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