Polysaccharide-based hydrogels crosslink density equation: A rheological and LF-NMR study of polymer-polymer interactions

Kopač, Tilen; Abrami, Michela; Grassi, Mario; Ručigaj, Aleš; Krajnc, Matjaž

doi:10.1016/j.carbpol.2021.118895

Cited by 59 publications

(12 citation statements)

References 66 publications

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“…The root-mean-square deviation (RMSD) was employed to determine whether the system had reached equilibrium, and then the equilibrium state was corroborated by observing the changes in end-to-end distance and radius of gyration over time, as shown in Figure S1. For our model, the system density was calculated with the experimental water gel density, as shown in Figure S2, and the result was consistent with the experimental value of 1 g/cm 3 . , This comparison demonstrates the credibility of our simulation approach in describing the spatial structure and intermolecular interactions within the system.…”

Section: Resultssupporting

confidence: 75%

Effects of the Degree of Phenol Substitution on Molecular Structures and Properties of Chitosan-Phenol-Based Self-Healing Hydrogels

Gong,

Hsu,

Chang

et al. 2023

ACS Biomater. Sci. Eng.

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Click chemistry is commonly used to prepare hydrogels, and chitosan-phenol prepared by using a Schiff base has been widely employed in the field of biomaterials. Chitosan-phenol is a derivative of chitosan; the phenol groups can disrupt both the inter-and intramolecular hydrogen bonds in chitosan, thereby reducing its crystallinity and improving its water solubility. In addition, chitosan-phenol exhibits various beneficial physiological functions. However, it is still unclear whether the degree of phenol substitution in the chitosan main chain affects the molecular interactions and structural properties of the self-healing hydrogels. To explore this issue, we investigated the molecular structure and network of self-healing hydrogels composed of chitosan-phenol with varying degrees of phenol substitution and dibenzaldehyde poly(ethylene oxide) (DB-PEO) using molecular dynamics simulations. We observed that when the degree of phenol substitution in the self-healing hydrogel was less than 15%, an increase in the degree of phenol substitution led to an increase in the interactions between chitosan-phenol and DB-PEO, and it enhanced the dynamic covalent bond cross-linking generated through the Schiff base reaction. However, when the degree of phenol substitution exceeded 15%, excessive phenol groups caused excessive intramolecular interactions within chitosan-phenol molecules, which reduced the binding between chitosan-phenol and DB-PEO. Our results revealed the influence of the degree of phenol substitution on the molecular structure of the self-healing hydrogels and showed an optimal degree of phenol substitution. These findings provide important insights for the future design of self-healing hydrogels based on chitosan and should help in enhancing the applicability of hydrogels in the field of biomedicine.

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Section: Resultssupporting

confidence: 75%

Effects of the Degree of Phenol Substitution on Molecular Structures and Properties of Chitosan-Phenol-Based Self-Healing Hydrogels

Gong,

Hsu,

Chang

et al. 2023

ACS Biomater. Sci. Eng.

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“…The curve of PMCTH-4 in Figure 5d shows that G″ is always slightly lower than G′ and there is no intersection point, illustrating that the elastic response of PMCTH-4 is stronger than the viscous response. The over-high concentration of the crosslinking agent MC will enhance the gel crosslinking degree, which is the reason why the gel elasticity is dominant and exhibits an elastic solid behavior at this time, 31 resulting in the LCST falling back (Figure 6).…”

Section: Rheological Studiesmentioning

confidence: 99%

Thermosensitive PNIPAM-Based Hydrogel Crosslinked by Composite Nanoparticles as Rapid Wound-Healing Dressings

Liu

Gao

et al. 2023

Biomacromolecules

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Chronic wounds are prone to produce excessive reactive oxygen species (ROS), which are the main reason for multiple bacterial infections and ulcers at the wound. Therefore, regulating ROS is the key in the process of wound healing. Herein, a new type of thermosensitive hydrogels is developed to improve the scavenging efficiency of ROS and accelerate wound repair. Nano-CeO2 was uniformly dispersed on the surface of mesoporous silica (MSN). The nanocomposite particles were physically crosslinked with poly(N-isopropylacrylamide) (PNIPAM) to form a MSN-CeO2@PNIPAM thermoresponsive hydrogel (PMCTH). The stability, temperature sensitivity, rheological properties, biocompatibility, and wound healing ability of the PMCTH were evaluated in detail. The results showed that the hydrogel could not only maintain the stability of the system for a long time with low biological toxicity but also have a phase transition temperature close to the human body temperature. In addition, the PMCTH was directly applied onto the skin surface. The MSN-CeO2 nanoparticles would be dispersed in the hydrogel to restrict ROS exacerbation effects and promoted the formation of blood vessels as well as surrounding tissues, accelerating the wound healing. More importantly, animal experiments showed that when the mass ratio of CeO2 to MSN was 40%, the wound healing rate reached up to 78% on the 10th day, which was far higher than that of other experimental groups. This study provides a new strategy and experimental basis for the applications of functional hydrogels in wound repair.

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“…the spatial organization of the sample network that heavily affects the S/V ratio [26]. For instance, in many polymeric systems, crosslinking induces a spatial reorganization of the polymeric chains contained in the original solution that involves the increase of the ratio S/V [31,32]. This, in turn, reflects in the increase of (1/T 2 ) m and in the decrease of T 2m .…”

Section: Low-field Nmrmentioning

confidence: 99%

Effect of chest physiotherapy on cystic fibrosis sputum nanostructure: an experimental and theoretical approach

Abrami

Maschio

Conese

et al. 2022

Drug Deliv. and Transl. Res.

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Cystic fibrosis (CF) is a disease characterized by the production of viscous mucoid secretions in multiple organs, particularly the airways. The pathological increase of proteins, mucin and biological polymers determines their arrangement into a three-dimensional polymeric network, affecting the whole mucus and impairing the muco-ciliary clearance which promotes inflammation and bacterial infection. Thus, to improve the efficacy of the drugs usually applied in CF therapy (e.g., mucolytics, anti-inflammatory and antibiotics), an in-depth understanding of the mucus nanostructure is of utmost importance. Drug diffusivity inside a gel-like system depends on the ratio between the diffusing drug molecule radius and the mesh size of the network. Based on our previous findings, we propose the combined use of rheology and low field NMR to study the mesh size distribution of the sputum from CF patients. Specifically, we herein explore the effects of chest physiotherapy on CF sputum characteristic as evaluated by rheology, low field NMR and the drug penetration through the mucus via mathematical simulation. These data show that chest physiotherapy has beneficial effects on patients, as it favourably modifies sputum and enhances drug penetration through the respiratory mucus. Graphical abstract

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Polysaccharide-based hydrogels crosslink density equation: A rheological and LF-NMR study of polymer-polymer interactions

Cited by 59 publications

References 66 publications

Effects of the Degree of Phenol Substitution on Molecular Structures and Properties of Chitosan-Phenol-Based Self-Healing Hydrogels

Effects of the Degree of Phenol Substitution on Molecular Structures and Properties of Chitosan-Phenol-Based Self-Healing Hydrogels

Thermosensitive PNIPAM-Based Hydrogel Crosslinked by Composite Nanoparticles as Rapid Wound-Healing Dressings

Effect of chest physiotherapy on cystic fibrosis sputum nanostructure: an experimental and theoretical approach

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