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A special issue of Gels (ISSN 2310-2861).

Deadline for manuscript submissions: closed (31 October 2017) | Viewed by 74015

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Dr. Ferenc Horkay

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Section on Quantitative Imaging and Tissue Sciences, Eunice Kennedy Shriver National Institute of Child Health and Human Development, National Institutes of Health, Bethesda, MD 20892, USA
Special Issues, Collections and Topics in MDPI journals

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Dear Colleagues,

This Special Issue on “Polyelectrolyte Gels” is dedicated to recent developments from theoretical and fundamental aspects to the synthesis, characterization, and applications of polyelectrolyte networks and gels. Within this context, a broad range of subjects, including structure and dynamics, molecular modeling and simulation, and applications will be discussed.

Polyelectrolytes are complex polymer systems of which properties reflect chain connectivity, electrostatic effects, and other molecular interactions over multiple length scales. Owing to the complexity of the interactions, an understanding of these materials has been slow to develop despite the importance of charged polymers, both to biology and to materials science. In living systems, many biopolymers are highly-charged macromolecules. In their natural environment, they are exposed to different ions. Synthetic polyelectrolyte gels have a variety of applications in materials science and engineering, including materials for energy storage, separation, and drug delivery. Polyelectrolyte-based materials in which the constituents are organized across multiple length scales have the potential to address a wide range of technological challenges. The precise control of the molecular and supramolecular architecture enables novel applications in biomedicine. Progress in this field requires an interdisciplinary effort to accomplish a more detailed understanding of the structure and interactions that define the behavior of complex polyelectrolyte systems, and makes it possible to tailor the properties of these materials.

Since it is impossible to cover all aspects of polyelectrolyte gel science in one issue, this Special Issue will contain only a few representative examples, illustrating the complexity of the polyelectrolyte problem. It is hoped that the topics will stimulate new research and discoveries in the field of polyelectrolyte networks and gels.

Dr. Ferenc Horkay
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Gels is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2600 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

Synthetic and Biological Polyelectrolytes
Theory of Polyelectrolyte Networks and Gels
Synthesis and Characterization
Structure–Property Relationships
Dynamic Properties
Modeling
Applications

Related Special Issue

Polyelectrolyte Gels: Volume II in Gels (11 articles)

Published Papers (14 papers)

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Research

Jump to: Review

20 pages, 463 KiB

Open AccessFeature PaperArticle

Electrodiffusion-Mediated Swelling of a Two-Phase Gel Model of Gastric Mucus

by Owen L. Lewis, James P. Keener and Aaron L. Fogelson

Gels 2018, 4(3), 76; https://doi.org/10.3390/gels4030076 - 06 Sep 2018

Cited by 10 | Viewed by 3397

Abstract

Gastric mucus gel is known to exhibit dramatic and unique swelling behaviors in response to the ionic composition of the hydrating solution. This swelling behavior is important in the maintenance of the mucus layer lining the stomach wall, as the layer is constantly digested by enzymes in the lumen, and must be replenished by new mucus that swells as it is secreted from the gastric wall. One hypothesis suggests that the condensed state of mucus at secretion is maintained by transient bonds with calcium that form crosslinks. These crosslinks are lost as monovalent cations from the environment displace divalent crosslinkers, leading to a dramatic change in the energy of the gel and inducing the swelling behavior. Previous modeling work has characterized the equilibrium behavior of polyelectrolyte gels that respond to calcium crosslinking. Here, we present an investigation of the dynamic swelling behavior of a polyelectrolytic gel model of mucus. In particular, we quantified the rate at which a globule of initially crosslinked gel swells when exposed to an ionic bath. The dependence of this swelling rate on several parameters was characterized. We observed that swelling rate has a non-monotone dependence on the molarity of the bath solution, with moderate concentrations of available sodium inducing the fastest swelling. Full article

(This article belongs to the Special Issue Polyelectrolyte Gels)

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9 pages, 4068 KiB

Open AccessFeature PaperArticle

Mechanical Properties and Structures of Clay-Polyelectrolyte Blend Hydrogels

by Hiroyuki Takeno and Shiori Nagai

Gels 2018, 4(3), 71; https://doi.org/10.3390/gels4030071 - 30 Aug 2018

Cited by 8 | Viewed by 4190

Abstract

Our recent studies have shown that the hydrogels prepared by blending clay, a dispersant of clay, and a polyelectrolyte (sodium polyacrylate (PAAS)) possess excellent mechanical properties. In order to clarify the mechanism of the toughness, we have so far investigated the effects of the composition, molecular mass of the polymer, and kinds of polymers on the mechanical properties. This study has focused upon the mechanical properties and structures of the clay/PAAS gels using three kinds of smectite clay minerals such as synthetic hectorite (laponite XLG), saponite (sumecton-SA), montmorillonite (kunipia-F), whose particle size becomes larger according to the sequence. Laponite/PAAS and sumecton/PAAS gels were quite tough for high compression, whereas kunipia-F/PAAS did not gelate. In comparison between sumecton/PAAS gel and laponite/PAAS gel, the mechanical property of the former gel was poorer than that of the latter gel due to the inhomogeneous distribution of clay platelets in the gel. Synchrotron small-angle X-ray scattering experiments revealed that their clay platelets laid down in the stretching direction under elongation. Furthermore, it was found that sumecton/PAAS gel under elongation was arranged with an interparticle distance of ~6.3 nm in the direction perpendicular to the stretching. Such local ordering under elongation may originate in local aggregation of sumecton platelets in the original state without elongation. Full article

(This article belongs to the Special Issue Polyelectrolyte Gels)

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11 pages, 2989 KiB

Open AccessArticle

Fiber Network Formation in Semi-Flexible Polymer Solutions: An Exploratory Computational Study

by Fernando Vargas-Lara and Jack F. Douglas

Gels 2018, 4(2), 27; https://doi.org/10.3390/gels4020027 - 22 Mar 2018

Cited by 19 | Viewed by 3840

Abstract

The formation of gels through the bundling of semi-flexible polymer chains into fiber networks is ubiquitous in diverse manufactured and natural materials, and, accordingly, we perform exploratory molecular dynamics simulations of a coarse-grained model of semi-flexible polymers in a solution with attractive lateral interchain interactions to understand essential features of this type of gel formation. After showing that our model gives rise to fibrous gels resembling real gels of this kind, we investigate how the extent of fiber bundling influences the “melting” temperature,

T_{m}

, and the emergent rigidification of model bundled fibers having a fixed number of chains, N, within them. Based on our preliminary observations, we suggest the fiber size is kinetically selected by a reduced thermodynamic driving force and a slowing of the dynamics within the fibers associated with their progressive rigidification with the inclusion of an increasing number of chains in the bundle. Full article

(This article belongs to the Special Issue Polyelectrolyte Gels)

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16 pages, 4239 KiB

Open AccessArticle

The Influence of Polymer and Ion Solvation on the Conformational Properties of Flexible Polyelectrolytes

by Alexandros Chremos and Jack F. Douglas

Gels 2018, 4(1), 20; https://doi.org/10.3390/gels4010020 - 02 Mar 2018

Cited by 22 | Viewed by 4952

Abstract

The study of the coupling between the conformational properties of a polyelectrolyte chain and the distribution of counter-ions surrounding the chain is important in developing predictive theories for more complex polymer materials, such as polyelectrolyte gels. We investigated the influence of solvent affinity to counter-ions and the polyelectrolyte backbone on the conformational properties of highly charged flexible polymer chains using molecular dynamics simulations that include both ions and an explicit solvent. We find that the solvation of the polyelectrolyte backbone can be achieved by either increasing the solvent affinity for the polyelectrolyte segments or by increasing the solvent affinity for the counter-ions. However, these two mechanisms influence the conformational properties of the polyelectrolyte chain in rather different ways, suggesting the inadequacy of polyelectrolyte solution models that treat the solvent as a continuum medium. Full article

(This article belongs to the Special Issue Polyelectrolyte Gels)

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10 pages, 7167 KiB

Open AccessArticle

Shape-Changing Tubular Hydrogels

by Srinivasa R. Raghavan, Neville J. Fernandes and Bani H. Cipriano

Gels 2018, 4(1), 18; https://doi.org/10.3390/gels4010018 - 22 Feb 2018

Cited by 6 | Viewed by 5668

Abstract

We describe the creation of hollow tubular hydrogels in which different zones along the length of the tube are composed of different gels. Our method to create these gels is adapted from a technique developed previously in our lab for creating solid hybrid hydrogels. The zones of our tubular gel are covalently bonded at the interfaces; as a result, these interfaces are highly robust. Consequently, the tube can be picked up, manipulated and stretched without suffering any damage. The hollow nature of these gels allows them to respond 2–30-fold faster to external stimuli compared to a solid gel of identical composition. We study the case where one zone of the hybrid tube is responsive to pH (due to the incorporation of an ionic monomer) while the other zones are not. Initially, the entire tube has the same diameter, but when pH is changed, the diameter of the pH-responsive zone alone increases (i.e., this zone bulges outward) while the other zones maintain their original diameter. The net result is a drastic change in the shape of the gel, and this can be reversed by reverting the pH to its original value. Similar localized changes in gel shape are shown for two other stimuli: temperature and solvent composition. Our study points the way for researchers to design three-dimensional soft objects that can reversibly change their shape in response to stimuli. Full article

(This article belongs to the Special Issue Polyelectrolyte Gels)

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8 pages, 6854 KiB

Open AccessArticle

Crystal Crosslinked Gels for the Deposition of Inorganic Salts with Polyhedral Shapes

by Yumi Mochizuki, Chihiro Oka, Takumi Ishiwata, Kenta Kokado and Kazuki Sada

Gels 2018, 4(1), 16; https://doi.org/10.3390/gels4010016 - 06 Feb 2018

Cited by 2 | Viewed by 3561

Abstract

Biomineralization has been given a great deal of attention by materials chemists because of its low environmental load and sustainability. With the goal of synthesizing such processes, various methods have been developed, especially for inorganic salts of calcium. In this report, we focused on the deposition of inorganic salts, such as calcium carbonate and calcium phosphate using crystal crosslinked gels (CCG), which are prepared by crystal crosslinking of metal-organic frameworks (MOFs). Due to the crystalline nature of MOFs, CCGs intrinsically possess polyhedral shapes derived from the original MOF crystals. As the result of deposition, the obtained inorganic salts also exhibited a polyhedral shape derived from the CCG. The deposition mainly occurred near the surface of the CCG, and the amorphous nature of the deposited inorganic salts was also confirmed. Full article

(This article belongs to the Special Issue Polyelectrolyte Gels)

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12 pages, 4558 KiB

Open AccessArticle

Relaxation Behavior by Time-Salt and Time-Temperature Superpositions of Polyelectrolyte Complexes from Coacervate to Precipitate

by Samim Ali and Vivek M. Prabhu

Gels 2018, 4(1), 11; https://doi.org/10.3390/gels4010011 - 18 Jan 2018

Cited by 54 | Viewed by 7001

Abstract

Complexation between anionic and cationic polyelectrolytes results in solid-like precipitates or liquid-like coacervate depending on the added salt in the aqueous medium. However, the boundary between these polymer-rich phases is quite broad and the associated changes in the polymer relaxation in the complexes across the transition regime are poorly understood. In this work, the relaxation dynamics of complexes across this transition is probed over a wide timescale by measuring viscoelastic spectra and zero-shear viscosities at varying temperatures and salt concentrations for two different salt types. We find that the complexes exhibit time-temperature superposition (TTS) at all salt concentrations, while the range of overlapped-frequencies for time-temperature-salt superposition (TTSS) strongly depends on the salt concentration (C_s) and gradually shifts to higher frequencies as C_s is decreased. The sticky-Rouse model describes the relaxation behavior at all C_s. However, collective relaxation of polyelectrolyte complexes gradually approaches a rubbery regime and eventually exhibits a gel-like response as C_s is decreased and limits the validity of TTSS. Full article

(This article belongs to the Special Issue Polyelectrolyte Gels)

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20 pages, 3577 KiB

Open AccessArticle

Binding of Lysozyme to Spherical Poly(styrenesulfonate) Gels

by Martin Andersson and Per Hansson

Gels 2018, 4(1), 9; https://doi.org/10.3390/gels4010009 - 16 Jan 2018

Cited by 7 | Viewed by 3355

Abstract

Polyelectrolyte gels are useful as carriers of proteins and other biomacromolecules in, e.g., drug delivery. The rational design of such systems requires knowledge about how the binding and release are affected by electrostatic and hydrophobic interactions between the components. To this end we have investigated the uptake of lysozyme by weakly crosslinked spherical poly(styrenesulfonate) (PSS) microgels and macrogels by means of micromanipulator assisted light microscopy and small angle X-ray scattering (SAXS) in an aqueous environment. The results show that the binding process is an order of magnitude slower than for cytochrome c and for lysozyme binding to sodium polyacrylate gels under the same conditions. This is attributed to the formation of very dense protein-rich shells in the outer layers of the microgels with low permeability to the protein. The shells in macrogels contain 60 wt % water and nearly charge stoichiometric amounts of lysozyme and PSS in the form of dense complexes of radius 8 nm comprising 30–60 lysozyme molecules. With support from kinetic modelling results we propose that the rate of protein binding and the relaxation rate of the microgel are controlled by the protein mass transport through the shell, which is strongly affected by hydrophobic and electrostatic interactions. The mechanism explains, in turn, an observed dependence of the diffusion rate on the apparent degree of crosslinking of the networks. Full article

(This article belongs to the Special Issue Polyelectrolyte Gels)

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14 pages, 4254 KiB

Open AccessArticle

Ionically Paired Layer-by-Layer Hydrogels: Water and Polyelectrolyte Uptake Controlled by Deposition Time

by Victor Selin, John F. Ankner and Svetlana A. Sukhishvili

Gels 2018, 4(1), 7; https://doi.org/10.3390/gels4010007 - 11 Jan 2018

Cited by 12 | Viewed by 4926

Abstract

Despite intense recent interest in weakly bound nonlinear (“exponential”) multilayers, the underlying structure-property relationships of these films are still poorly understood. This study explores the effect of time used for deposition of individual layers of nonlinearly growing layer-by-layer (LbL) films composed of poly(methacrylic acid) (PMAA) and quaternized poly-2-(dimethylamino)ethyl methacrylate (QPC) on film internal structure, swelling, and stability in salt solution, as well as the rate of penetration of invading polyelectrolyte chains. Thicknesses of dry and swollen films were measured by spectroscopic ellipsometry, film internal structure—by neutron reflectometry (NR), and degree of PMAA ionization—by Fourier-transform infrared spectroscopy (FTIR). The results suggest that longer deposition times resulted in thicker films with higher degrees of swelling (up to swelling ratio as high as 4 compared to dry film thickness) and stronger film intermixing. The stronger intermixed films were more swollen in water, exhibited lower stability in salt solutions, and supported a faster penetration rate of invading polyelectrolyte chains. These results can be useful in designing polyelectrolyte nanoassemblies for biomedical applications, such as drug delivery coatings for medical implants or tissue engineering matrices. Full article

(This article belongs to the Special Issue Polyelectrolyte Gels)

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2739 KiB

Open AccessArticle

Swelling, Mechanics, and Thermal/Chemical Stability of Hydrogels Containing Phenylboronic Acid Side Chains

by Arum Kim, Heelim Lee, Clinton F. Jones, Siddharthya K. Mujumdar, Yuandong Gu and Ronald A. Siegel

Gels 2018, 4(1), 4; https://doi.org/10.3390/gels4010004 - 29 Dec 2017

Cited by 8 | Viewed by 4620

Abstract

We report here studies of swelling, mechanics, and thermal stability of hydrogels consisting of 20 mol % methacrylamidophenylboronic acid (MPBA) and 80 mol % acrylamide (AAm), lightly crosslinked with methylenebisacrylamide (Bis). Swelling was measured in solutions of fixed ionic strength, but with varying pH values and fructose concentrations. Mechanics was studied by compression and hold. In the absence of sugar or in the presence of fructose, the modulus was mostly maintained during the hold period, while a significant stress relaxation was seen in the presence of glucose, consistent with reversible, dynamic crosslinks provided by glucose, but not fructose. Thermal stability was determined by incubating hydrogels at pH 7.4 at room temperature, and 37, 50, and 65 °C, and monitoring swelling. In PBS (phosphate buffered saline) solutions containing 9 mM fructose, swelling remained essentially complete for 50 days at room temperature, but decreased substantially with time at the higher temperatures, with accelerated reduction of swelling with increasing temperature. Controls indicated that over long time periods, both the MPBA and AAm units were experiencing conversion to different species. Full article

(This article belongs to the Special Issue Polyelectrolyte Gels)

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975 KiB

Open AccessFeature PaperArticle

Computer Simulations of Static and Dynamical Properties of Weak Polyelectrolyte Nanogels in Salty Solutions

by David Sean, Jonas Landsgesell and Christian Holm

Gels 2018, 4(1), 2; https://doi.org/10.3390/gels4010002 - 27 Dec 2017

Cited by 18 | Viewed by 4412

Abstract

We investigate the chemical equilibria of weak polyelectrolyte nanogels with reaction ensemble Monte Carlo simulations. With this method, the chemical identity of the nanogel monomers can change between neutral or charged following the acid-base equilibrium reaction HA ⇌ A⁻ + H⁺ [...] Read more.

K_{a}

. These simulations allow for the extraction of static properties like swelling equilibria and the way in which charge—both monomer and ionic—is distributed inside the nanogel. Our findings reveal that, depending on the value of

K_{a}

, added salt can either increase or decrease the gel size. Using the calculated mean-charge configurations of the nanogel from the reaction ensemble simulation as a quenched input to coupled lattice-Boltzmann molecular dynamics simulations, we investigate dynamical nanogel properties such as the electrophoretic mobility

μ

and the diffusion coefficient D. Full article

(This article belongs to the Special Issue Polyelectrolyte Gels)

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7326 KiB

Open AccessArticle

Improved Concrete Materials with Hydrogel-Based Internal Curing Agents

by Matthew J. Krafcik, Nicholas D. Macke and Kendra A. Erk

Gels 2017, 3(4), 46; https://doi.org/10.3390/gels3040046 - 25 Nov 2017

Cited by 43 | Viewed by 8452

Abstract

This research article will describe the design and use of polyelectrolyte hydrogel particles as internal curing agents in concrete and present new results on relevant hydrogel-ion interactions. When incorporated into concrete, hydrogel particles release their stored water to fuel the curing reaction, resulting in reduced volumetric shrinkage and cracking and thus increasing concrete service life. The hydrogel’s swelling performance and mechanical properties are strongly sensitive to multivalent cations that are naturally present in concrete mixtures, including calcium and aluminum. Model poly(acrylic acid(AA)-acrylamide(AM))-based hydrogel particles with different chemical compositions (AA:AM monomer ratio) were synthesized and immersed in sodium, calcium, and aluminum salt solutions. The presence of multivalent cations resulted in decreased swelling capacity and altered swelling kinetics to the point where some hydrogel compositions displayed rapid deswelling behavior and the formation of a mechanically stiff shell. Interestingly, when incorporated into mortar, hydrogel particles reduced mixture shrinkage while encouraging the formation of specific inorganic phases (calcium hydroxide and calcium silicate hydrate) within the void space previously occupied by the swollen particle. Full article

(This article belongs to the Special Issue Polyelectrolyte Gels)

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3768 KiB

Open AccessArticle

Micromechanical Characterization of Hydrogels Undergoing Swelling and Dissolution at Alkaline pH

by Wei Hu, Francois Martin, Romain Jeantet, Xiao Dong Chen and Ruben Mercadé-Prieto

Gels 2017, 3(4), 44; https://doi.org/10.3390/gels3040044 - 18 Nov 2017

Cited by 5 | Viewed by 4629

Abstract

The swelling of polyelectrolyte hydrogels usually depends on the pH, and if the pH is high enough degradation can occur. A microindentation device was developed to dynamically test these processes in whey protein isolate hydrogels at alkaline pH 7–14. At low alkaline pH the shear modulus decreases during swelling, consistent with rubber elasticity theory, yet when chemical degradation occurs at pH ≥ 11.5 the modulus decreases quickly and extensively. The apparent modulus was constant with the indentation depth when swelling predominates, but gradients were observed when fast chemical degradation occurs at 0.05–0.1 M NaOH. In addition, these profiles were constant with time when dissolution rates are also constant, the first evidence that a swollen layer with steady state mechanical properties is achieved despite extensive dissolution. At >0.5 M NaOH, we provide mechanical evidence showing that most interactions inside the gels are destroyed, gels were very weak and hardly swell, yet they still dissolve very slowly. Microindentation can provide complementary valuable information to study the degradation of hydrogels. Full article

(This article belongs to the Special Issue Polyelectrolyte Gels)

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Review

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14 pages, 1134 KiB

Open AccessReview

Weak and Strong Gels and the Emergence of the Amorphous Solid State

by Jack F. Douglas

Gels 2018, 4(1), 19; https://doi.org/10.3390/gels4010019 - 23 Feb 2018

Cited by 52 | Viewed by 9960

Abstract

Gels are amorphous solids whose macroscopic viscoelastic response derives from constraints in the material that serve to localize the constituent molecules or particles about their average positions in space. These constraints may either be local in nature, as in chemical cross-linking and direct physical associations, or non-local, as in case of topological “entanglement” interactions between highly extended fiber or sheet structures in the fluid. Either of these interactions, or both combined, can lead to “gelation” or “amorphous solidification”. While gels are often considered to be inherently non-equilibrium materials, and correspondingly termed “soft glassy matter”, this is not generally the case. For example, the formation of vulcanized rubbers by cross-linking macromolecules can be exactly described as a second order phase transition from an equilibrium fluid to an equilibrium solid state, and amorphous solidification also arises in diverse physical gels in which molecular and particle localization occurs predominantly through transient molecuar associations, or even topological interactions. As equilibrium, or near equilibrium systems, such gels can be expected to exhibit universal linear and non-linear viscoelastic properties, especially near the “critical” conditions at which the gel state first emerges. In particular, a power-law viscoelastic response is frequently observed in gel materials near their “gelation” or “amorphous solidification” transition. Another basic property of physical gels of both theoretical and practical interest is their response to large stresses at constant shear rate or under a fixed macrocopic strain. In particular, these materials are often quite sensitive to applied stresses that can cause the self-assembled structure to progressively break down under flow or deformation. This disintegration of gel structure can lead to “yield” of the gel material, i.e., a fluidization transition, followed by shear thinning of the resulting heterogeneous “jelly-like” fluid. When the stress is removed, however, the material can relax back to its former equilibrium gel state, i.e., gel rejuvenation. In constrast, a non-equilibrium material will simply change its form and properties in a way that depends on processing history. Physical gels are thus unique self-healing materials in which the existence of equilibrium ensures their eventual recovery. The existence of equilibrium also has implications for the nature of both the linear and non-linear rheological response of gel materials, and the present paper explores this phenomenon based on simple scaling arguments of the kind frequently used in describing phase transitions and the properties of polymer solutions. Full article

(This article belongs to the Special Issue Polyelectrolyte Gels)

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