Unraveling the gallol-driven assembly mechanism of thermoreversible supramolecular hydrogels inspired by ascidians

Wolfel, Alexis; Euti, Esteban M.; Picchio, Matías L.; Romero, Marcelo Ricardo; Josa, Víctor M. Galván; Martinelli, Marisa; Minari, Roque Javier; Igarzabal, Cecilia Inés Álvarez

doi:10.1039/d0py01036g

Cited by 15 publications

(19 citation statements)

References 55 publications

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“…In previous studies, the mechanical and rheological properties of the supramolecular hydrogels have been demonstrated, indicating a dependence on their chemical composition. , For example, the thermoreversible gel–sol phase transition of PVA/PC hydrogels can be tuned by the concentration and nature of the phenolic molecule. , Therefore, it is of interest in the present work to evaluate the effect of the Au NPs on the rheological properties of the supramolecular PVA–GA gels. The DMTA results are shown in Figure S3.…”

Section: Results and Discussionmentioning

confidence: 95%

“…The formation of supramolecular gels from PVA and GA was previously described. , These thermoreversible materials were easily prepared through a one-pot hot-dissolution/cooling step. The formation of dynamic interactions between the polymer and GA allows the arrangement of the structure to form a supramolecular network with outstanding viscoelastic and mechanical properties.…”

Section: Results and Discussionmentioning

confidence: 99%

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In Situ Preparation of Plasmonic Gold Nanoparticle-Supramolecular Hydrogel Nanocomposites with Tunable Optical Properties: Correlating Theory and Experiments

et al. 2022

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Supramolecular plasmonic polymer nanocomposites are versatile soft materials that hold great promise for many bioapplications as they combine the functional properties of inorganic nanoparticles with the dynamic nature of the polymer matrix. Herein, we exploited the supramolecular chemistry and reducing properties of plant-derived gallic acid (GA) to drive the in situ formation of gold nanoparticles (Au NPs) into poly(vinyl alcohol) (PVA)–GA hydrogels. The size and shape of Au NPs in the plasmonic nanocomposites were tuned from 25 to 221 nm and from anisotropic to spherical, respectively, varying the Au3+ concentration. From experimental and theoretical simulation of the extinction spectra, it was possible to assess the change of the average refractive index of the surrounding Au NPs in two Au3+ concentration regimes. The changes of the chemical environment were also tested by Raman and infrared spectroscopy characterization. Furthermore, the viscoelastic behavior of the supramolecular PVA–GA hydrogel was also investigated for the plasmonic nanocomposites. At the highest concentration investigated, the formation of Au NP aggregates (dimers and trimers) was observed and rationalized with electrodynamic simulations. Finally, the surface-enhanced Raman spectroscopy properties were also analyzed using Rhodamine 6G, revealing the extraordinary capacity of these materials for their application as sensing platforms.

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Section: Results and Discussionmentioning

confidence: 95%

Section: Results and Discussionmentioning

confidence: 99%

In Situ Preparation of Plasmonic Gold Nanoparticle-Supramolecular Hydrogel Nanocomposites with Tunable Optical Properties: Correlating Theory and Experiments

et al. 2022

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“…[38] Hydrogen-bonded hydrogels with the ability to selfheal include gelators based on ureidopyrimidinones (Figure 4), gallol and benzene-1,3,5-tricarboxamide. [9,39,40] Different selfhealing hydrogels can be prepared separately and mixed to form a multi-gel scaffold. In this way, a single scaffold is able to coculture multiple cell types to differentiate and proliferate, as the hydrogel may have regions with different mechanical properties.…”

Section: Connections Through Hydrogen Bondingmentioning

confidence: 99%

“…Self‐healing hydrogelators feature a much higher number of repeating motifs capable of reversible, multisite bonding [38] . Hydrogen‐bonded hydrogels with the ability to self‐heal include gelators based on ureidopyrimidinones (Figure 4), gallol and benzene‐1,3,5‐tricarboxamide [9,39,40] . Different self‐healing hydrogels can be prepared separately and mixed to form a multi‐gel scaffold.…”

Section: Supramolecular Interactions and Design Considerationsmentioning

confidence: 99%

Supramolecular Hydrogels: Design Strategies and Contemporary Biomedical Applications

Omar

Ponsford

Dreiss

et al. 2022

Chemistry An Asian Journal

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Self‐assembly of supramolecular hydrogels is driven by dynamic, non‐covalent interactions between molecules. Considerable research effort has been exerted to fabricate and optimise supramolecular hydrogels that display shear‐thinning, self‐healing, and reversibility, in order to develop materials for biomedical applications. This review provides a detailed overview of the chemistry behind the dynamic physicochemical interactions that sustain hydrogel formation (hydrogen bonding, hydrophobic interactions, ionic interactions, metal‐ligand coordination, and host‐guest interactions). Novel design strategies and methodologies to create supramolecular hydrogels are highlighted, which offer promise for a wide range of applications, specifically drug delivery, wound healing, tissue engineering and 3D bioprinting. To conclude, future prospects are briefly discussed, and consideration given to the steps required to ultimately bring these biomaterials into clinical settings.

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“…(C) The DOPA content of the five specific mussel proteins. (D) The catechol content of the polymer with catechol groups 34–38.…”

Section: Mussel Protein and Adhesion Mechanismmentioning

confidence: 99%

Mussel‐inspired polymer materials derived from nonphytogenic and phytogenic catechol derivatives and their applications

Wang

Zhang

et al. 2021

Polymer International

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When it comes to underwater adhesion, mussel is the true expert that can firmly attach onto wet rocks under dynamic and turbulent environments. Catechol‐like 3,4‐dihydroxyphenylalanine and its biochemical interactions have been largely implicated in mussels' strong adhesion to various substrates. We successfully determined that a copolymerization polymer molecule could be designed according to the catechol structural features and that high‐performance biomimetic mussel materials can be prepared from petrochemical materials or renewable materials, and because of their excellent performance in various application areas show a broad application prospect. The adhesion mechanism of the mussel protein and the recent advances in biomimetic mussel protein polymers based on nonphytogenic catechol derivatives and phytogenic catechol derivatives from different sources are comprehensively summarized. By comparing the application of nonphytogenic catechol derivatives and phytogenic catechol derivatives in industrial and biomedical fields, we found that the synthesis of phytogenic catechol derivatives is more facile and universal, and their application performance is as good as that of nonphytogenic catechol derivatives. In addition, the challenges and prospects for this field in the future are also discussed. © 2021 Society of Industrial Chemistry.

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Unraveling the gallol-driven assembly mechanism of thermoreversible supramolecular hydrogels inspired by ascidians

Abstract: Polyphenol-based supramolecular hydrogels have recently attracted much attention as smart materials for applications in several technologies. Although great advances have been made in this field, there is a challenging need...

Cited by 15 publications

References 55 publications

In Situ Preparation of Plasmonic Gold Nanoparticle-Supramolecular Hydrogel Nanocomposites with Tunable Optical Properties: Correlating Theory and Experiments

In Situ Preparation of Plasmonic Gold Nanoparticle-Supramolecular Hydrogel Nanocomposites with Tunable Optical Properties: Correlating Theory and Experiments

Supramolecular Hydrogels: Design Strategies and Contemporary Biomedical Applications

Mussel‐inspired polymer materials derived from nonphytogenic and phytogenic catechol derivatives and their applications

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