The design of supramolecular (SM) hydrogels based on host-guest complexes represents an effective strategy to develop drug delivery systems. In this work, we designed SM hydrogels based on α-cyclodextrin and high-molar mass amphiphilic poly(ether urethane)s (PEUs, ) based on Poloxamer® 407 and differing in their chain extender. The successful formation of poly(pseudo)rotaxanes and their supramolecular interactions were chemically demonstrated. Then, self-healing (80-100% mechanical recovery) supramolecular hydrogels were developed by mixing PEU and α-cyclodextrin solutions at different concentrations. Stability in physiological-like environment and mechanical properties improved with increasing α-cyclodextrin content (9-10% w/v), meanwhile gelation time decreased. A synergistic effect of poly(pseudo)rotaxanes crystals and PEU micellar structures on gel properties was observed: the first were predominant at low PEU concentrations (1-5% w/v), while the latter prevailed at high PEU concentrations (7-9% w/v). Increasing PEU concentration led to gels with increased dissolution rate, not-fully developed networks and slight cytotoxicity, meanwhile residence time in aqueous media improved (>7 d). At low PEU concentrations (1-5% w/v), cytocompatible gels (100% cell viability) were obtained, which maintained their shape in aqueous medium up to 5 d and completely dissolved within 7 d. PEU chemical composition affected PEU/α-cyclodextrin interactions, with longer gelation time and lower mechanical properties in gels based on PEU with pendant functionalities. Gels progressively released a model molecule (fluorescein isothiocyanate-dextran) within 3-4 days with no initial burst release. We thus demonstrated the suitability of custom-made PEUs as constituent of SM hydrogels with α-cyclodextrin and the high potential of the resulting systems for drug delivery applications.

Supramolecular hydrogels based on custom-made poly(ether urethane)s and cyclodextrins as potential drug delivery vehicles: design and characterization / Torchio, Alessandro; Boffito, Monica; Gallina, Andrea; Lavella, Mario; Cassino, Claudio; Ciardelli, Gianluca. - In: JOURNAL OF MATERIALS CHEMISTRY. B. - ISSN 2050-750X. - ELETTRONICO. - 8:34(2020), pp. 7696-7712. [10.1039/d0tb01261k]

Supramolecular hydrogels based on custom-made poly(ether urethane)s and cyclodextrins as potential drug delivery vehicles: design and characterization

Alessandro Torchio;Monica Boffito;Andrea Gallina;Mario Lavella;Gianluca Ciardelli
2020

Abstract

The design of supramolecular (SM) hydrogels based on host-guest complexes represents an effective strategy to develop drug delivery systems. In this work, we designed SM hydrogels based on α-cyclodextrin and high-molar mass amphiphilic poly(ether urethane)s (PEUs, ) based on Poloxamer® 407 and differing in their chain extender. The successful formation of poly(pseudo)rotaxanes and their supramolecular interactions were chemically demonstrated. Then, self-healing (80-100% mechanical recovery) supramolecular hydrogels were developed by mixing PEU and α-cyclodextrin solutions at different concentrations. Stability in physiological-like environment and mechanical properties improved with increasing α-cyclodextrin content (9-10% w/v), meanwhile gelation time decreased. A synergistic effect of poly(pseudo)rotaxanes crystals and PEU micellar structures on gel properties was observed: the first were predominant at low PEU concentrations (1-5% w/v), while the latter prevailed at high PEU concentrations (7-9% w/v). Increasing PEU concentration led to gels with increased dissolution rate, not-fully developed networks and slight cytotoxicity, meanwhile residence time in aqueous media improved (>7 d). At low PEU concentrations (1-5% w/v), cytocompatible gels (100% cell viability) were obtained, which maintained their shape in aqueous medium up to 5 d and completely dissolved within 7 d. PEU chemical composition affected PEU/α-cyclodextrin interactions, with longer gelation time and lower mechanical properties in gels based on PEU with pendant functionalities. Gels progressively released a model molecule (fluorescein isothiocyanate-dextran) within 3-4 days with no initial burst release. We thus demonstrated the suitability of custom-made PEUs as constituent of SM hydrogels with α-cyclodextrin and the high potential of the resulting systems for drug delivery applications.
File in questo prodotto:
File Dimensione Formato  
Paper Supramolecular Hydrogels_accepted paper.pdf

Open Access dal 23/07/2021

Descrizione: accepted paper
Tipologia: 2. Post-print / Author's Accepted Manuscript
Licenza: PUBBLICO - Tutti i diritti riservati
Dimensione 4.22 MB
Formato Adobe PDF
4.22 MB Adobe PDF Visualizza/Apri
d0tb01261k1.pdf

accesso aperto

Descrizione: supplementary material
Tipologia: Altro materiale allegato
Licenza: PUBBLICO - Tutti i diritti riservati
Dimensione 272.6 kB
Formato Adobe PDF
272.6 kB Adobe PDF Visualizza/Apri
authorreprints.pdf

non disponibili

Descrizione: versione editoriale
Tipologia: 2a Post-print versione editoriale / Version of Record
Licenza: Non Pubblico - Accesso privato/ristretto
Dimensione 5.32 MB
Formato Adobe PDF
5.32 MB Adobe PDF   Visualizza/Apri   Richiedi una copia
Pubblicazioni consigliate

I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.

Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11583/2843832