A hyperelastic theory for nonlinear hydrogel diffusiophoresis

TL;DR

This paper develops a nonlinear poroelastic theory to describe large, fast deformations in hydrogels caused by solute gradients, with potential applications in soft robotics and drug delivery.

Contribution

It introduces a nonlinear theoretical framework for hydrogel diffusiophoresis, including models for external and internally generated solute gradients, extending previous linear models.

Findings

Deformations can be stored while the stimulus gradient persists.

Varying stimulus concentration increases strain rate up to four times.

Changing solute particle size up to 25 times and flow up to 40 times significantly boosts deformation.

Abstract

Hydrogel diffusiophoresis is the deformation of a hydrogel due to a solute gradient that leads to a gradient of pairwise interactions between the solute particles and the hydrogel polymers to trigger osmotic flux. Unlike typical osmosis, it occurs without any interface selectivity of the gel to the solute and can overcome the diffusive swelling without any structural modifications to the gel. We have recently shown this effect for linear deformations of a chemically responsive polyacrylic acid (PAA) hydrogel that releases ions upon arrival of a stimulus (acid), thus internally generating the solute gradient required for diffusiophoresis [Phys. Rev. Lett. 132, 208201 (2024)]. Here we develop a nonlinear poroelastic theory for large diffusiophoretic gel strains in two models: Model I considers deformations of a generic gel when an external solute gradient is imposed. In Model II, the gel generates the solute gradient internally, motivated by the coupled PAA gel, solute (copper), and stimulus (acid) system. In Model II, we investigate the nonlinear deformations for high stimulus concentrations or by changing the solute particle size to boost steric polymer-solute interactions, as well as under a stimulus flow through the gel driven by a pressure drop across the domain. Model I indicates that deformations can be stored while the stimulus gradient persists. Compared to the experimental strain rates in Katke [Phys. Rev. Lett. 132, 208201 (2024)], Model II demonstrates that varying the stimulus concentration can increase the strain rate up to four times, changing the solute particle size up to $\sim 25$ times, and imposed flow up to $\sim 40$ times. Our theory couples nonlinear poroelasticity, polymer-solute interactions, and reaction-transport dynamics to predict large and fast diffusiophoretic gel deformations, which may find applications in hydrogel-based soft robotics and drug delivery.