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Functional Polymer Gels for Advanced Applications in Biomedicine, Energy and Optoelectronics

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A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Polymer Applications".

Deadline for manuscript submissions: closed (20 May 2022) | Viewed by 26922

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Special Issue Editors

Dr. Rebeca Hernandez Velasco

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Guest Editor

Institute of Polymer Science and Technology, (ICTP – CSIC), 28006 Madrid, Spain
Interests: polymers; gels; biomedical applications
Special Issues, Collections and Topics in MDPI journals

Dr. Miryam Criado-Gonzalez

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Guest Editor

Departamento de Nanomateriales Poliméricos y Biomateriales, Instituto de Ciencia y Tecnología de Polímeros (CSIC), C/Juan de la Cierva, 3, 28006 Madrid, Spain
Interests: polymers; gels; biomedical applications

Special Issue Information

Dear Colleagues,

Polymer gels attract a great deal of attention in academia and industry as functional materials capable of responding to external stimuli, such as magnetic fields, temperature, pH, light, electrochemical potentials, and mechanical signals, in a well-controlled manner. Polymer gels are polymer networks crosslinked through physical or chemical bonds able to swell in a solvent. These materials present intermediate properties between those of a solid and a liquid because they combine the characteristic elasticity of solids with the diffusive properties and viscous character of a liquid. In order to enhance the properties of single-network gels, such as swelling/deswelling response or mechanical properties, composite hydrogels (multicomponent hydrogels and interpenetrating polymer networks) arise as innovative matrixes, and they can also offer multifunctionality, attributed to the intrinsic properties of each polymer. Moreover, the incorporation of inorganic nanoparticles (i.e., magnetic iron oxides, gold nanoparticles, and silver nanoparticles, among others) within the polymer gels gives rise to nanocomposite gels with additional functionalities. Progress in the design of functional gels has driven a number of advanced applications such as matrixes for drug release and tissue engineering, actuators and sensors, solid state-electrochemical devices, quasi-solid dye sensitized solar cells or electrochromic displays, to name a few.

The scope of this Special Issue is to address the recent developments and applications of functional gels, including fundamental structure/property relationship, methods of preparation (conventional methods for chemical and physical gelation of macro, micro- and nanogels and gels obtained through 3D printing and bioprinting) and modeling. Special emphasis will be placed on the development of gels for advanced applications in biomedicine, energy, and optoelectronics.

Dr. Rebeca Hernandez Velasco
Dr. Miryam Criado-Gonzalez
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Polymers is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

functional gels
polymers
biomedicine
energy
optoelectronics
microgels
nanogels

Published Papers (6 papers)

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Research

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16 pages, 4226 KiB

Open AccessArticle

Optimization of the Rheological Properties of Self-Assembled Tripeptide/Alginate/Cellulose Hydrogels for 3D Printing

by Alejandro Hernández-Sosa, Rosa Ana Ramírez-Jiménez, Luis Rojo, Fouzia Boulmedais, María Rosa Aguilar, Miryam Criado-Gonzalez and Rebeca Hernández

Polymers 2022, 14(11), 2229; https://doi.org/10.3390/polym14112229 - 30 May 2022

Cited by 24 | Viewed by 3019

Abstract

3D printing is an emerging and powerful technique to create shape-defined three-dimensional structures for tissue engineering applications. Herein, different alginate–cellulose formulations were optimized to be used as printable inks. Alginate (Alg) was chosen as the main component of the scaffold due to its tunable mechanical properties, rapid gelation, and non-toxicity, whereas microcrystalline cellulose (MCC) was added to the hydrogel to modulate its mechanical properties for printing. Additionally, Fmoc-FFY (Fmoc: 9-fluorenylmethoxycarbonyl; F: phenylalanine; Y: tyrosine), a self-assembled peptide that promotes cell adhesion was incorporated into the ink without modifying its rheological properties and shear-thinning behavior. Then, 3D-printed scaffolds made of Alg, 40% of MCC inks and Fmoc-FFY peptide were characterized by scanning electron microscopy and infrared spectroscopy, confirming the morphological microstructure of the hydrogel scaffolds with edged particles of MCC homogeneously distributed within the alginate matrix and the self-assembly of the peptide in a β-sheet conformation. Finally, the cytocompatibility of the scaffolds was tested in contact with the MG63 osteosarcoma cells, confirming the absence of cytotoxic components that may compromise their viability. Interestingly, MG63 cell growth was retarded in the scaffolds containing the peptide, but cells were more likely to promote adhesive interactions with the material rather than with the other cells, indicating the benefits of the peptide in promoting biological functionality to alginate-based biomaterials. Full article

(This article belongs to the Special Issue Functional Polymer Gels for Advanced Applications in Biomedicine, Energy and Optoelectronics)

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23 pages, 4422 KiB

Open AccessEditor’s ChoiceArticle

Elastin-Plasma Hybrid Hydrogels for Skin Tissue Engineering

by Marija Stojic, Joaquín Ródenas-Rochina, María Luisa López-Donaire, Israel González de Torre, Miguel González Pérez, José Carlos Rodríguez-Cabello, Lucy Vojtová, José Luis Jorcano and Diego Velasco

Polymers 2021, 13(13), 2114; https://doi.org/10.3390/polym13132114 - 28 Jun 2021

Cited by 18 | Viewed by 3766

Abstract

Dermo-epidermal equivalents based on plasma-derived fibrin hydrogels have been extensively studied for skin engineering. However, they showed rapid degradation and contraction over time and low mechanical properties which limit their reproducibility and lifespan. In order to achieve better mechanical properties, elasticity and biological properties, we incorporated a elastin-like recombinamer (ELR) network, based on two types of ELR, one modified with azide (SKS-N₃) and other with cyclooctyne (SKS-Cyclo) chemical groups at molar ratio 1:1 at three different SKS (serine-lysine-serine sequence) concentrations (1, 3, and 5 wt.%), into plasma-derived fibrin hydrogels. Our results showed a decrease in gelation time and contraction, both in the absence and presence of the encapsulated human primary fibroblasts (hFBs), higher mechanical properties and increase in elasticity when SKSs content is equal or higher than 3%. However, hFBs proliferation showed an improvement when the lowest SKS content (1 wt.%) was used but started decreasing when increasing SKS concentration at day 14 with respect to the plasma control. Proliferation of human primary keratinocytes (hKCs) seeded on top of the hybrid-plasma hydrogels containing 1 and 3% of SKS showed no differences to plasma control and an increase in hKCs proliferation was observed for hybrid-plasma hydrogels containing 5 wt.% of SKS. These promising results showed the need to achieve a balance between the reduced contraction, the better mechanical properties and biological properties and indicate the potential of using this type of hydrogel as a testing platform for pharmaceutical products and cosmetics, and future work will elucidate their potential. Full article

(This article belongs to the Special Issue Functional Polymer Gels for Advanced Applications in Biomedicine, Energy and Optoelectronics)

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14 pages, 3968 KiB

Open AccessCommunication

Localized Enzyme-Assisted Self-Assembly in the Presence of Hyaluronic Acid for Hybrid Supramolecular Hydrogel Coating

by Jennifer Rodon Fores, Alexis Bigo-Simon, Déborah Wagner, Mathilde Payrastre, Camille Damestoy, Lucille Blandin, Fouzia Boulmedais, Julien Kelber, Marc Schmutz, Morgane Rabineau, Miryam Criado-Gonzalez, Pierre Schaaf and Loïc Jierry

Polymers 2021, 13(11), 1793; https://doi.org/10.3390/polym13111793 - 29 May 2021

Cited by 10 | Viewed by 2937

Abstract

Hydrogel coating is highly suitable in biomaterial design. It provides biocompatibility and avoids protein adsorption leading to inflammation and rejection of implants. Moreover, hydrogels can be loaded with biologically active compounds. In this field, hyaluronic acid has been largely studied as an additional component since this polysaccharide is naturally present in extracellular matrix. Strategies to direct hydrogelation processes exclusively from the surface using a fully biocompatible approach are rare. Herein we have applied the concept of localized enzyme-assisted self-assembly to direct supramolecular hydrogels in the presence of HA. Based on electronic and fluorescent confocal microscopy, rheological measurements and cell culture investigations, this work highlights the following aspects: (i) the possibility to control the thickness of peptide-based hydrogels at the micrometer scale (18–41 µm) through the proportion of HA (2, 5 or 10 mg/mL); (ii) the structure of the self-assembled peptide nanofibrous network is affected by the growing amount of HA which induces the collapse of nanofibers leading to large assembled microstructures underpinning the supramolecular hydrogel matrix; (iii) this changing internal architecture induces a decrease of the elastic modulus from 2 to 0.2 kPa when concentration of HA is increasing; (iv) concomitantly, the presence of HA in supramolecular hydrogel coatings is suitable for cell viability and adhesion of NIH 3T3 fibroblasts. Full article

(This article belongs to the Special Issue Functional Polymer Gels for Advanced Applications in Biomedicine, Energy and Optoelectronics)

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16 pages, 3212 KiB

Open AccessArticle

Chloroaluminate Gel Electrolytes Prepared with Copolymers Based on Imidazolium Ionic Liquids and Deep Eutectic Solvent AlCl₃:Urea

by Jesús L. Pablos, Pilar Tiemblo, Gary Ellis and Teresa Corrales

Polymers 2021, 13(7), 1050; https://doi.org/10.3390/polym13071050 - 27 Mar 2021

Cited by 4 | Viewed by 2713

Abstract

Polymer gel electrolytes (PGEs) have been prepared with copolymers based on imidazolium ionic liquids and the deep eutectic mixture of AlCl₃:urea (uralumina) as liquid electrolyte. The copolymers were synthesized by photopolymerization of vinylpirrolidone or methylmethacrylate with imidazolium bis (trifluoromethane sulfonyl) imide (TFSI) ionic liquid monomer and mixed in an increasing range of wt.% with uralumina. The rheology and electrochemical activity of PGEs were highly dependent on the molar ratio of charged groups and copolymer content. Structure of the PGEs was studied by FTIR and Raman spectroscopy and a correlation between interactions polymer/uralumina and changes in speciation of uralumina was established. Despite the low molecular weight of the copolymers, the resulting polymer electrolytes develop elastomeric character associated with the binding ionic species. Although there is room to improve the electrochemical activity, in this study these new gels provide sufficient electroactivity to make them feasible alternatives as electrolytes in secondary aluminum batteries. Full article

(This article belongs to the Special Issue Functional Polymer Gels for Advanced Applications in Biomedicine, Energy and Optoelectronics)

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Review

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32 pages, 8265 KiB

Open AccessReview

Shaping Macromolecules for Sensing Applications—From Polymer Hydrogels to Foldamers

by Simone Giuseppe Giuffrida, Weronika Forysiak, Pawel Cwynar and Roza Szweda

Polymers 2022, 14(3), 580; https://doi.org/10.3390/polym14030580 - 31 Jan 2022

Cited by 5 | Viewed by 3716

Abstract

Sensors are tools for detecting, recognizing, and recording signals from the surrounding environment. They provide measurable information on chemical or physical changes, and thus are widely used in diagnosis, environment monitoring, food quality checks, or process control. Polymers are versatile materials that find a broad range of applications in sensory devices for the biomedical sector and beyond. Sensory materials are expected to exhibit a measurable change of properties in the presence of an analyte or a stimulus, characterized by high sensitivity and selectivity of the signal. Signal parameters can be tuned by material features connected with the restriction of macromolecule shape by crosslinking or folding. Gels are crosslinked, three-dimensional networks that can form cavities of different sizes and forms, which can be adapted to trap particular analytes. A higher level of structural control can be achieved by foldamers, which are macromolecules that can attain well-defined conformation in solution. By increasing control over the three-dimensional structure, we can improve the selectivity of polymer materials, which is one of the crucial requirements for sensors. Here, we discuss various examples of polymer gels and foldamer-based sensor systems. We have classified and described applied polymer materials and used sensing techniques. Finally, we deliberated the necessity and potential of further exploration of the field towards the increased selectivity of sensory devices. Full article

(This article belongs to the Special Issue Functional Polymer Gels for Advanced Applications in Biomedicine, Energy and Optoelectronics)

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22 pages, 3398 KiB

Open AccessReview

Injectable Hydrogels: From Laboratory to Industrialization

by Jose Maria Alonso, Jon Andrade del Olmo, Raul Perez Gonzalez and Virginia Saez-Martinez

Polymers 2021, 13(4), 650; https://doi.org/10.3390/polym13040650 - 22 Feb 2021

Cited by 77 | Viewed by 8982

Abstract

The transfer of some innovative technologies from the laboratory to industrial scale is many times not taken into account in the design and development of some functional materials such as hydrogels to be applied in the biomedical field. There is a lack of knowledge in the scientific field where many aspects of scaling to an industrial process are ignored, and products cannot reach the market. Injectable hydrogels are a good example that we have used in our research to show the different steps needed to follow to get a product in the market based on them. From synthesis and process validation to characterization techniques used and assays performed to ensure the safety and efficacy of the product, following regulation, several well-defined protocols must be adopted. Therefore, this paper summarized all these aspects due to the lack of knowledge that exists about the industrialization of injectable products with the great importance that it entails, and it is intended to serve as a guide on this area to non-initiated scientists. More concretely, in this work, the characteristics and requirements for the development of injectable hydrogels from the laboratory to industrial scale is presented in terms of (i) synthesis techniques employed to obtain injectable hydrogels with tunable desired properties, (ii) the most common characterization techniques to characterize hydrogels, and (iii) the necessary safety and efficacy assays and protocols to industrialize and commercialize injectable hydrogels from the regulatory point of view. Finally, this review also mentioned and explained a real example of the development of a natural hyaluronic acid hydrogel that reached the market as an injectable product. Full article

(This article belongs to the Special Issue Functional Polymer Gels for Advanced Applications in Biomedicine, Energy and Optoelectronics)

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