Combining thermosensitive physical self-assembly and covalent cycloaddition chemistry as simultaneous dual cross-linking mechanisms for the preparation of injectable hydrogels with tuneable properties

Yan, Jie; Krasowska, Marta; Ge, Wei; Platts, Kirsten; Marina, Paula Facal; Blencowe, Anton

doi:10.1016/j.eurpolymj.2022.111761

Cited by 7 publications

(4 citation statements)

References 74 publications

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“…According to Siepmann [70], the apparent diffusivity of the active component can be calculated using Equation (4). Since it is an equation that derives from the Higuchi model (Equation ( 3)), Table 2 shows the adjustment parameters of both.…”

Section: Carvacrol Release Kineticsmentioning

confidence: 99%

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Rheological Study of the Formation of Pullulan Hydrogels and Their Use as Carvacrol-Loaded Nanoemulsion Delivery Systems

Santamaría

Barros

González

et al. 2023

Gels

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Hydrogels have been extensively studied as delivery systems for lipophilic compounds. Pullulan hydrogels were prepared, and their gelation kinetics were studied over time. Pullulan exhibited a relatively slow gelling reaction in basic medium (KOH) using trisodium metaphosphate (STMP) as a cross-linking agent, so capsules cannot be obtained by dripping as easily as in the case of alginate and chitosan. The kinetics of pullulan gelation were studied through rheological analysis over time. An optimal [Pullulan]/[KOH] ratio was found for a fixed [Pullulan]/[STMP] ratio. For this given relationship, gelling time measurements indicated that when the concentration of pullulan increased, the gelation time decreased from 60 min for 6% w/w pullulan to 10 min for 10% w/w. After the gel point, a hardening of the hydrogel was observed over the next 5 h. The formed hydrogels presented high degrees of swelling (up to 1800%). Freeze-dried gels were capable of being rehydrated, obtaining gels with rheological characteristics and visual appearance similar to fresh gels, which makes them ideal to be freeze-dried for storage and rehydrated when needed. The behavior of the hydrogels obtained as active ingredient release systems was studied. In this case, the chosen molecule was carvacrol (the main component of oregano oil). As carvacrol is hydrophobic, it was incorporated into the droplets of an oil-in-water nanoemulsion, and the nanoemulsion was incorporated into the hydrogel. The release of the oil was studied at different pHs. It was observed that as the pH increased (from pH 2 to pH 7), the released amount of carvacrol for the gel with pullulan 10% w/w reached 100%; for the other cases, the cumulative release amount was lower. It was attributed to two opposite phenomena in the porous structure of the hydrogel, where more porosity implied a faster release of carvacrol but also a higher degree of swelling that promoted a higher entry of water flow in the opposite direction. This flow of water prevented the active principle from spreading to the release medium.

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Section: Carvacrol Release Kineticsmentioning

confidence: 99%

“…The properties of physically cross-linked hydrogels depend on their molecular structure, their synthesis [ 2 ], and their cross-linking density. If the cross-linking density of a cross-linked hydrogel is very high, it becomes brittle and shows poor mechanical properties [ 3 , 4 ].…”

Section: Introductionmentioning

confidence: 99%

Rheological Study of the Formation of Pullulan Hydrogels and Their Use as Carvacrol-Loaded Nanoemulsion Delivery Systems

Santamaría

Barros

González

et al. 2023

Gels

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“…Currently, local drug delivery systems demonstrate benefits in terms of tumor drug accumulation and regulated drug release. , Among them, localized drug delivery platforms have the capability to establish drug reservoirs at the tumor area, enabling sustained and controlled release of loaded drugs over an extended duration. As a result, these systems effectively impede tumor growth. , In situ hydrogels, especially temperature-sensitive hydrogels, have good fluidity and can be directly injected into or around tumors. − The transformation from liquid to gel under the action of body temperature can well cover the tumor tissue on the one hand and prolong the local residence time of the drug on the other hand, forming a high-concentration drug reservoir. , Therefore, local drug delivery systems combining injectable hydrogels with nanomedicines are expected to produce synergistic effects, which are of great significance for tumor therapy. ,, …”

Section: Introductionmentioning

confidence: 99%

Thermo-Sensitive Nanoparticle-Hydrogel Composite Based on Pluronic F127 and Phycocyanin for an Enhanced Chemo-Photodynamic Antitumor Effect

Song

Zhang

et al. 2023

ACS Appl. Polym. Mater.

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The concurrent utilization of chemotherapy and photodynamic therapy (PDT) can successfully slow the growth of tumors while minimizing systemic toxicity. An injectable temperature-sensitive hydrogel was constructed based on Pluronic F127 and phycocyanin (PC). Nanoparticles formed by self-assembly of doxorubicin and ursolic acid (DOX–UA NPS) were further loaded into the hydrogel to give a local drug delivery platform (DOX–UA NPs@Gel). DOX–UA NPs@Gel can be enriched in situ in tumors and continuously release DOX–UA NPs and free PC. UA can promote the responsiveness of tumor cells to DOX. As a natural photosensitizer, PC can produce reactive oxygen species (ROS) when exposed to laser radiation and has significant PDT activity. The MTT assay demonstrated that DOX–UA NPs@Gel under irradiation caused the highest cytotoxicity at 91.6%. The anti-tumor efficiency of various nanoparticles and nanoparticle-loaded hydrogels (the injection dose of DOX is 6 mg/kg) was verified in the H22 tumor-bearing mice (male ICR). In vivo antitumor results demonstrated that DOX–UA NPs@Gel with the combination of chemotherapy and PDT exhibited unique anticancer efficacy with low toxicity. When exposed to radiation after the experiment, the DOX–UA NPs@Gel showed a tumor volume of merely 319 mm3, displaying an exceptional tumor growth inhibition rate of 91.05%. Therefore, the local drug delivery system based on the thermosensitive hydrogel can effectively achieve synergistic antitumor effects.

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“…They can also be functionalized with growth factors to stimulate the growth of cells and support tissue repair and regeneration. Another key feature of these systems is their capability to be used as bioinks for 3D bioprinting techniques in order to create complex shapes or hybrid systems in combination with other polymers [24,25] and their possibility of being designed even at the nanoscale [26]. In this respect, hydrogels are so versatile because by varying the chemical composition and material types, the molecular weight and crosslinking degree and the solid contents and functionalization, they can be used to mimic the mechanical behavior of the IVD [27][28][29].…”

Section: Introductionmentioning

confidence: 99%

Polymeric Hydrogels for Intervertebral Disc Replacement/Integration: Playing with the Chemical Composition for Tuning Shear Behavior and Hydrophilicity

Maniglio,

Bissoli,

Callone

et al. 2023

Gels

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Damages to the intervertebral disc (IVD) due to improper loading or degeneration result in back pain, which is a common disease affecting an increasing number of patients. Different strategies for IVD remediation have been developed, from surgical treatment to disc replacement, by using both metallic and non-metallic materials. Hydrogels are very attractive materials due to their ability to simulate the properties of many soft tissues; moreover, their chemical composition can be varied in order to assure performances similar to the natural disc. In particular, for the replacement of the IVD outer ring, namely, the anulus fibrosus, the shear properties are of paramount importance. In this work, we produced hydrogels through the photo-induced crosslinking of different mixtures composed of two hydrophilic monofunctional and difunctional polymers, namely, poly(ethyleneglycol) methyl ether methacrylate (PEGMEMA) and poly(ethyleneglycol) dimethacrylate (PEGDMA), together with a hydrophobic molecule, i.e., tert-butyl acrylate (tBA). By changing the ratio among the precursors, we demonstrated the tunability of both the shear properties and hydrophilicity. The structural properties of hydrogels were studied by solid-state nuclear magnetic resonance (NMR). These experiments provided insights on both the structure and molecular dynamics of polymeric networks and, together with information obtained by differential scanning calorimetry (DSC), allowed for correlating the physical properties of the hydrogels with their chemical composition.

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Combining thermosensitive physical self-assembly and covalent cycloaddition chemistry as simultaneous dual cross-linking mechanisms for the preparation of injectable hydrogels with tuneable properties

Cited by 7 publications

References 74 publications

Rheological Study of the Formation of Pullulan Hydrogels and Their Use as Carvacrol-Loaded Nanoemulsion Delivery Systems

Rheological Study of the Formation of Pullulan Hydrogels and Their Use as Carvacrol-Loaded Nanoemulsion Delivery Systems

Thermo-Sensitive Nanoparticle-Hydrogel Composite Based on Pluronic F127 and Phycocyanin for an Enhanced Chemo-Photodynamic Antitumor Effect

Polymeric Hydrogels for Intervertebral Disc Replacement/Integration: Playing with the Chemical Composition for Tuning Shear Behavior and Hydrophilicity

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