Evaluation of the Accessibility of Molecules in Hydrogels Using a Scale of Spin Probes

In this work, we explored by means of electron paramagnetic resonance (EPR) spectroscopy the accessibility of a series of spin probes, covering a scale of molecular weights in the range of 200–60,000 Da, in a variety of hydrogels: covalent network, ionotropic, interpenetrating polymer network (IPN)...

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Main Authors: Iulia Matei, Ana-Maria Ariciu, Elena Irina Popescu, Sorin Mocanu, Alexandru Vincentiu Florian Neculae, Florenta Savonea, Gabriela Ionita
Format: Article
Language:English
Published: MDPI AG 2022-07-01
Series:Gels
Subjects:
Online Access:https://www.mdpi.com/2310-2861/8/7/428
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author Iulia Matei
Ana-Maria Ariciu
Elena Irina Popescu
Sorin Mocanu
Alexandru Vincentiu Florian Neculae
Florenta Savonea
Gabriela Ionita
author_facet Iulia Matei
Ana-Maria Ariciu
Elena Irina Popescu
Sorin Mocanu
Alexandru Vincentiu Florian Neculae
Florenta Savonea
Gabriela Ionita
author_sort Iulia Matei
collection DOAJ
description In this work, we explored by means of electron paramagnetic resonance (EPR) spectroscopy the accessibility of a series of spin probes, covering a scale of molecular weights in the range of 200–60,000 Da, in a variety of hydrogels: covalent network, ionotropic, interpenetrating polymer network (IPN) and semi-IPN. The covalent gel network consists of polyethylene or polypropylene chains linked <i>via</i> isocyanate groups with cyclodextrin, and the ionotropic gel is generated by alginate in the presence of Ca<sup>2+</sup> ions, whereas semi-IPN and IPN gel networks are generated in a solution of alginate and chitosan by adding crosslinking agents, Ca<sup>2+</sup> for alginate and glutaraldehyde for chitosan. It was observed that the size of the diffusing species determines the ability of the gel to uptake them. Low molecular weight compounds can diffuse into the gel, but when the size of the probes increases, the gel cannot uptake them. Spin-labelled Pluronic F127 cannot be encapsulated by any covalent gel, whereas spin-labelled albumin can diffuse in alginate gels and in most of the IPN networks. The EPR spectra also evidenced the specific interactions of spin probes inside hydrogels. The results suggest that EPR spectroscopy can be an alternate method to evaluate the mesh size of gel systems and to provide information on local interactions inside gels.
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spelling doaj.art-c9745360f64640aa86d49ec072b4cfc62023-11-30T23:13:38ZengMDPI AGGels2310-28612022-07-018742810.3390/gels8070428Evaluation of the Accessibility of Molecules in Hydrogels Using a Scale of Spin ProbesIulia Matei0Ana-Maria Ariciu1Elena Irina Popescu2Sorin Mocanu3Alexandru Vincentiu Florian Neculae4Florenta Savonea5Gabriela Ionita6“Ilie Murgulescu” Institute of Physical Chemistry of the Romanian Academy, 202 Splaiul Independentei, 060021 Bucharest, RomaniaIPG Health Consulting, King Edward Street, Macclesfield SK19 1AQ, UK“Ilie Murgulescu” Institute of Physical Chemistry of the Romanian Academy, 202 Splaiul Independentei, 060021 Bucharest, Romania“Ilie Murgulescu” Institute of Physical Chemistry of the Romanian Academy, 202 Splaiul Independentei, 060021 Bucharest, Romania“Ilie Murgulescu” Institute of Physical Chemistry of the Romanian Academy, 202 Splaiul Independentei, 060021 Bucharest, Romania“Ilie Murgulescu” Institute of Physical Chemistry of the Romanian Academy, 202 Splaiul Independentei, 060021 Bucharest, Romania“Ilie Murgulescu” Institute of Physical Chemistry of the Romanian Academy, 202 Splaiul Independentei, 060021 Bucharest, RomaniaIn this work, we explored by means of electron paramagnetic resonance (EPR) spectroscopy the accessibility of a series of spin probes, covering a scale of molecular weights in the range of 200–60,000 Da, in a variety of hydrogels: covalent network, ionotropic, interpenetrating polymer network (IPN) and semi-IPN. The covalent gel network consists of polyethylene or polypropylene chains linked <i>via</i> isocyanate groups with cyclodextrin, and the ionotropic gel is generated by alginate in the presence of Ca<sup>2+</sup> ions, whereas semi-IPN and IPN gel networks are generated in a solution of alginate and chitosan by adding crosslinking agents, Ca<sup>2+</sup> for alginate and glutaraldehyde for chitosan. It was observed that the size of the diffusing species determines the ability of the gel to uptake them. Low molecular weight compounds can diffuse into the gel, but when the size of the probes increases, the gel cannot uptake them. Spin-labelled Pluronic F127 cannot be encapsulated by any covalent gel, whereas spin-labelled albumin can diffuse in alginate gels and in most of the IPN networks. The EPR spectra also evidenced the specific interactions of spin probes inside hydrogels. The results suggest that EPR spectroscopy can be an alternate method to evaluate the mesh size of gel systems and to provide information on local interactions inside gels.https://www.mdpi.com/2310-2861/8/7/428polymeric gelsdiffusionEPR spectroscopynitroxides
spellingShingle Iulia Matei
Ana-Maria Ariciu
Elena Irina Popescu
Sorin Mocanu
Alexandru Vincentiu Florian Neculae
Florenta Savonea
Gabriela Ionita
Evaluation of the Accessibility of Molecules in Hydrogels Using a Scale of Spin Probes
Gels
polymeric gels
diffusion
EPR spectroscopy
nitroxides
title Evaluation of the Accessibility of Molecules in Hydrogels Using a Scale of Spin Probes
title_full Evaluation of the Accessibility of Molecules in Hydrogels Using a Scale of Spin Probes
title_fullStr Evaluation of the Accessibility of Molecules in Hydrogels Using a Scale of Spin Probes
title_full_unstemmed Evaluation of the Accessibility of Molecules in Hydrogels Using a Scale of Spin Probes
title_short Evaluation of the Accessibility of Molecules in Hydrogels Using a Scale of Spin Probes
title_sort evaluation of the accessibility of molecules in hydrogels using a scale of spin probes
topic polymeric gels
diffusion
EPR spectroscopy
nitroxides
url https://www.mdpi.com/2310-2861/8/7/428
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