Supramolecular polysaccharide-based hydrogels have attracted considerable research interest recently due to their high structural functionality, low toxicity, and potential applications in foods, cosmetics, catalysis, drug delivery, tissue engineering and the environment. Modulation of the stability of hydrogels is of paramount importance, especially in the case of stimuli-responsive systems. This review will update the recent progress related to the rational design of supramolecular hydrogels with the objective of understanding the gelation process and improving their physical gelation properties for tailored applications. Emphasis will be given to supramolecular host–guest systems with reference to conventional gels in describing general aspects of gel formation. A brief account of the structural characterization of various supramolecular hydrogels is also provided in order to gain a better understanding of the design of such materials relevant to the nature of the intermolecular interactions, thermodynamic properties of the gelation process, and the critical concentration values of the precursors and the solvent components. This mini-review contributes to greater knowledge of the rational design of supramolecular hydrogels with tailored applications in diverse fields ranging from the environment to biomedicine.

Physicochemical Properties and the Gelation Process of Supramolecular Hydrogels: A Review

Chitosan-based blends for biomedical applications.

Introduction: The ever-increasing developments in pharmaceutical formulations have led to the widespread use of biodegradable polymers in various forms and configurations. In particular, interpenetrating network (IPN) and semi-IPN polymer structures that are capable of releasing drugs in a controlled manner have gained much wider importance in recent years.Areas covered: Recently, IPNs and semi-IPNs have emerged as innovative materials of choice in controlled release (CR) of drugs as the release from these systems depends on pH of the media and temperature in addition to the nature of the system. These networks can be prepared as smart hydrogels following chemical or physical crosslinking methods to show remarkable drug release patterns compared to single polymer systems.Expert opinion: A large number of IPNs and semi-IPNs have been reported in the literature. The present review is focused on the preparation methods and their CR properties with reference to anticancer, anti-asthmatic, antibiotic, anti-inf...

Controlled release of therapeutics using interpenetrating polymeric networks

Superabsorbent hydrogels of chitosan-g-polyacrylamide with N,N′-methylene-bis-acrylamide as a crosslinker were prepared via UV irradiation in the absence of photoinitiator under homogeneous conditions. The product was characterized by Fourier transform infrared spectroscopy, differential scanning calorimetry, and scanning electron microscopy to confirm the formation of hydrogels. The transparent hydrogels have been observed to exhibit as much as 2987% swelling in acidic solution. In addition, the hydrogel which hydrolyzed for 6 h (0.24 × 103 min) can have a water uptake of 106 times its weight (5300% swelling for 0.5 g hydrogel). The effect of several variables such as time, temperature, pH, acrylamide/chitosan ratio, crosslinker amount, and different media was explored. Finally, the prepared hydrogel have been used in adsorption of Zn(II) ions from water with high removal efficiency (0.636 meq g−1 or 20.8 mg g−1) at pH = 7. The experimental data of the adsorption equilibrium from Zn(II) solution fit well with the pseudo-second-order model.

UV-induced synthesis of chitosan-g-polyacrylamide semi-IPN superabsorbent hydrogels

Lidocaine hydrochloride (LidH) was formulated in sodium carboxymethyl cellulose/ gelatine (NaCMC/GEL) hydrogel and a ‘poke and patch’ microneedle delivery method was used to enhance permeation flux of LidH. The microparticles were formed by electrostatic interactions between NaCMC and GEL macromolecules within a water/oil emulsion in paraffin oil and the covalent crosslinking was by glutaraldehyde. The GEL to NaCMC mass ratio was varied between 1.6 and 2.7. The LidH encapsulation yield was 1.2 to 7% w/w. LidH NaCMC/GEL was assessed for encapsulation efficiency, zeta potential, mean particle size and morphology. Subsequent in vitro skin permeation studies were performed via passive diffusion and microneedle assisted permeation of LidH NaCMC/GEL to determine the maximum permeation rate through full thickness skin. LidH 2.4% w/w NaCMC/GEL 1:1.6 and 1:2.3 respectively, possessed optimum zeta potential. LidH 2.4% w/w NaCMC/GEL 1:2.3 and 1:2.7 demonstrate higher pseudoplastic behaviour. Encapsulation efficiency (14.9–17.2%) was similar for LidH 2.4% w/w NaCMC/GEL 1:1.6–1:2.3. Microneedle assisted permeation flux was optimum for LidH 2.4% w/w NaCMC/GEL 1:2.3 at 6.1 μg/ml/h. LidH 2.4% w/w LidH NaCMC/GEL 1:2.3 crossed the minimum therapeutic drug threshold with microneedle skin permeation in less than 70 min.

/pdf/microneedle-assisted-permeation-of-lidocaine-1w4gzh5nj3.pdf

Microneedle-assisted permeation of lidocaine carboxymethylcellulose with gelatine co-polymer hydrogel.

Semi-interpenetrating network microspheres of chitosan-(dextran-g-acrylamide) were prepared by emulsion-crosslinking method using glutaraldehyde (GA) as a crosslinking agent. Graft copolymerization of dextran with acrylamide (Dx-g-AAm) was carried out by aqueous free-radical polymerization using ceric ammonium nitrate (CAN) as initiator. The grafting efficiency was found to be 92%. Theophylline (TH), antiasthmatic drug, was successfully encapsulated into semi-INP microspheres by varying the ratio of Dx-g-AAm and amount of GA. The laser light scattering technique shows that the particles size increased with increasing amount of graft copolymer and decrease with increasing amount of GA. The % encapsulation efficiency was found to vary between 50 and 78. MPs were characterized by FTIR spectroscopy and differential scanning calorimetry (DSC) techniques to confirm the graft copolymer, formation of semi-IPN structure of MPs and molecular distribution of the drug molecules in the polymer matrix. In vitro release studies of TH from these matrices have been investigated at Ph 1.2 and 7.4 media and the slow release were extended up to 18 h at 37°C. The release rates were fitted to an empirical equation to estimate the diffusion exponent n, which indicated that the release from the MPs follows non-Fickian type.

Controlled release of theophylline through semi-interpenetrating network microspheres of chitosan-(dextran-g-acrylamide)

An interconnection between tissue inflammation and regeneration has been established through the regulation of defense and repair mechanisms within diseased dental tissue triggered by the release of immune-resolvent mediators. To better our understanding of the role of specific pro-resolving mediators (SPMs) in inflamed human bone marrow-derived mesenchymal stem cells (hBMMSCs), we studied the effects of Resolvin E1 (RvE1) and Maresin 1 (MaR1) in lipopoly-saccharide (LPS) stimulated hBMMSCs. The hBMMSCs were divided into five different groups, each of which was treated with or without SPMs. Group-1: negative control (no LPS stimulation), Group-2: positive control (LPS-stimulated), Group-3: RvE1 100 nM + 1 μg/mL LPS, Group-4: MaR1 100 nM + 1 µg/mL LPS, and Group-5: RvE1 100 nM + MaR1100 nM + 1 μg/mL LPS. Cell proliferation, apoptosis, migration, colony formation, Western blotting, cytokine array, and LC/MS analysis were all performed on each group to determine the impact of SPMs on inflammatory stem cells. According to our data, RvE1 plus MaR1 effectively reduced inflammation in hBMMSCs. In particular, IL-4, 1L-10, and TGF-β1 activation and downregulation of RANKL, TNF-α, and IFN-γ compared to groups receiving single SPM were shown to be significantly different (Group 3 and 4). In addition, the LC/MS analysis revealed the differentially regulated peptide’s role in immunological pathways that define the cellular state against inflammation. Inflamed hBMMSCs treated with a combination of Resolvin E1 (RvE1) and Maresin 1 (MaR1) promoted the highest inflammatory resolution compared to the other groups; this finding suggests a potential new approach of treating bacterially induced dental infections.

/pdf/anti-inflammatory-effect-of-specialized-proresolving-lipid-1vo99qaa.pdf

Ahmed A. Al-Kahtani

Papers

Controlled release of theophylline through semi-interpenetrating network microspheres of chitosan-(dextran-g-acrylamide)

Anti-Inflammatory Effect of Specialized Proresolving Lipid Mediators on Mesenchymal Stem Cells: An In Vitro Study