Hybrid supramolecular gels of Fmoc-F/halloysite nanotubes: systems for sustained release of camptothecin

Author(s): C. Rizzo ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵ , R. Arrigo ⁶ ^, ⁷ ^, ³ ^, ⁴ ^, ⁵ , F. D'Anna ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵ , F. Di Blasi ⁸ ^, ⁹ ^, ¹⁰ ^, ¹¹ ^, ⁵ , N. T. Dintcheva ⁶ ^, ⁷ ^, ³ ^, ⁴ ^, ⁵ , G. Lazzara ¹² ^, ³ ^, ⁴ ^, ⁵ , F. Parisi ¹² ^, ³ ^, ⁴ ^, ⁵ , S. Riela ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵ , G. Spinelli ⁸ ^, ⁹ ^, ¹⁰ ^, ¹¹ ^, ⁵ , M. Massaro ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵

Publication date (Electronic): 2017

Journal: Journal of Materials Chemistry B

Publisher: Royal Society of Chemistry (RSC)

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Abstract

Novel supramolecular gel hybrids were prepared by self-assembly of Fmoc- l-phenylalanine in the presence of functionalized halloysite nanotubes and employed as carriers for the delivery of camptothecin molecules.

Abstract

Supramolecular gel hybrids obtained by self-assembly of Fmoc- l-phenylalanine (Fmoc-F) in the presence of functionalized halloysite nanotubes (f-HNT) were obtained in biocompatible solvents and employed as carriers for the delivery of camptothecin (CPT) molecules. The synthesis of the new f-HNT material as well as its characterization are described. The properties of the hybrid hydrogels and organogels were analyzed by several techniques. The presence of small amounts of f-HNT allows good dispersion of the tubes and the subsequent formation of homogeneous gels. The experimental results show that f-HNT functions only as an additive in the hybrid gels and does not demonstrate gelator behavior. The in vitro kinetic release from both f-HNT/CPT and Fmoc-F/f-HNT/CPT was studied in media that imitates physiological conditions, and the factors controlling the release process were determined and discussed. Furthermore, the antiproliferative in vitro activities of the gels were evaluated towards human cervical cancer HeLa cells. A comparison of data collected in both systems shows the synergistic action of f-HNT and the gel matrix in controlling the release of CPT in the media and maintaining the drug in its active form. Finally, a comparison with pristine HNT is also reported. This study suggests a suitable strategy to obtain two-component gel hybrids based on nanocarriers with controlled drug carrier capacity for biomedical applications.

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Supramolecular Hydrogelators and Hydrogels: From Soft Matter to Molecular Biomaterials

Xuewen Du, Jie Zhou, Junfeng Shi … (2015)

In this review we intend to provide a relatively comprehensive summary of the work of supramolecular hydrogelators after 2004 and to put emphasis particularly on the applications of supramolecular hydrogels/hydrogelators as molecular biomaterials. After a brief introduction of methods for generating supramolecular hydrogels, we discuss supramolecular hydrogelators on the basis of their categories, such as small organic molecules, coordination complexes, peptides, nucleobases, and saccharides. Following molecular design, we focus on various potential applications of supramolecular hydrogels as molecular biomaterials, classified by their applications in cell cultures, tissue engineering, cell behavior, imaging, and unique applications of hydrogelators. Particularly, we discuss the applications of supramolecular hydrogelators after they form supramolecular assemblies but prior to reaching the critical gelation concentration because this subject is less explored but may hold equally great promise for helping address fundamental questions about the mechanisms or the consequences of the self-assembly of molecules, including low molecular weight ones. Finally, we provide a perspective on supramolecular hydrogelators. We hope that this review will serve as an updated introduction and reference for researchers who are interested in exploring supramolecular hydrogelators as molecular biomaterials for addressing the societal needs at various frontiers.

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Eric A Appel, Jesús del Barrio, Xian Loh … (2012)

The supramolecular crosslinking of polymer chains in water by specific, directional and dynamic non-covalent interactions has led to the development of novel supramolecular polymeric hydrogels. These aqueous polymeric networks constitute an interesting class of soft materials exhibiting attractive properties such as stimuli-responsiveness and self-healing arising from their dynamic behaviour and that are crucial for a wide variety of emerging applications. We present here a critical review summarising the formation of dynamic polymeric networks through specific non-covalent interactions, with a particular emphasis on those systems based on host-guest complex formation, as well as the characterisation of their physical characteristics. Aqueous supramolecular chemistry has unlocked a versatile toolbox for the design and fine-tuning of the material properties of these hydrogels (264 references).