Inputs of Macromolecular Engineering in the Design of Injectable Hydrogels Based on Synthetic Thermoresponsive Polymers

Perreten, Vincent; Trimaille, Thomas; Gigmès, Didier

doi:10.1021/acs.macromol.9b00705

Cited by 22 publications

(26 citation statements)

References 105 publications

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“…Hydrogels are three-dimensional (3D) polymer networks that hold large amounts of water. − This feature allows the encapsulation of active molecules and/or cells and the exchange of nutrients and metabolites. , Among them, injectable and biodegradable hydrogels have gained particular attention because of the minimally invasive treatment manner and have been widely investigated for drug delivery, − tissue regeneration, − 3D cell culture, , wound healing, postsurgical antiadhesion, and so on. , Thermosensitive hydrogels that undergo sol–gel transitions upon heating are an important class of injectable systems. ,,− Their low-viscous sol state at low temperatures facilitates the incorporation of fragile drugs and cells through simple mixing, and this low-temperature loading procedure advantageously protects the activity of fragile agents, such as proteins or polypeptides, and the viability of cells. After the liquid formulation was injected into the body, an in situ gel matrix for drug delivery or cell growth was spontaneously generated.…”

Section: Introductionmentioning

confidence: 99%

Decisive Influence of Hydrophobic Side Chains of Polyesters on Thermoinduced Gelation of Triblock Copolymer Aqueous Solutions

Chen

et al. 2021

Macromolecules

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A series of amphiphilic triblock copolymers composed of poly(ethylene glycol) (PEG) and poly(ε-caprolactone-co-5-alkyl δlactone)s bearing distinct alkyl side groups were synthesized via ringopening copolymerization of ε-caprolactone and a small amount of various 5-alkyl δ-lactones using PEG as the macroinitiator and metalfree diphenyl phosphate as the catalyst. The analysis of 1 H NMR, GPC, DSC, and XRD confirmed that the synthetic copolymers had similar molecular weights and bulk properties; nevertheless, they exhibited quite different aqueous behaviors in response to temperature variations. While the polyesters without side chains simply presented a free-flowing sol over the entire examined temperature range, those bearing methyl or n-propyl side groups underwent a sol−gel transition upon heating and harvested a reversed thermosensitive hydrogel (T-Gel). Meanwhile, the sol−gel transition temperature of the polymer/water system could be easily tailored by adjusting the content of the n-propyl side group. In contrast, the polyesters containing longer n-amyl side groups formed a normal hydrogel (N-Gel) exhibiting a gel−sol (suspension) transition upon heating. Their different aqueous behaviors stemmed from the difference in the hydrophilic−hydrophobic equilibrium of the amphiphilic copolymers. The sol−gel transitions of the thermosensitive hydrogels were attributed to the aggregation of micelles and the dehydration of PEG. The copolymers bearing n-propyl side groups had good cytocompatibility and were fairly stable in a phosphate buffered saline for 80 days, whereas the formed thermosensitive hydrogel (20 wt %) was rapidly degraded via surface erosion within half a month after subcutaneous injection into mice. Consequently, this study indicates that subtle variation in the length of hydrophobic side chains plays a decisive role in the physical gelation of PEG/polyester copolymers. In addition, the thermosensitive hydrogels have the potential for drug and cell delivery based on their good biocompatibility and biodegradability.

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Section: Introductionmentioning

confidence: 99%

Decisive Influence of Hydrophobic Side Chains of Polyesters on Thermoinduced Gelation of Triblock Copolymer Aqueous Solutions

Chen

et al. 2021

Macromolecules

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“…Besides the most structurally simple polymers, like PEG, polymers that contain a functional side group come in hand for post-polymerization coupling of biomolecules or for the formation of chemical or physical cross-links within the hydrogel network. This approach involves the polymerization of monomers that bear a functional group that will not be attacked or degraded during the polymerization, but can then be modified and reacted afterwards [ 124 , 125 ]. Representative examples include PAAc and its analogues, polyamines and analogues, and poly(NHS) esters.…”

Section: Synthetic Criteria For Hydrogel Productionmentioning

confidence: 99%

Design of Bio-Conjugated Hydrogels for Regenerative Medicine Applications: From Polymer Scaffold to Biomolecule Choice

et al. 2020

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Bio-conjugated hydrogels merge the functionality of a synthetic network with the activity of a biomolecule, becoming thus an interesting class of materials for a variety of biomedical applications. This combination allows the fine tuning of their functionality and activity, whilst retaining biocompatibility, responsivity and displaying tunable chemical and mechanical properties. A complex scenario of molecular factors and conditions have to be taken into account to ensure the correct functionality of the bio-hydrogel as a scaffold or a delivery system, including the polymer backbone and biomolecule choice, polymerization conditions, architecture and biocompatibility. In this review, we present these key factors and conditions that have to match together to ensure the correct functionality of the bio-conjugated hydrogel. We then present recent examples of bio-conjugated hydrogel systems paving the way for regenerative medicine applications.

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“…The PNIPAM enrichment with the 10 mol% with the hydrophobic NtBAM provides some advantages, namely, regulation of the LCST [ 36 ] and in turn the gelation temperature and strengthening of the hydrophobic interactions responsible for the formation of the network crosslinks. The synergy of both thermo- and shear-responsiveness rendered this hydrogel with promising injectable self-assembling capability [ 37 ] that has great potential to be used in bioapplications.…”

Section: Introductionmentioning

confidence: 99%

pH/Thermo-Responsive Grafted Alginate-Based SiO2 Hybrid Nanocarrier/Hydrogel Drug Delivery Systems

et al. 2021

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We report the preparation of mesoporous silica nanoparticles covered by layer by layer (LbL) oppositely charged weak polyelectrolytes, comprising poly(allylamine hydrochloride) (PAH) and a sodium alginate, highly grafted by N-isopropylacrylamide/N-tert-butylacrylamide random copolymers, NaALG-g-P(NIPAM90-co-NtBAM10) (NaALG-g). Thanks to the pH dependence of the degree of ionization of the polyelectrolytes and the LCST-type thermosensitivity of the grafting chains of the NaALG-g, the as-prepared hybrid nanoparticles (hNP) exhibit pH/thermo-responsive drug delivery capabilities. The release kinetics of rhodamine B (RB, model drug) can be controlled by the number of PAH/NaALG-g bilayers and more importantly by the environmental conditions, namely, pH and temperature. As observed, the increase of pH and/or temperature accelerates the RB release under sink conditions. The same NaALG-g was used as gelator to fabricate a hNP@NaALG-g hydrogel composite. This formulation forms a viscous solution at room temperature, and it is transformed to a self-assembling hydrogel (sol-gel transition) upon heating at physiological temperature provided that its Tgel was regulated at 30.7 °C, by the NtBAM hydrophobic monomer incorporation in the side chains. It exhibits excellent injectability thanks to its combined thermo- and shear-responsiveness. The hNP@NaALG-g hydrogel composite, encapsulating hNP covered with one bilayer, exhibited pH-responsive sustainable drug delivery. The presented highly tunable drug delivery system (DDS) (hNP and/or composite hydrogel) might be useful for biomedical potential applications.

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Inputs of Macromolecular Engineering in the Design of Injectable Hydrogels Based on Synthetic Thermoresponsive Polymers

Cited by 22 publications

References 105 publications

Decisive Influence of Hydrophobic Side Chains of Polyesters on Thermoinduced Gelation of Triblock Copolymer Aqueous Solutions

Decisive Influence of Hydrophobic Side Chains of Polyesters on Thermoinduced Gelation of Triblock Copolymer Aqueous Solutions

Design of Bio-Conjugated Hydrogels for Regenerative Medicine Applications: From Polymer Scaffold to Biomolecule Choice

pH/Thermo-Responsive Grafted Alginate-Based SiO2 Hybrid Nanocarrier/Hydrogel Drug Delivery Systems

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