An official website of the United States government
Hydrogels are commonly used in research and energy, manufacturing, agriculture, and biomedical applications. These uses typically require hydrogel mechanics and internal water transport, described by the poroelastic diffusion coefficient, to be characterized. Sophisticated indentation-based approaches are typically used for this purpose, but they require expensive instrumentation and are often limited to planar samples. Here, we present Sha pe Re laxation (SHARE), an alternative way to assess the poroelastic diffusion coefficient of hydrogel particles that is cost-effective, straightforward, and versatile. This approach relies on first indenting a hydrogel particle via swelling within a granular packing, and then monitoring how the indented shape of the hydrogel relaxes after it is removed from the packing. We validate this approach using experiments in packings with varying grain sizes and confining stresses; these yield measurements of the poroelastic diffusion coefficient of polyacrylamide hydrogels that are in good agreement with those previously obtained using indentation approaches. We therefore anticipate that the SHARE approach will find broad use in a range of applications of hydrogels and other swellable soft materials.
more »
« less
Under pressure: Hydrogel swelling in a granular medium
Hydrogels hold promise in agriculture as reservoirs of water in dry soil, potentially alleviating the burden of irrigation. However, confinement in soil can markedly reduce the ability of hydrogels to absorb water and swell, limiting their widespread adoption. Unfortunately, the underlying reason remains unknown. By directly visualizing the swelling of hydrogels confined in three-dimensional granular media, we demonstrate that the extent of hydrogel swelling is determined by the competition between the force exerted by the hydrogel due to osmotic swelling and the confining force transmitted by the surrounding grains. Furthermore, the medium can itself be restructured by hydrogel swelling, as set by the balance between the osmotic swelling force, the confining force, and intergrain friction. Together, our results provide quantitative principles to predict how hydrogels behave in confinement, potentially improving their use in agriculture as well as informing other applications such as oil recovery, construction, mechanobiology, and filtration.
more »
« less
- Award ID(s):
- 2011750
- PAR ID:
- 10324975
- Date Published:
- Journal Name:
- Science Advances
- Volume:
- 7
- Issue:
- 7
- ISSN:
- 2375-2548
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract Hydrogels are explored for applications in agriculture, water purification, and biomedicine, leveraging softness, elasticity, and high water uptake. However, hydrogels are notoriously brittle, especially at high water content. This shortcoming puts the improvement of hydrogel mechanics at the forefront of current research. Yet modern strategies for enhancing gel resilience come at the expense of softness and swelling. This problem is addressed using bottlebrush networks with disentangled strands and hidden length reservoirs, which synergistically enhance gel swelling and robustness while maintaining their softness. Implementing a facile one‐pot synthesis of single‐stranded bottlebrush networks with a relatively hydrophobic poly(2‐hydroxyethyl methacrylate) (PHEMA) backbone and hydrophilic poly(2‐methyl‐2‐oxazoline) (PMOx) side chains, hydrogels are prepared with a modulus below <1 kPa and swelling ratios up to 125 that can withstand up to 10‐fold extension.more » « less
-
Charged double network (DN) hydrogels are widely studied for their desirable mechanical strength and tunable properties. In this work, the influence of polymer concentration on microstructure and properties of agarose/polyacrylic acid DN hydrogels is studied. Agarose, the first network, is a brittle biopolymer, while polyacrylic acid (PAAc) is a weak polyelectrolyte. The microstructure, visualized in liquid environment, displays an agarose scaffold coated and interconnected by PAAc, deviating from the common assumption of an entangled double network. Importantly, the charging of PAAc in the hydrogel is regulated not only by the pH and weak polyelectrolyte effects, but also by the restricted swelling of the double network, and hence, it is an inherent regulation mechanism of charged hydrogels. The interactions between the hydrogel and the ionic environment induce microstructural changes and charging of the double network, impacting surface properties such as topography, stiffness, and adhesion, which are spatially resolved by liquid‐environment atomic force microscopy. The responsiveness of the DN hydrogels significantly depends on both polymer concentrations and ion concentrations. These findings provide insights into the responsive behavior of double network hydrogels and reveal universal mechanisms for charged hydrogels, which can guide the future development of functional soft materials.more » « less
-
From pasta to biological tissues to contact lenses, gel and gel-like materials inherently soften as they swell with water. In dry, low-relative-humidity environments, these materials stiffen as they de-swell with water. Here, we use semi-dilute polymer theory to develop a simple power-law relationship between hydrogel elastic modulus and swelling. From this relationship, we predict hydrogel stiffness or swelling at arbitrary relative humidities. Our close predictions of properties of hydrogels across three different polymer mesh families at varying crosslinking densities and relative humidities demonstrate the validity and generality of our understanding. This predictive capability enables more rapid material discovery and selection for hydrogel applications in varying humidity environments.more » « less
-
Poly(acrylamide- co -acrylic acid) (P(AAm- co -AA)) hydrogels are highly tunable and pH-responsive materials frequently used in biomedical applications. The swelling behavior and mechanical properties of these gels have been extensively characterized and are thought to be controlled by the protonation state of the acrylic acid (AA) through the regulation of solution pH. However, their tribological properties have been underexplored. Here, we hypothesized that electrostatics and the protonation state of AA would drive the tribological properties of these polyelectrolyte gels. P(AAm- co -AA) hydrogels were prepared with constant acrylamide (AAm) concentration (33 wt%) and varying AA concentration to control the amount of ionizable groups in the gel. The monomer:crosslinker molar ratio (200:1) was kept constant. Hydrogel swelling, stiffness, and friction behavior were studied by systematically varying the acrylic acid (AA) concentration from 0–12 wt% and controlling solution pH (0.35, 7, 13.8) and ionic strength ( I = 0 or 0.25 M). The stiffness and friction coefficient of bulk hydrogels were evaluated using a microtribometer and borosilicate glass probes as countersurfaces. The swelling behavior and elastic modulus of these polyelectrolyte hydrogels were highly sensitive to solution pH and poorly predicted the friction coefficient ( µ ), which decreased with increasing AA concentration. P(AAm- co -AA) hydrogels with the greatest AA concentrations (12 wt%) exhibited superlubricity ( µ = 0.005 ± 0.001) when swollen in unbuffered, deionized water (pH = 7, I = 0 M) and 0.5 M NaOH (pH = 13.8, I = 0.25 M) ( µ = 0.005 ± 0.002). Friction coefficients generally decreased with increasing AA and increasing solution pH. We postulate that tunable lubricity in P(AAm- co -AA) gels arises from changes in the protonation state of acrylic acid and electrostatic interactions between the probe and hydrogel surface.more » « less
- Free Publicly Accessible Full Text
-
Accepted Manuscript
- Journal Article:
- https://doi.org/10.1126/sciadv.abd2711
