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Droplet absorption and spreading into thin layers of polymer hydrogels

Published online by Cambridge University Press:  25 October 2023

Merlin A. Etzold*
Affiliation:
The Defence Science and Technology Laboratory, Porton Down, Salisbury, Wiltshire SP4 0JQ, UK Department of Applied Mathematics and Theoretical Physics, Centre for Mathematical Sciences, University of Cambridge, Wilberforce Road, Cambridge CB3 0WA, UK
George T. Fortune
Affiliation:
Department of Applied Mathematics and Theoretical Physics, Centre for Mathematical Sciences, University of Cambridge, Wilberforce Road, Cambridge CB3 0WA, UK
Julien R. Landel
Affiliation:
Department of Mathematics, University of Manchester, Alan Turing Building, Oxford Road, Manchester M13 9PL, UK
Stuart B. Dalziel
Affiliation:
Department of Applied Mathematics and Theoretical Physics, Centre for Mathematical Sciences, University of Cambridge, Wilberforce Road, Cambridge CB3 0WA, UK
*
Email address for correspondence: metzold@dstl.gov.uk

Abstract

From biological tissues to microactuators and absorption of solvents into layers of paint, macroscopically non-porous materials with the capacity to swell when in contact with a solvent are ubiquitous. In these systems, owing to strong solid–fluid interactions, chemically driven flows can yield large geometric changes. We study experimentally and theoretically the canonical problem of the swelling of a thin hydrogel layer by a single water drop. Using a bespoke experimental set-up, we observe fast absorption leading to a radially spreading axisymmetric blister. We use a fully three-dimensional linear poroelastic framework with nonlinear kinematic equations to obtain governing equations, which we then reduce with thin-layer scalings to a one-dimensional nonlinear diffusion equation for the evolution of the blister geometry. In the limits of large and small deformations, the evolution of the blister characteristic height and radius are self-similar, following power laws in time. Our experimental measurements show that the evolution of the blister is broadly within the theoretical predictions in the large and small deformation regimes. In the general intermediate deformation regime, the measurements are well captured by our reduced one-dimensional diffusion model, which does not require the sophisticated and computationally expensive numerical approaches necessary for the original two-dimensional nonlinear coupled transport problem. By adapting modelling techniques from the fluid dynamics of thin porous elastic layers to a polymer swelling problem, our modelling framework extends the range of polymer swelling problems that can be treated with semi-analytical methods. Moreover, our detailed experimental data can serve as a test case for future nonlinear poroelastic frameworks of swelling polymer materials.

Information

Type
JFM Papers
Creative Commons
Creative Common License - CCCreative Common License - BY
This is an Open Access article, distributed under the terms of the Creative Commons Attribution licence (http://creativecommons.org/licenses/by/4.0), which permits unrestricted re-use, distribution and reproduction, provided the original article is properly cited.
Copyright
© The Author(s), 2023. Published by Cambridge University Press.
Figure 0

Figure 1. Laboratory experiments investigating the absorption and subsequent spreading of water into a hydrogel sheet. (a) Photograph of the preliminary experimental set-up without oil in a cell sealed from the atmosphere with an evaporation barrier. (b) Photograph of the full experimental set-up with an oil bath. In both cases, the side view camera is positioned outside the region of the apparatus captured by the photograph, pointing in the direction given by the red arrow with label camera. (c) Schematic of the experimental apparatus.

Figure 1

Figure 2. Sequence of photographs showing the absorption of a $100\,{\mathrm {\mu }}{\rm l}$ droplet into the hydrogel sheet.(ad) States with liquid water remaining. (ef) A surface instability forms. ( fh) Transition towards the long-time spreading regime which is shown in (hl). The visible hydrogel sheet is marked blue in (a). From (c) onward a red line marks the hydrogel–oil interface.

Figure 2

Figure 3. Raw data with corresponding error bars showing for a range of experiments how the swollen region radius varies as a function of time. Darker blue curves denote experiments with larger water droplets (see text for drop volumes). Error bars are generated through an uncertainty analysis that is described in § 2.4 and Appendix A.

Figure 3

Figure 4. Schematic of a hydrogel sheet. An axisymmetric blister of thickness $h(r,t)$ and characteristic radius $R(t)$ spreads out on the surface of a hydrogel sheet of undeformed thickness $a$, fixed to a rigid horizontal boundary at $z = 0$. The red dashed line highlights how $R(t)$ is calculated from experimental or numerical profile data using (2.2) or (4.33), respectively. Inset: the hydrogel is a solution of polymer (volume fraction $\phi _p$) and water (volume fraction $\phi _f = 1 - \phi _p$). The pore-averaged velocities of the solid and fluid phases are denoted by $\boldsymbol {u_p} = (u_p, w_p)$ and $\boldsymbol {u_f} = (u_f, w_f)$ respectively.

Figure 4

Figure 5. Swelling dynamics of thin hydrogel sheets according to the proposed poroelastic model for(a) $\beta =3/2>1$ and (b) $\beta = 2/3<1$; for both figures $\mathcal {V}=1-\mathcal {A}$ and $\mathcal {A} \in [0.001,0.01,0.1,0.5,0.9]$ (light blue to dark blue), namely darker shades of blue denote larger $\mathcal {A}$. Dotted lines with circles plot the scaled blister radius $R^{*} = R(t)/R(0)$ of numerical solutions of (4.13) as a function of time, starting from a self-similar initial height profile of the form given in (4.29). For comparison, solid lines show the radius predicted by the self-similar solution in the large deformation limit (see (4.30)).

Figure 5

Table 1. Experimental $t_s$ from which the initial condition for the numerical solution was obtained with corresponding values $\{ H_0, R_0, \mathcal {A}, t_0 \}$. The second column refers to the frame number in the corresponding attached raw dataset.

Figure 6

Figure 6. The experimental temporal evolution of (a) the scaled maximum blister height $\max (h^{*})$ and (b) the characteristic blister radius $R^{*}$ formed by a $50\,{\mathrm {\mu }}{\rm l}$ droplet (dots) superimposed onto a set of blue lines computed using the theoretical model (4.13), using the initial experimental height profile as the initial condition, where $\beta \in \{ 2/3,1,4/3,11/6,25/12,9/4,5/2,3 \}$. Curves in a darker shade of blue correspond to larger values of $\beta$. The dimensionless time scale $t^{*}$ was matched to real time $t$ using the relation $\varOmega = 6.72\times 10^{9}\,{\rm s}\,{\rm m}^{-2}$ obtained as best fit for $\beta =2.25$ (thicker blue line). Error bars are generated through an uncertainty analysis that is described in § 2.4 and Appendix A.

Figure 7

Figure 7. The temporal evolution of the maximum scaled height $\max (h^{*})$. Inset: comparison of experimental profiles (dots), at the times indicated by the red stars, with numerical profiles (solid lines). Error bars represent uncertainties. Curves in lighter shades of blue correspond to larger initial droplet volumes. Numerical solutions are generated using initial conditions taken directly from the experimental data that they are fitted against. Error bars are generated through an uncertainty analysis that is described in § 2.4 and Appendix A.

Figure 8

Figure 8. The temporal evolution of the scaled radius $R^{*}$ of the swelling region for a range of different initial droplet volumes, plotting experimental data with dots and numerical solutions with lines. Error bars represent uncertainties in the experimental data. Curves in lighter shades of blue correspond to larger initial droplet volumes, with the same volume/colour combinations as in figure 7. Numerical solutions are generated using initial conditions taken directly from the experimental data that they are fitted against once the crumpling instability has decayed. Red dots indicate the strongest deviations between numerics and experiment at late times. Error bars are generated through an uncertainty analysis that is described in § 2.4 and Appendix A.

Figure 9

Figure 9. Comparison between experimentally observed swelling and numerical solutions of the poroelastic model, plotting the spatial dependence of the scaled height $h^{*}$ for a blister formed by a $50\,{\mathrm {\mu }}{\rm l}$ droplet at different times during the experiment. Here, experimental data are denoted by circles while numerical solutions are denoted by lines. The lightest blue curve corresponds to $t - t_s = 2\,{\rm min}$ with each subsequent darker blue curve twice the previous time. Curves in darker shades of blue denote later times. Numerical solutions are generated using initial conditions taken directly from the experimental data that they are fitted against. Error bars are generated through an uncertainty analysis that is described in § 2.4 and Appendix A.

Figure 10

Figure 10. Illustration of the uncertainties inherent in the imaging. (a) Side view of the experimental configuration, showing how a misalignment (exaggerated for clarity) causes part of the droplet to be hidden from the camera by the edge of the hydrogel sheet. (b) Image (linear projection) of the droplet on the hydrogel sheet as seen by the camera. Dashed lines are not visible for the camera and give rise to an uncertainty in the position of the hydrogel surface $\delta a$, that creates a corresponding uncertainty $\delta R$ in the determination of $R$. The uncertainty due to finite pixel resolution in the radial and vertical directions are defined as $\delta r$ and $\delta z$, respectively.

Figure 11

Figure 11. Absorption of a dyed (0.01 % by weight methylene blue) droplet (100–200 ${\mathrm {\mu }}{\rm l}$) observed in plan view against a bright background. (a) Immediately after droplet placement the only visible structure is a pattern arising from gauze that was embedded within the hydrogel during the manufacturing process. (be) As the water droplet is absorbed into the hydrogel, a surface instability emerges, growing coarser as time progresses. ( f) The instability has fully decayed as the droplet and hydrogel have dried out. Panels show (a) 0 s, (b) 13 s, (c) 87 s, (d) 493 s, (e) 1037 s, ( f) 2083 s.

Figure 12

Figure 12. Raw data with corresponding error bars showing for a range of experiments how the apparent volume of the blister (found by direct integration) varies as a function of time. Darker blue curves denote experiments with larger water droplets and black dotted lines indicate the nominal droplet volume. Error bars are generated through an uncertainty analysis that is described in § 2.4 and Appendix A.