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Gels, Volume 4, Issue 1 (March 2018) – 24 articles

Cover Story (view full-size image): The image shows a snapshot of molecular dynamics simulation of a material composed of carbon nanotube clusters having a physically realistic morphology for commercial multiwall carbon nanotube materials (See Figure 1 of Vargas and Lara, Soft Matter 11, 4888 (2015)). The carbon nanotube clusters, termed “tumbleweeds”, interpenetrate and exhibit local topological interactions that lead to a topologically entangled state, as described in the review article by Douglas (gels-260712) in this issue. View the paper here.
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6 pages, 646 KiB  
Communication
A Simple Method of Interpretating the Effects of Electric Charges on the Volume Phase Transition of Thermosensitive Gels
by Hiroshi Maeda, Shigeo Sasaki, Hideya Kawasaki and Rie Kakehashi
Gels 2018, 4(1), 24; https://doi.org/10.3390/gels4010024 - 19 Mar 2018
Cited by 3 | Viewed by 2807
Abstract
Various apparently inconsistent experimental observations have been reported on the effects of electric charges on the volume phase transition of thermosensitive gels. A simple method of interpretating these results is presented. Full article
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9 pages, 2259 KiB  
Article
Effect of Sweeteners on the Solvent Transport Behaviour of Mechanically-Constrained Agarose Gels
by Isamu Kaneda
Gels 2018, 4(1), 23; https://doi.org/10.3390/gels4010023 - 16 Mar 2018
Cited by 4 | Viewed by 3839
Abstract
Investigating the solvent transport behaviour of edible gels is important because it is strongly related to flavour release. We previously reported the solvent transport behaviour of mechanically-constrained agarose gels. These studies clearly showed that agarose gels can be treated as soft porous bodies. [...] Read more.
Investigating the solvent transport behaviour of edible gels is important because it is strongly related to flavour release. We previously reported the solvent transport behaviour of mechanically-constrained agarose gels. These studies clearly showed that agarose gels can be treated as soft porous bodies. Herein, we investigated the effect of sweeteners on the solvent transport speed, which is an important issue in the food industry, using sucrose and xylitol. Sucrose caused a concentration-dependent reduction in solvent transport speed. One of the reasons for the effect is that the solvent to which sucrose was added reduced solvent flow speed within the porous agarose network. This finding provides valuable information for flavour release from compressed gels. Moreover, we found a similar effect for xylitol, which is a promising candidate for substituting sucrose in low-calorie foods. This study would provide basic knowledge for the development of a new type of low-calorie foods. Full article
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13 pages, 2114 KiB  
Article
Effect of Monomer Sequence along Network Chains on Thermoresponsive Properties of Polymer Gels
by Shohei Ida, Toru Kawahara, Hidekazu Kawabata, Tatsuya Ishikawa and Yoshitsugu Hirokawa
Gels 2018, 4(1), 22; https://doi.org/10.3390/gels4010022 - 10 Mar 2018
Cited by 11 | Viewed by 5192
Abstract
The effect of monomer sequence along the network chain on the swelling behavior of polymer gels should be clarified for the advanced control of swelling properties of gel materials. To this end, we systematically investigated the swelling properties of poly(acrylamide derivative) gels with [...] Read more.
The effect of monomer sequence along the network chain on the swelling behavior of polymer gels should be clarified for the advanced control of swelling properties of gel materials. To this end, we systematically investigated the swelling properties of poly(acrylamide derivative) gels with the same composition but different monomer sequence by utilizing two gel synthetic methods: copolymerization giving a random network and co-crosslinking giving a blocky network. Both of the copolymerization and the co-crosslinking gels were prepared from the combination of two of the three following monomers: hydrophilic N,N-dimethylacrylamide (DMAAm), hydrophobic N-n-butylacrylamide (NBAAm), and thermoresponsive N-isopropylacrylamide (NIPAAm) with various monomer compositions. The swelling measurement of the obtained gels showed totally different behaviors between the copolymerization and the co-crosslinking gels, even with the same monomer composition. The copolymerization gels had the average property from the two monomers, depending on monomer composition, because random monomer distribution changed the affinity of each network chain to water. On the other hand, the co-crosslinking gels behaved as if two components independently contributed to the swelling properties, probably due to the domain structure derived from two kinds of prepolymers. Full article
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11 pages, 2215 KiB  
Review
Hydrogels Based on Dynamic Covalent and Non Covalent Bonds: A Chemistry Perspective
by Francesco Picchioni and Henky Muljana
Gels 2018, 4(1), 21; https://doi.org/10.3390/gels4010021 - 08 Mar 2018
Cited by 54 | Viewed by 7861
Abstract
Hydrogels based on reversible covalent bonds represent an attractive topic for research at both academic and industrial level. While the concept of reversible covalent bonds dates back a few decades, novel developments continue to appear in the general research area of gels and [...] Read more.
Hydrogels based on reversible covalent bonds represent an attractive topic for research at both academic and industrial level. While the concept of reversible covalent bonds dates back a few decades, novel developments continue to appear in the general research area of gels and especially hydrogels. The reversible character of the bonds, when translated at the general level of the polymeric network, allows reversible interaction with substrates as well as responsiveness to variety of external stimuli (e.g., self-healing). These represent crucial characteristics in applications such as drug delivery and, more generally, in the biomedical world. Furthermore, the several possible choices that can be made in terms of reversible interactions generate an almost endless number of possibilities in terms of final product structure and properties. In the present work, we aim at reviewing the latest developments in this field (i.e., the last five years) by focusing on the chemistry of the systems at hand. As such, this should allow molecular designers to develop a toolbox for the synthesis of new systems with tailored properties for a given application. Full article
(This article belongs to the Special Issue Hydrogels Based on Dynamic Covalent Chemistry)
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16 pages, 4239 KiB  
Article
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 4883
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 [...] Read more.
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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14 pages, 1134 KiB  
Review
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 48 | Viewed by 9808
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 [...] Read more.
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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10 pages, 7167 KiB  
Article
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 5 | Viewed by 5583
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 [...] Read more.
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, 1293 KiB  
Article
Using Aggregation-Induced Emission to Understand Dipeptide Gels
by Ana M. Castilla, Bart Dietrich and Dave J. Adams
Gels 2018, 4(1), 17; https://doi.org/10.3390/gels4010017 - 09 Feb 2018
Cited by 13 | Viewed by 4654
Abstract
We describe the formation of structured liquids and gels from a functionalised dipeptide based on tetraphenylethylene. Tetraphenylethylene is well-known to be able to undergo aggregation-induced emission. We use the emission data to understand the behaviour of the dipeptide in water under a variety [...] Read more.
We describe the formation of structured liquids and gels from a functionalised dipeptide based on tetraphenylethylene. Tetraphenylethylene is well-known to be able to undergo aggregation-induced emission. We use the emission data to understand the behaviour of the dipeptide in water under a variety of conditions. The dipeptide forms viscous solutions at high pH. Gels can be formed by a pH-trigger, but syneresis occurs. Addition of a calcium salt also leads to a gel with slight syneresis. Addition of sodium chloride leads to a self-supporting material, but this is not a true gel from the rheological perspective. From the emission data, we infer that there are limited structural changes on addition of sodium chloride or acid, but there are significant changes in molecular packing when the gel is formed by addition of a calcium salt. Full article
(This article belongs to the Special Issue Supramolecular Gels)
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8 pages, 6854 KiB  
Article
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 3457
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 [...] Read more.
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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8 pages, 10152 KiB  
Communication
Controlling the Organization of Colloidal Sphero-Cylinders Using Confinement in a Minority Phase
by Niek Hijnen and Paul S. Clegg
Gels 2018, 4(1), 15; https://doi.org/10.3390/gels4010015 - 02 Feb 2018
Cited by 1 | Viewed by 3535
Abstract
We demonstrate experimentally that a phase-separating host solvent can be used to organize colloidal rods into different cluster and network states. The rods are silica sphero-cylinders which are preferentially wet by the water-rich phase of an oil–water binary liquid system. By beginning with [...] Read more.
We demonstrate experimentally that a phase-separating host solvent can be used to organize colloidal rods into different cluster and network states. The rods are silica sphero-cylinders which are preferentially wet by the water-rich phase of an oil–water binary liquid system. By beginning with the rods dispersed in the single-fluid phase and then varying the temperature to enter the demixed regime, a precisely chosen volume of water-rich phase can be created. We then show how this can be used to create independent clusters of rods, a percolating network, a network of clusters or a system that undergoes hindered phase separation. These different modes are selected by choosing the relative volumes of the rods and the water-rich phase and by the timing of the temperature change. Full article
(This article belongs to the Special Issue Colloid Chemistry)
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14 pages, 5179 KiB  
Review
Non-Conventional Methods for Gelation of Alginate
by Pavel Gurikov and Irina Smirnova
Gels 2018, 4(1), 14; https://doi.org/10.3390/gels4010014 - 01 Feb 2018
Cited by 87 | Viewed by 10924
Abstract
This review presents and critically evaluates recent advances in non-conventional gelation method of native alginate. A special focus is given to the following three methods: cryotropic gelation, non-solvent induced phase separation and carbon dioxide induced gelation. A few other gelation approaches are also [...] Read more.
This review presents and critically evaluates recent advances in non-conventional gelation method of native alginate. A special focus is given to the following three methods: cryotropic gelation, non-solvent induced phase separation and carbon dioxide induced gelation. A few other gelation approaches are also briefly reviewed. Results are discussed in the context of subsequent freeze and supercritical drying. The methods are selected so as to provide the readers with a range of novel tools and tactics of pore engineering for alginate and other anionic polysaccharides. Full article
(This article belongs to the Special Issue Aerogels 2018)
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13 pages, 1537 KiB  
Review
Stimuli-Responsive Cationic Hydrogels in Drug Delivery Applications
by G. Roshan Deen and Xian Jun Loh
Gels 2018, 4(1), 13; https://doi.org/10.3390/gels4010013 - 01 Feb 2018
Cited by 53 | Viewed by 7639
Abstract
Stimuli-responsive, smart, intelligent, or environmentally sensitive polymers respond to changes in external stimuli such as pH, temperature, ionic strength, surfactants, pressure, light, biomolecules, and magnetic field. These materials are developed in various network architectures such as block copolymers, crosslinked hydrogels, nanogels, inter-penetrating networks, [...] Read more.
Stimuli-responsive, smart, intelligent, or environmentally sensitive polymers respond to changes in external stimuli such as pH, temperature, ionic strength, surfactants, pressure, light, biomolecules, and magnetic field. These materials are developed in various network architectures such as block copolymers, crosslinked hydrogels, nanogels, inter-penetrating networks, and dendrimers. Stimuli-responsive cationic polymers and hydrogels are an interesting class of “smart” materials that respond reversibly to changes in external pH. These materials have the ability to swell extensively in solutions of acidic pH and de-swell or shrink in solutions of alkaline pH. This reversible swelling-shrinking property brought about by changes in external pH conditions makes these materials useful in a wide range of applications such as drug delivery systems and chemical sensors. This article focuses mainly on the properties of these interesting materials and their applications in drug delivery systems. Full article
(This article belongs to the Special Issue Stimuli-Responsive Gels)
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9 pages, 775 KiB  
Article
Densification and Strengthening of Aerogels by Sintering Heat Treatments or Plastic Compression
by Thierry Woignier and Laurent Duffours
Gels 2018, 4(1), 12; https://doi.org/10.3390/gels4010012 - 31 Jan 2018
Cited by 13 | Viewed by 3565
Abstract
Due to their broad range of porosity, aerogels are suited to various applications. The advantages of a broad range of porosity are used directly, for example, in thermal and acoustic insulation, as materials for space applications or in catalysers. However, an overly high [...] Read more.
Due to their broad range of porosity, aerogels are suited to various applications. The advantages of a broad range of porosity are used directly, for example, in thermal and acoustic insulation, as materials for space applications or in catalysers. However, an overly high pore volume can also be a drawback, for example, in a glass precursor and host matrix. Fortunately, aerogel porosity can be tailored using sintering or isostatic compression. Sets of silica aerogels—sintered and compressed aerogels—have been studied with the objective of comparing these different densification mechanisms. We focus on the mechanical changes during the two processes of densification. Full article
(This article belongs to the Special Issue Aerogels 2018)
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12 pages, 4558 KiB  
Article
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 53 | Viewed by 6909
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 [...] Read more.
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 (Cs) and gradually shifts to higher frequencies as Cs is decreased. The sticky-Rouse model describes the relaxation behavior at all Cs. However, collective relaxation of polyelectrolyte complexes gradually approaches a rubbery regime and eventually exhibits a gel-like response as Cs 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  
Article
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 3292
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 [...] Read more.
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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2 pages, 159 KiB  
Editorial
Gels as Templates for the Syntheses of Shape-Controlled Nanostructured Materials
by Pablo H. Di Chenna
Gels 2018, 4(1), 10; https://doi.org/10.3390/gels4010010 - 16 Jan 2018
Cited by 2 | Viewed by 2237
Abstract
The preparation of inorganic, organic and/or hybrid nanostructured materials with controlled shape and size is crucial for the development of nanotechnology, and it is nowadays the focus of intense research.[...] Full article
(This article belongs to the Special Issue Gels as Templates for Transcription)
15 pages, 8712 KiB  
Article
Clay-Facilitated Aqueous Dispersion of Graphite and Poly(vinyl alcohol) Aerogels Filled with Binary Nanofillers
by Lei Liu, Yuxin Wang, Saeed M. Alhassan, Hua Sun, Kyungwho Choi, Choongho Yu and David A. Schiraldi
Gels 2018, 4(1), 8; https://doi.org/10.3390/gels4010008 - 12 Jan 2018
Cited by 8 | Viewed by 4073
Abstract
Dispersion of graphite in water was achieved using clay as dispersing aid. In the absence of polymer, the clay/graphite suspensions were sufficiently stable to produce aerogels composed of very thin layers of uniformly dispersed nanoparticles. Poly(vinyl alcohol) (PVOH) aerogels containing binary nanofillers (clay [...] Read more.
Dispersion of graphite in water was achieved using clay as dispersing aid. In the absence of polymer, the clay/graphite suspensions were sufficiently stable to produce aerogels composed of very thin layers of uniformly dispersed nanoparticles. Poly(vinyl alcohol) (PVOH) aerogels containing binary nanofillers (clay plus graphite) were then fabricated and tested. These composites were found to maintain low thermal and electrical conductivities even with high loading of graphite. A unique compressive stress-strain behavior was observed for the aerogel, exhibiting a plateau in the densification region, likely due to sliding between clay and graphite layers within the PVOH matrix. The aerogels containing only graphite exhibited higher compressive modulus, yield stress and toughness values than the samples filled with binary nanofillers. X-ray diffraction (XRD) spectra for the same composite aerogel before and after compression testing illustrated the compression-induced dispersion changes of nanofillers. Composites containing 50 wt % graphite demonstrated a downshift of its 2D Raman peak implying graphite exfoliation to graphene with less than 5 layers. Full article
(This article belongs to the Special Issue Aerogels 2018)
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14 pages, 4254 KiB  
Article
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 4863
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 [...] Read more.
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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2 pages, 132 KiB  
Editorial
Acknowledgement to Reviewers of Gels in 2017
by Gels Editorial Office
Gels 2018, 4(1), 6; https://doi.org/10.3390/gels4010006 - 10 Jan 2018
Viewed by 1957
Abstract
Peer review is an essential part in the publication process, ensuring that Gels maintains high quality standards for its published papers[...] Full article
13 pages, 3673 KiB  
Article
Enhancement Studies on Manufacturing and Properties of Novel Silica Aerogel Composites
by Sunil Chandrakant Joshi, Periyasamy Manikandan and Yogeswari Jothi
Gels 2018, 4(1), 5; https://doi.org/10.3390/gels4010005 - 07 Jan 2018
Cited by 7 | Viewed by 5094
Abstract
Silica Aerogel composites are ultra-low density, highly porous foam-like materials that exhibit excellent thermal insulation and high strain recovery characteristics. In the present work, environment-friendly silica aerogel composites are fabricated using silica aerogel granules with bio based porcine-gelatin as the binding agent dissolved [...] Read more.
Silica Aerogel composites are ultra-low density, highly porous foam-like materials that exhibit excellent thermal insulation and high strain recovery characteristics. In the present work, environment-friendly silica aerogel composites are fabricated using silica aerogel granules with bio based porcine-gelatin as the binding agent dissolved in water and by further drying the mix at sub-zero condition. This article focuses on improvement studies carried on the mold design and the manufacturing process to achieve better geometric compliance for the silica aerogel composites. It also presents contact angle measurements, compressive behavior under different cycles of loading, time dependent behavior and flexural response of the composites. The influence of additives, such as fumed silica and carbon nanotubes on mechanical properties of the composites is also deliberated. Water droplet contact angle experiments confirmed the ultra-hydrophobic nature of the composites. The mechanical properties were characterized under cyclic loading-unloading compression and three-point flexure tests. On successive compression in three consecutive load cycles, the strain and thickness recovery were found to decrease by around 30%. The flexural properties of the aerogel composites were investigated using it as the core covered by thin carbon composite face sheets. It was found that the flexural strength and the failure strain of this aerogel sandwich composites is approximately half of the conventional nomex honeycomb sandwich equivalent. Full article
(This article belongs to the Special Issue Aerogels 2018)
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2739 KiB  
Article
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 7 | Viewed by 4542
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 [...] Read more.
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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5083 KiB  
Review
Kinetics of Supercritical Drying of Gels
by İbrahim Şahin, Yaprak Özbakır, Zeynep İnönü, Zeynep Ulker and Can Erkey
Gels 2018, 4(1), 3; https://doi.org/10.3390/gels4010003 - 29 Dec 2017
Cited by 84 | Viewed by 11050
Abstract
Supercritical drying of gels is considered as the most important step of aerogel production since it enables preservation of the three-dimensional pore structure which lead to unique material properties such as high porosity, low density, and large surface area. An understanding of the [...] Read more.
Supercritical drying of gels is considered as the most important step of aerogel production since it enables preservation of the three-dimensional pore structure which lead to unique material properties such as high porosity, low density, and large surface area. An understanding of the kinetics of supercritical drying is necessary to provide insight into material development, scale-up, and optimization of the aerogel manufacturing process. Thus, investigation of supercritical drying is gaining increased attention in recent years. This review paper covers the experimental considerations and techniques to study the kinetics of supercritical drying, fundamental mass transfer mechanisms during the drying process and modeling efforts to predict the drying kinetics for varying operating conditions and gel properties. Transport phenomena involving diffusion, convection, spillage by volume expansion, and axial dispersion are discussed by providing the fundamental equations and empirical correlations to predict transfer coefficients. A detailed review of literature covering experimental and theoretical studies on kinetics of supercritical drying is presented. Full article
(This article belongs to the Special Issue Aerogels 2018)
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975 KiB  
Article
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 4354
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.
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+. We investigate the effect of changing the chemical equilibria by modifying the dissociation constant 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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4500 KiB  
Communication
Supramolecular Gel Formation Based on Glycolipids Derived from Renewable Resources
by Krishnamoorthy Lalitha, Kandasamy Gayathri, Yadavali Siva Prasad, Rajendhiran Saritha, A. Thamizhanban, C. Uma Maheswari, Vellaisamy Sridharan and Subbiah Nagarajan
Gels 2018, 4(1), 1; https://doi.org/10.3390/gels4010001 - 24 Dec 2017
Cited by 7 | Viewed by 5915
Abstract
The potential applications of self-assembled supramolecular gels based on natural molecules encouraged the researchers to develop a versatile synthetic method for their structural analogues. Herein, we report a facile synthesis of glycolipid from renewable resources, cashew nut shell liquid,d and d-glucose in [...] Read more.
The potential applications of self-assembled supramolecular gels based on natural molecules encouraged the researchers to develop a versatile synthetic method for their structural analogues. Herein, we report a facile synthesis of glycolipid from renewable resources, cashew nut shell liquid,d and d-glucose in good yield. Gelation behavior of these glycolipids were studied in a wide range of solvents and oils. To our delight, compound 5b formed a hydrogel with Critical gelator concentration (CGC) of 0.29% w/v. Morphological analysis of the hydrogel depicts the formation of twisted fibers with an entangled network. Formation of a twisted fibrous structure was further identified by CD spectral studies with respect to temperature. The molecular self-assembly assisted by hydrogen bonding, hydrophobic, and π–π stacking interactions were identified by X-ray diffraction (XRD) and FTIR studies. Rheological analysis depicted the mechanical strength and stability of the hydrogel, which is crucial in predicting the practical applications of supramolecular soft materials. Full article
(This article belongs to the Special Issue Supramolecular Gels)
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