Modelling the interplay between covalent and physical interactions in cyclodextrin-based hydrogel: effect of water confinement

Crupi, V.; Majolino, D.; Rossi, Barbara; Trotta, Francesco; Venuti, Valentina

doi:10.1039/c3sm50827g

Cited by 41 publications

(82 citation statements)

References 34 publications

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“…the gel). 35 This description of swelling phenomena of nanosponges seems to be consistent with the experimental observation [36][37][38] that NS hydrogels undergo the change of their physical state, from a highly viscous gel to a liquid phase, by varying the hydration level or the temperature of the system. Recent HR-MAS NMR experiments 24 revealed that the regime of diffusivity of molecular species in NS hydrogels is modulated both by structural factors (i.e.…”

Section: 40supporting

confidence: 67%

“…35,36,[39][40][41] The separate and complementary investigation of the molecular dynamics of the confined water and nanosponge polymer matrix [39][40][41] revealed that the engaged water molecules turned out to be more liquid-like and less strongly bound to the polymer's functional groups of NS. 40,41 Consequently, the gelation phenomena in NS hydrogels are thought to be driven not only by the formation of hydrogen-bond (HB) networks between water and the hydrophilic groups of polymers, but also by dispersion effects, such as the establishment of non-covalent interactions between the solvent and the more hydrophobic parts of the polymer skeleton.…”

Section: 40mentioning

confidence: 99%

“…Based on previous spectroscopic investigations, 35 a model has been proposed for describing the swelling behaviour that leads to the formation of a NS hydrogel. When NS are brought into contact with the solvent molecules, the latter tends to progressively penetrate into the pores of nanosponges and they are retained inside the covalent polymeric network.…”

Section: 40mentioning

confidence: 99%

“…n = cross-linking agent in molar excess with respect to CD) used in the synthesis of NS. [29][30][31][32][33][34] Moreover, strong experimental evidence has been found that the mechanism of water uptake and the gelling behaviour of NS are intimately connected with the structural arrangement of the polymer network [35][36][37][38] as well as with the balance between hydrophobic and hydrophilic moieties in the chain side groups of the polymer.…”

Section: Introductionmentioning

confidence: 99%

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Toward an understanding of the thermosensitive behaviour of pH-responsive hydrogels based on cyclodextrins

et al. 2015

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The molecular mechanism responsible for the thermosensitive behaviour exhibited by pH-responsive cyclodextrin-based hydrogels is explored here with the twofold aim of clarifying some basic aspects of H-bond interactions in hydrogel phases and contributing to a future engineering of cyclodextrin hydrogels for targeted delivery and release of bioactive agents. The degree of H-bond association of water molecules entrapped in the gel network and the extent of intermolecular interactions involving the hydrophobic/ hydrophilic moieties of the polymer matrix are probed by UV Raman and IR experiments, in order to address the question of how these different and complementary aspects combine to determine the pH-dependent thermal activation exhibited by these hydrogels. Complementary vibrational spectroscopies are conveniently employed in this study with the aim of safely disentangling the spectral response arising from the two main components of the hydrogel systems, i.e. the polymer matrix and water solvent. The experimental evidence suggests that the dominant effects in the mechanism of solvation of cyclodextrin-based hydrogels are due to the changes occurring, upon increasing of temperature, in the hydrophobicity character of specific chemical moieties of the polymer, as triggered by pH variations. The achievements of this work corroborate the potentiality of the UV Raman scattering technique, in combination with more conventional IR experiments, to provide a ''molecular view'' of complex macroscopic phenomena exhibited in hydrogel phases.

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Section: 40supporting

confidence: 67%

Section: 40mentioning

confidence: 99%

Section: 40mentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Toward an understanding of the thermosensitive behaviour of pH-responsive hydrogels based on cyclodextrins

et al. 2015

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“…22,44 The spectral components found in this way for the NS modes (grey colored area in Fig. 4(b)) have been then subtracted from the experimental IR spectra of NSs hydrated with H 2 O, providing the so-called NS-free spectrum.…”

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confidence: 99%

Vibrational signatures of the water behaviour upon confinement in nanoporous hydrogels

Rossi

Venuti

Punta

et al. 2016

Phys. Chem. Chem. Phys.

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The fundamental question of how the reorganization of the hydrogen-bond (HB) network of water is influenced by the combination of nano-confinement and hydrophobic/hydrophilic solvation effects is addressed here using a spectroscopic study of water absorbed in a model, pH-sensitive polysaccharide hydrogel. The effects of temperature, hydration level and pH on the vibrational dynamics associated with the water molecules and the polymer skeleton are disentangled and analysed by a complementary and combined use of UV-Raman scattering and IR spectroscopy. The experimental data give evidence that the solvation effects in the hydrogel matrix are essentially dominated by the hydration of more hydrophobic parts of the polymer network, while the effect of pH on the HB reorganization of confined water molecules is found to be similar to that induced by cooling of the system. A tentative explanation of these results has been provided in terms of interplay between different kinds of interactions, i.e. hydrophobic vs. hydrophilic.

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Cyclodextrin Nanosponges

Swaminathan

Trotta

2019

Nanosponges

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Modelling the interplay between covalent and physical interactions in cyclodextrin-based hydrogel: effect of water confinement

Cited by 41 publications

References 34 publications

Toward an understanding of the thermosensitive behaviour of pH-responsive hydrogels based on cyclodextrins

Toward an understanding of the thermosensitive behaviour of pH-responsive hydrogels based on cyclodextrins

Vibrational signatures of the water behaviour upon confinement in nanoporous hydrogels

Cyclodextrin Nanosponges

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