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Keywords = polyelectrolyte gel complexes

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19 pages, 3340 KB  
Article
Lidocaine-Loaded Thermoresponsive Gel for Accelerated Wound Healing in Dry Socket and Oral Wounds
by Nuttawut Supachawaroj, Kunchorn Kerdmanee and Sucharat Limsitthichaikoon
Gels 2024, 10(11), 739; https://doi.org/10.3390/gels10110739 - 14 Nov 2024
Cited by 6 | Viewed by 6652
Abstract
Dry socket, also known as alveolar osteitis, presents significant challenges in oral surgery because of severe pain and delayed wound healing. This study aims to address these challenges by developing and evaluating a lidocaine-loaded polyelectrolyte complex thermoresponsive gel (LG) designed to enhance wound [...] Read more.
Dry socket, also known as alveolar osteitis, presents significant challenges in oral surgery because of severe pain and delayed wound healing. This study aims to address these challenges by developing and evaluating a lidocaine-loaded polyelectrolyte complex thermoresponsive gel (LG) designed to enhance wound healing and provide effective pain management in oral wounds. The thermoresponsive gel transitions from a liquid to a gel at body temperature, ensuring sustained contact with the wound site and prolonged release of lidocaine. The in vitro assessments, including cytotoxicity and wound scratch assays, demonstrated the biocompatibility and therapeutic potential of the LG formulation. Following this, palatal wounds were induced in rats, with healing monitored over a 14-days period. Histological analyses were conducted to assess tissue regeneration and inflammation. The results indicated that the LG formulation significantly improved wound closure rates, reduced inflammation, and accelerated epithelialization compared with control groups, primarily because of the high content of hyaluronic acid (HA). The synergistic effects of HA combined with the thermoresponsive properties of the gel facilitated faster healing. These findings suggest that LG is a promising therapeutic option for enhancing oral wound healing and effectively managing pain, particularly in conditions such as dry socket. Full article
(This article belongs to the Special Issue Advanced Gel-Based Materials and Coatings with Enhanced Bioactivity)
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20 pages, 5992 KB  
Review
Recent Progress in Polyion Complex Nanoparticles with Enhanced Stability for Drug Delivery
by Xinlin Ma, Tianyi Zhao, Xiaoyue Ren, Hui Lin and Pan He
Polymers 2024, 16(13), 1871; https://doi.org/10.3390/polym16131871 - 30 Jun 2024
Cited by 7 | Viewed by 3560
Abstract
Polyion complex (PIC) nanoparticles, including PIC micelles and PICsomes, are typically composed of poly(ethylene glycol) block copolymers coupled with oppositely charged polyelectrolytes or therapeutic agents via electrostatic interaction. Due to a simple and rapid preparation process with high drug-loading efficiency, PIC nanoparticles are [...] Read more.
Polyion complex (PIC) nanoparticles, including PIC micelles and PICsomes, are typically composed of poly(ethylene glycol) block copolymers coupled with oppositely charged polyelectrolytes or therapeutic agents via electrostatic interaction. Due to a simple and rapid preparation process with high drug-loading efficiency, PIC nanoparticles are beneficial to maintaining the chemical integrity and high biological activity of the loaded drugs. However, the stability of PIC nanoparticles can be disrupted in high-ionic-strength solutions because electrostatic interaction is the DRIVING force; these disruptions can thus impair drug delivery. Herein, we summarize the advances in the use of PIC nanoparticles for delivery of charged drugs, focusing on the different chemical and physical strategies employed to enhance their stability, including enhancing the charge density, crosslinking, increasing hydrophobic interactions, forming hydrogen bonds, and the development of PIC-based gels. In particular, we describe the use of PIC nanoparticles to load peptide antibiotics targeting antibiotic-resistant and biofilm-related diseases and the use of nanoparticles that load chemotherapeutics and gaseous donors for cancer treatment. Furthermore, the application of PIC nanoparticles as magnetic resonance imaging contrast agents is summarized for the first time. Therefore, this review is of great significance for advances in the use of polymeric nanoparticles for functional drug delivery. Full article
(This article belongs to the Special Issue Biopolymer-Based Materials in Medical Applications)
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13 pages, 5452 KB  
Article
A Study on the Stoichiometry of Casein/Chitosan Gel Complexes as a Delivery System for Quercetin
by Sofia Milenkova, Nikolay Zahariev, Rita Ambrus, Bissera Pilicheva and Maria Marudova
Appl. Sci. 2023, 13(19), 10868; https://doi.org/10.3390/app131910868 - 30 Sep 2023
Cited by 7 | Viewed by 2538
Abstract
As a well-known plant flavanol, quercetin possesses a diverse range of biological properties. These include its ability to act as an antioxidant, reduce inflammation, and exhibit anticancer effects. Consequently, it finds extensive application in numerous models related to wound healing. However, the poor [...] Read more.
As a well-known plant flavanol, quercetin possesses a diverse range of biological properties. These include its ability to act as an antioxidant, reduce inflammation, and exhibit anticancer effects. Consequently, it finds extensive application in numerous models related to wound healing. However, the poor physicochemical characteristics of the molecule (which include low solubility, stability, and permeability) eventually reduce its bioavailability at the targeted sites. A variety of nano formulations with great therapeutic potential have been created in order to get around these obstacles on the way to successful therapy. The current investigation aims to examine the properties of nano- and micro-sized casein/chitosan gel polyelectrolyte complexes (PECs) with respect to their potential for quercetin loading and release. Four different types of hydrogel particles at pH 6 and different casein/chitosan charge ratios were synthesized; namely, 1:1, 2:1, 4:1, and 6:1 in excesses of casein. The attractive electrostatic interactions between the oppositely charged polyelectrolytes were proved by FT-IR spectroscopy. The process yield increased from 37.5% to 72.5% in excesses of casein. The gel particle’s size varied between 377 nm and 5.72 µm depending on the casein/chitosan stoichiometry. The morphology of the obtained gel polyelectrolyte complexes was found to be spherical, based on scanning electron microscopy and atomic force microscopy analysis. The quercetin loading efficiency was above 95% for all investigated hydrogel complexes. Investigation of the physical state of the loaded polyphenol by the differential scanning calorimetry and X-ray powdered diffraction technique suggested the occurrence of partial recrystallization phenomena. The quercetin release test was performed in phosphate buffer (pH 5.5) at 32 °C and permanent stirring at 50 rpm. A zero-order model was used to describe in the best way the release kinetics. The reported casein/chitosan complexes loaded with quercetin may find application in wound healing as a concomitant treatment. Full article
(This article belongs to the Special Issue Hydrogels and Microgels: Fundamentals, Fabrication and Applications)
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15 pages, 3576 KB  
Article
Flocculation of Cellulose Microfiber and Nanofiber Induced by Chitosan–Xylan Complexes
by Gabriela Adriana Bastida, Quim Tarrés, Roberto Aguado, Marc Delgado-Aguilar, Miguel Ángel Zanuttini and María Verónica Galván
Nanomaterials 2023, 13(17), 2420; https://doi.org/10.3390/nano13172420 - 25 Aug 2023
Cited by 1 | Viewed by 2136
Abstract
This study aims to provide a comprehensive understanding of the key factors influencing the rheological behavior and the mechanisms of natural polyelectrolyte complexes (PECs) as flocculation agents for cellulose microfibers (CMFs) and nanofibers (CNFs). PECs were formed by combining two polyelectrolytes: xylan (Xyl) [...] Read more.
This study aims to provide a comprehensive understanding of the key factors influencing the rheological behavior and the mechanisms of natural polyelectrolyte complexes (PECs) as flocculation agents for cellulose microfibers (CMFs) and nanofibers (CNFs). PECs were formed by combining two polyelectrolytes: xylan (Xyl) and chitosan (Ch), at different Xyl/Ch mass ratios: 60/40, 70/30, and 80/20. First, Xyl, Ch, and PEC solutions were characterized by measuring viscosity, critical concentration (c*), rheological parameter, ζ-potential, and hydrodynamic size. Then, the flocculation mechanisms of CMF and CNF suspensions with PECs under dynamic conditions were studied by measuring viscosity, while the flocculation under static conditions was examined through gel point measurements, floc average size determination, and ζ-potential analysis. The findings reveal that PEC solutions formed with a lower xylan mass ratio showed higher intrinsic viscosity, higher hydrodynamic size, higher z-potential, and a lower c*. This is due to the high molecular weight, charge, and gel-forming ability. All the analyzed solutions behave as a typical non-Newtonian shear-thinning fluid. The flocculation mechanisms under dynamic conditions showed that a very low dosage of PEC (between 2 and 6 mg PEC/g of fiber) was sufficient to produce flocculation. Under dynamic conditions, an increase in viscosity indicates flocculation at this low PEC dosage. Finally, under static conditions, maximum floc sizes were observed at the same PEC dosage where minimum gel points were reached. Higher PEC doses were required for CNF suspensions than for CMF suspensions. Full article
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17 pages, 4591 KB  
Article
pH-Sensitive Poly(acrylic acid)-g-poly(L-lysine) Charge-Driven Self-Assembling Hydrogels with 3D-Printability and Self-Healing Properties
by Maria-Eleni Kargaki, Foteini Arfara, Hermis Iatrou and Constantinos Tsitsilianis
Gels 2023, 9(7), 512; https://doi.org/10.3390/gels9070512 - 25 Jun 2023
Cited by 5 | Viewed by 2884
Abstract
We report the rheological behavior of aqueous solutions of a graft copolymer polyampholyte, constituted of polyacrylic acid (PAA) backbone grafted by Poly(L-lysine) (PAA-b-PLL). The graft copolymer self-assembles in aqueous media, forming a three-dimensional (3D) network through polyelectrolyte complexation of the oppositely [...] Read more.
We report the rheological behavior of aqueous solutions of a graft copolymer polyampholyte, constituted of polyacrylic acid (PAA) backbone grafted by Poly(L-lysine) (PAA-b-PLL). The graft copolymer self-assembles in aqueous media, forming a three-dimensional (3D) network through polyelectrolyte complexation of the oppositely charged PAA and PLL segments. Rheological investigations showed that the hydrogel exhibits interesting properties, namely, relatively low critical gel concentration, elastic response with slow dynamics, remarkable extended critical strain to flow, shear responsiveness, injectability, 3D printability and self-healing. Due to the weak nature of the involved polyelectrolyte segments, the hydrogel properties display pH-dependency, and they are affected by the presence of salt. Especially upon varying pH, the PLL secondary structure changes from random coil to α-helix, affecting the crosslinking structural mode and, in turn, the overall network structure as reflected in the rheological properties. Thanks to the biocompatibility of the copolymer constituents and the biodegradability of PLL, the designed gelator seems to exhibit potential for bioapplications. Full article
(This article belongs to the Special Issue Structured Gels: Mechanics, Responsivity and Applications)
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14 pages, 2685 KB  
Article
Flexible Humidity Sensor Based on Au Nanoparticles/Organosilica-Containing Polyelectrolyte Composite
by Pi-Guey Su and Chih-Chang Hsu
Chemosensors 2023, 11(5), 291; https://doi.org/10.3390/chemosensors11050291 - 13 May 2023
Cited by 3 | Viewed by 2625
Abstract
A novel flexible humidity sensor incorporating gold nanoparticles (Au NPs) and a trifunctional organosilica compound has been developed through the integration of sol–gel processing, free radical polymerization, and self-assembly techniques. The trifunctional organosilica was initially synthesized by modifying (3-mercaptopropyl)trimethoxysilane (thiol-MPTMS) with 3-(trimethoxysilyl)propyl methacrylate [...] Read more.
A novel flexible humidity sensor incorporating gold nanoparticles (Au NPs) and a trifunctional organosilica compound has been developed through the integration of sol–gel processing, free radical polymerization, and self-assembly techniques. The trifunctional organosilica was initially synthesized by modifying (3-mercaptopropyl)trimethoxysilane (thiol-MPTMS) with 3-(trimethoxysilyl)propyl methacrylate (vinyl-TMSPMA). Subsequently, a hydrophilic polyelectrolyte, [3(methacryloylamino)propyl]trimethyl ammonium chloride (MAPTAC), was grafted onto the MPTMS-TMSPMA gel. The Au NPs were assembled onto the thiol groups present in the MPTMS-TMSPMA-MAPTAC gel network. The compositional and microstructural properties of the Au NPs/MPTMS-TMSPMA-MAPTAC composite film were investigated utilizing Fourier transform infrared spectroscopy (FTIR) and scanning electron microscopy (SEM). The presence of thiol groups and mesoporous silica skeletons ensured the stability of the humidity-sensing film on the substrate under highly humid conditions, while the hydrophilic groups functioned as humidity-sensitive sites. This innovative humidity sensor demonstrated high sensitivity, acceptable linearity, minimal hysteresis, and rapid response time across a broad range of working humidity levels. Based on the complex impedance spectra analysis, hydronium ions (H3O+) were determined to govern the conductance process of the flexible humidity sensor. Full article
(This article belongs to the Section Materials for Chemical Sensing)
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14 pages, 6737 KB  
Article
Humic-Based Polyelectrolyte Complexes for Dust Suppression
by Alexander Volikov, Evgeniya A. Karpukhina, Konstantin S. Larionov, Daniil A. Kozlov and Irina V. Perminova
Polymers 2023, 15(6), 1514; https://doi.org/10.3390/polym15061514 - 18 Mar 2023
Cited by 3 | Viewed by 2894
Abstract
The present study proposes a novel application of humic substance–aminosilsesquioxane polyelectrolyte complexes (HS–ASQ) as dust suppressants. These complexes are synthesized through the reaction between humic substances (HS) and 3-aminopropyltriethoxysilane (APTES) in aqueous solution, resulting in the formation of active silanol groups that can [...] Read more.
The present study proposes a novel application of humic substance–aminosilsesquioxane polyelectrolyte complexes (HS–ASQ) as dust suppressants. These complexes are synthesized through the reaction between humic substances (HS) and 3-aminopropyltriethoxysilane (APTES) in aqueous solution, resulting in the formation of active silanol groups that can bind to mineral surfaces and condense, forming gels. The HS–ASQ compositions were found to have a high sorption capacity for dust particles and could form coatings on their surface without cementing the dust, making them potentially useful for environmental applications. The viscosity of the HS–ASQ compositions can be controlled by adding carboxymethylcellulose (CMC), which also enhances their dust suppression abilities. Different compositions of HS–ASQ were synthesized by varying the proportions of APTES and CMC, and dust treated with these samples was assessed for its resistance to wind erosion using a laboratory-scale setup. Treatment with the HS–ASQ composition resulted in substantial reductions in PM10 and PM2.5 concentrations (particulate matter with aerodynamic diameters of 10 µm and 2.5 µm, respectively) of up to 77% and 85%, respectively, compared to the control. Full article
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18 pages, 4063 KB  
Article
Comparative Study of Physicochemical Properties of Alginate Composite Hydrogels Prepared by the Physical Blending and Electrostatic Assembly Methods
by Yanshi Wen, Xiuqiong Chen, Huiqiong Yan and Qiang Lin
Gels 2022, 8(12), 799; https://doi.org/10.3390/gels8120799 - 5 Dec 2022
Cited by 10 | Viewed by 3593
Abstract
Alginate hydrogel commonly suffers from defects, such as weak mechanical properties, the shortage of long-term stability in physiological medium and the lack of mammalian cell adhesivity due to its strong hydrophilicity in biomedical application. For this reason, the homogeneous alginate hydrogels (Alg Gel) [...] Read more.
Alginate hydrogel commonly suffers from defects, such as weak mechanical properties, the shortage of long-term stability in physiological medium and the lack of mammalian cell adhesivity due to its strong hydrophilicity in biomedical application. For this reason, the homogeneous alginate hydrogels (Alg Gel) were successfully prepared by the D-glucono-δ-lactone/hydroxyapatite (HAP/GDL) cross-linking system, and then, the physical blending and alternating electrostatic assembly technology were proposed to fabricate alginate composite hydrogels (Alg-GT, Alg-CS-GT and ALG/GT-CS). The feasibility of the design methods was verified through the comparative analysis of their physicochemical properties and biological activity. In particular, the effects of physical blending and alternating electrostatic assembly technology on the pore structure, mechanical properties, swelling, degradation, cell adhesion and proliferation of composite hydrogels were also investigated. Experimental results showed that the formation of polyelectrolyte complexes by electrostatic assembly between biological macromolecules and the covalent cross-linking of EDC/NHS to GT improved the vulnerability of ion cross-linking, enhanced the mechanical properties and swelling stability of the composite hydrogels, and regulated their pore structure and in vitro biodegradability properties. Furthermore, MC3T3-E1 cells could exhibit good cell adhesion, cell viability and cell proliferation on the alginate composite hydrogels. Among them, Alg-CS-GT showed the best cell proliferation ability and differentiation effect due to its good cell adhesion. In view of the excellent physicochemical properties and biological activity of Alg-CS-GT, it exhibited great potential in biomedical application for tissue engineering. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Functional Gels)
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11 pages, 934 KB  
Perspective
Chitosan Schiff-Base Hydrogels—A Critical Perspective Review
by Ioana A. Duceac and Sergiu Coseri
Gels 2022, 8(12), 779; https://doi.org/10.3390/gels8120779 - 28 Nov 2022
Cited by 39 | Viewed by 6218
Abstract
Chitosan is quite a unique polysaccharide due to the presence of the amine groups naturally occurring in its structure. This feature renders it into a polycation which makes it appealing for preparing polyelectrolyte complexes or imine bonds gels. Therefore, the vast majority of [...] Read more.
Chitosan is quite a unique polysaccharide due to the presence of the amine groups naturally occurring in its structure. This feature renders it into a polycation which makes it appealing for preparing polyelectrolyte complexes or imine bonds gels. Therefore, the vast majority of hydrogels prepared using Schiff base chemistry have chitosan as one component. Usually, the counterpart is a low molecular weight aldehyde or a macromolecular periodate-oxidized polysaccharide, i.e., cellulose, pullulan, starch, alginate, hyaluronic acid, etc. Indisputable advantages of hydrogels include their quick gelation, no need for crosslinking agents, and self-healing and injectability properties. This gives grounds for further research, both fundamental in materials science and applicative in various domains. This article is a critical assessment of the most relevant aspects of this topic. It also provides a short review of some of the most interesting research reported in the literature supporting the main observations of this perspective. Full article
(This article belongs to the Special Issue Recent Developments in Chitosan Hydrogels)
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20 pages, 5808 KB  
Article
Modulation of Molecular Structure and Mechanical Properties of κ-Carrageenan-Gelatin Hydrogel with Multi-Walled Carbon Nanotubes
by Aidar T. Gubaidullin, Anastasiya O. Makarova, Svetlana R. Derkach, Nicolai G. Voron’ko, Aidar I. Kadyirov, Sufia A. Ziganshina, Vadim V. Salnikov, Olga S. Zueva and Yuri F. Zuev
Polymers 2022, 14(12), 2346; https://doi.org/10.3390/polym14122346 - 9 Jun 2022
Cited by 30 | Viewed by 4559
Abstract
Hydrogels, three-dimensional hydrophilic water-insoluble polymer networks having mechanical properties inherent for solids, have attracted continuous research attention over a long time period. Here, we studied the structure and properties of hydrogel based on gelatin, κ-carrageenan and CNTs using the combination of SAXS, PXRD, [...] Read more.
Hydrogels, three-dimensional hydrophilic water-insoluble polymer networks having mechanical properties inherent for solids, have attracted continuous research attention over a long time period. Here, we studied the structure and properties of hydrogel based on gelatin, κ-carrageenan and CNTs using the combination of SAXS, PXRD, AFM microscopy, SEM and rheology methods. We have shown that the integration of polysaccharide and protein in the composite hydrogel leads to suppression of their individual structural features and homogenization of two macromolecular components into a single structural formation. According to obtained SAXS results, we observed the supramolecular complex, which includes both polysaccharide and protein components associated with each other. It was determined that hydrogel structure formed in the initial solution state (dispersion) retains hydrogel supramolecular structure under its cooling up to gel state. The sizes of dense cores of these polyelectrolyte complexes (PEC) slightly decrease in the gel state in comparison with PEC water dispersion. The introduction of CNTs to hydrogel does not principally change the type of supramolecular structure and common structural tendencies observed for dispersion and gel states of the system. It was shown that carbon nanotubes embedded in hydrogel act as the supplementary template for formation of the three-dimensional net, giving additional mechanical strengthening to the studied system. Full article
(This article belongs to the Section Biobased and Biodegradable Polymers)
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32 pages, 8833 KB  
Review
Weak Polyelectrolytes as Nanoarchitectonic Design Tools for Functional Materials: A Review of Recent Achievements
by Noelia M. Sanchez-Ballester, Flavien Sciortino, Sajjad Husain Mir and Gaulthier Rydzek
Molecules 2022, 27(10), 3263; https://doi.org/10.3390/molecules27103263 - 19 May 2022
Cited by 23 | Viewed by 4791
Abstract
The ionization degree, charge density, and conformation of weak polyelectrolytes can be adjusted through adjusting the pH and ionic strength stimuli. Such polymers thus offer a range of reversible interactions, including electrostatic complexation, H-bonding, and hydrophobic interactions, which position weak polyelectrolytes as key [...] Read more.
The ionization degree, charge density, and conformation of weak polyelectrolytes can be adjusted through adjusting the pH and ionic strength stimuli. Such polymers thus offer a range of reversible interactions, including electrostatic complexation, H-bonding, and hydrophobic interactions, which position weak polyelectrolytes as key nano-units for the design of dynamic systems with precise structures, compositions, and responses to stimuli. The purpose of this review article is to discuss recent examples of nanoarchitectonic systems and applications that use weak polyelectrolytes as smart components. Surface platforms (electrodeposited films, brushes), multilayers (coatings and capsules), processed polyelectrolyte complexes (gels and membranes), and pharmaceutical vectors from both synthetic or natural-type weak polyelectrolytes are discussed. Finally, the increasing significance of block copolymers with weak polyion blocks is discussed with respect to the design of nanovectors by micellization and film/membrane nanopatterning via phase separation. Full article
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11 pages, 3350 KB  
Article
Electrochemical Glue for Binding Chitosan–Alginate Hydrogel Fibers for Cell Culture
by Yoshinobu Utagawa, Kosuke Ino, Tatsuki Kumagai, Kaoru Hiramoto, Masahiro Takinoue, Yuji Nashimoto and Hitoshi Shiku
Micromachines 2022, 13(3), 420; https://doi.org/10.3390/mi13030420 - 8 Mar 2022
Cited by 7 | Viewed by 5505
Abstract
Three-dimensional organs and tissues can be constructed using hydrogels as support matrices for cells. For the assembly of these gels, chemical and physical reactions that induce gluing should be induced locally in target areas without causing cell damage. Herein, we present a novel [...] Read more.
Three-dimensional organs and tissues can be constructed using hydrogels as support matrices for cells. For the assembly of these gels, chemical and physical reactions that induce gluing should be induced locally in target areas without causing cell damage. Herein, we present a novel electrochemical strategy for gluing hydrogel fibers. In this strategy, a microelectrode electrochemically generated HClO or Ca2+, and these chemicals were used to crosslink chitosan–alginate fibers fabricated using interfacial polyelectrolyte complexation. Further, human umbilical vein endothelial cells were incorporated into the fibers, and two such fibers were glued together to construct “+”-shaped hydrogels. After gluing, the hydrogels were embedded in Matrigel and cultured for several days. The cells spread and proliferated along the fibers, indicating that the electrochemical glue was not toxic toward the cells. This is the first report on the use of electrochemical glue for the assembly of hydrogel pieces containing cells. Based on our results, the electrochemical gluing method has promising applications in tissue engineering and the development of organs on a chip. Full article
(This article belongs to the Special Issue Frontiers in Micromachines in Japan)
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19 pages, 3013 KB  
Article
Evidence of Many-Body Interactions in the Virial Coefficients of Polyelectrolyte Gels
by Ferenc Horkay and Jack F. Douglas
Gels 2022, 8(2), 96; https://doi.org/10.3390/gels8020096 - 4 Feb 2022
Cited by 7 | Viewed by 2852
Abstract
Simulation studies of aqueous polymer solutions, and heuristic arguments by De Gennes for aqueous polyethylene oxide polymer solutions, have suggested that many-body interactions can give rise to the ‘anomalous’ situation in which the second osmotic virial coefficient is positive, while the third virial [...] Read more.
Simulation studies of aqueous polymer solutions, and heuristic arguments by De Gennes for aqueous polyethylene oxide polymer solutions, have suggested that many-body interactions can give rise to the ‘anomalous’ situation in which the second osmotic virial coefficient is positive, while the third virial coefficient is negative. This phenomenon was later confirmed in analytic calculations of the phase behavior and the osmotic pressure of complex fluids exhibiting cooperative self-assembly into extended dynamic polymeric structures by Dudowicz et al. In the present study, we experimentally confirm the occurrence of this osmotic virial sign inversion phenomenon for several highly charged model polyelectrolyte gels (poly(acrylic acid), poly(styrene sulfonate), DNA, hyaluronic acid), where the virial coefficients are deduced from osmotic pressure measurements. Our observations qualitatively accord with experimental and simulation studies indicating that polyelectrolyte materials exhibit supramolecular assembly in solution, another symptomatic property of fluids exhibiting many-body interactions. We also find that the inversion in the variation of the second (A2) and third (A2) virial coefficients upon approach to phase separation does not occur in uncharged poly(vinyl acetate) gels. Finally, we briefly discuss the estimation of the osmotic compressibility of swollen polyelectrolyte gels from neutron scattering measurements as an alternative to direct, time-consuming and meticulous osmotic pressure measurements. We conclude by summarizing some general trends and suggesting future research directions of natural and synthetic polyelectrolyte hydrogels. Full article
(This article belongs to the Collection Feature Papers in Gel Materials)
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14 pages, 2060 KB  
Article
Swelling and Mechanical Properties of Polyacrylamide-Derivative Dual-Crosslink Hydrogels Having Metal–Ligand Coordination Bonds as Transient Crosslinks
by Louis Debertrand, Jingwen Zhao, Costantino Creton and Tetsuharu Narita
Gels 2021, 7(2), 72; https://doi.org/10.3390/gels7020072 - 15 Jun 2021
Cited by 22 | Viewed by 4672
Abstract
Hydrogels that have both permanent chemical crosslinks and transient physical crosslinks are good model systems to represent tough gels. Such “dual-crosslink” hydrogels can be prepared either by simultaneous polymerization and dual crosslinking (one-pot synthesis) or by diffusion/complexation of the physical crosslinks to the [...] Read more.
Hydrogels that have both permanent chemical crosslinks and transient physical crosslinks are good model systems to represent tough gels. Such “dual-crosslink” hydrogels can be prepared either by simultaneous polymerization and dual crosslinking (one-pot synthesis) or by diffusion/complexation of the physical crosslinks to the chemical network (diffusion method). To study the effects of the preparation methods and of the crosslinking ratio on the mechanical properties, the equilibrium swelling of the dual-crosslink gels need to be examined. Since most of these gels are polyelectrolytes, their swelling properties are complex, so no systematic study has been reported. In this work, we synthesized model dual-crosslink gels with metal–ligand coordination bonds as physical crosslinks by both methods, and we proposed a simple way of adding salt to control the swelling ratio prepared by ion diffusion. Tensile and linear rheological tests of the gels at the same swelling ratio showed that during the one-pot synthesis, free radical polymerization was affected by the transition metal ions used as physical crosslinkers, while the presence of electrostatic interactions did not affect the role of the metal complexes on the mechanical properties. Full article
(This article belongs to the Special Issue Polyelectrolyte Gels: Volume II)
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24 pages, 5567 KB  
Article
Optimization of Novel Naproxen-Loaded Chitosan/Carrageenan Nanocarrier-Based Gel for Topical Delivery: Ex Vivo, Histopathological, and In Vivo Evaluation
by Sobia Noreen, Fahad Pervaiz, Akram Ashames, Manal Buabeid, Khairi Fahelelbom, Hina Shoukat, Irsah Maqbool and Ghulam Murtaza
Pharmaceuticals 2021, 14(6), 557; https://doi.org/10.3390/ph14060557 - 11 Jun 2021
Cited by 44 | Viewed by 7046
Abstract
Naproxen (NAP) is commonly used for pain, inflammation, and stiffness associated with arthritis. However, systemic administration is linked with several gastrointestinal tract (GIT) side effects. The present work aims to prepare and evaluate NAP nanoparticulate shells of chitosan (CS) and carrageenan (CRG) loaded [...] Read more.
Naproxen (NAP) is commonly used for pain, inflammation, and stiffness associated with arthritis. However, systemic administration is linked with several gastrointestinal tract (GIT) side effects. The present work aims to prepare and evaluate NAP nanoparticulate shells of chitosan (CS) and carrageenan (CRG) loaded into a Carbopol 940 (Ca-940) gel system with unique features of sustained drug delivery as well as improved permeation through a topical route. Moreover, this study aims to evaluate its ex vivo, histopathological, and in vivo anti-inflammatory activity in albino Wistar rats. The percentage of ex vivo drug permeation patterns in the optimized formulation (No) was higher (88.66%) than the control gel (36.195%). Oral toxicity studies of developed nanoparticles in albino rabbits showed that the NAP-loaded CS/CRG are non-toxic and, upon histopathological evaluation, no sign of incompatibility was observed compared to the control group. A In Vivo study showed that the optimized gel formulation (No) was more effective than the control gel (Nc) in treating arthritis-associated inflammation. The sustained permeation and the absence of skin irritation make this novel NAP nanoparticle-loaded gel based on CS/CRG a suitable drug delivery system for topical application and has the potential for improved patient compliance and reduced GIT-related side effects in arthritis. Full article
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