Design of Supramolecular Hydrogels

A special issue of Gels (ISSN 2310-2861). This special issue belongs to the section "Gel Processing and Engineering".

Deadline for manuscript submissions: 15 April 2025 | Viewed by 2235

Special Issue Editors


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Guest Editor
Department of Chemistry, Science Institute, University of Iceland, Dunhagi 3, 107 Reykjavík, Iceland
Interests: supramolecular gel; peptide hydrogel; metallogel; X-ray crystallography; antibacterial activity

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Guest Editor
School of Chemistry, Joseph Banks Laboratories, University of Lincoln, Lincoln LN6 7TS, UK
Interests: supramolecular chemistry

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Guest Editor
Department of Chemistry, University of Jyvaskyla, 40014 Jyväskylä, Finland
Interests: bio-organic supramolecular chemistry; NMR spectroscopy
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Special Issue Information

Dear Colleagues,

Supramolecular hydrogels, a fascinating class of soft materials, have gained significant attention in recent years due to their wide-ranging applications in fields such as drug delivery, tissue engineering, and environmental remediation. The Special Issue “Design of Supramolecular Hydrogels” aims to provide a comprehensive platform for researchers to showcase their innovative work and insights into the development and applications of supramolecular hydrogels.

The aim of this Special Issue is to explore various aspects of supramolecular hydrogel design, including the rational design of molecular building blocks, predicting gel-state properties, the incorporation of functional elements, and the optimization of gelation processes. We encourage the submission of contributions presenting the characterization of these hydrogels, their mechanical properties, elucidation of their unique self-assembly mechanisms, and exploration of potential applications in diverse fields.

Authors are invited to submit research articles, reviews, and perspectives that address challenges and advancements in supramolecular hydrogel design, from fundamental principles to practical applications. The submission of both theoretical and experimental studies is welcome. By fostering a deeper understanding of these materials, this Special Issue aims to accelerate progress in the field and inspire innovative approaches for designing supramolecular hydrogels with enhanced properties and broader utility. Researchers from diverse disciplines are encouraged to participate in this interdisciplinary exploration and strengthen collaboration and knowledge exchange in this exciting area of research.

Dr. Dipankar Ghosh
Dr. Gareth O. Lloyd
Dr. Elina I. Sievanen
Guest Editors

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Keywords

  • designing new supramolecular hydrogelators
  • prediction of gel properties
  • mechanism of self-assembly
  • hydrogel characterization
  • structure–property relationship
  • applications in diverse fields
  • smart hydrogels
  • 3D/4D printing
  • tissue engineering
  • regenerative medicine
  • controlled release system
  • biodegradable hydrogels

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Published Papers (3 papers)

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26 pages, 22121 KiB  
Article
Developing Innovative Apolar Gels Based on Cellulose Derivatives for Cleaning Metal Artworks
by Andrea Macchia, Camilla Zaratti, Davide Ciogli, Giovanni Rivici, Silvia Pilati, Nereo Sbiri, Tilde de Caro and Maria Assunta Navarra
Gels 2024, 10(11), 747; https://doi.org/10.3390/gels10110747 - 16 Nov 2024
Viewed by 363
Abstract
The use of organic solvents, particularly those of a non-polar nature, is a common practice during cleaning operations in the restoration of polychrome artworks and metallic artifacts. However, these solvents pose significant risks to the health of operators and the environment. This study [...] Read more.
The use of organic solvents, particularly those of a non-polar nature, is a common practice during cleaning operations in the restoration of polychrome artworks and metallic artifacts. However, these solvents pose significant risks to the health of operators and the environment. This study explores the formulation of innovative gels based on non-polar solvents and cellulose derivatives, proposing a safe and effective method for cleaning metallic artworks. The study is focused on a toxic apolar solvent, Ligroin, identified as one of the most widely used solvents in the cultural heritage treatments, and some “green” alternatives such as Methyl Myristate and Isopropyl Palmitate. The main challenge lies in overcoming the chemical incompatibility between non-polar solvents and polar thickening agents like cellulose ethers. To address this problem, the research was based on a hydrophilic–lipophilic balance (HLB) system and Hansen solubility parameters (HSPs) to select appropriate surfactants, ensuring the stability and effectiveness of the formulated gels. Stability, viscosity, and solvent release capacity of gels were analyzed using Static Light Multiple Scattering (Turbiscan), viscometry, and thermogravimetric analysis (TGA). The efficacy of cleaning in comparison with Ligroin liquid was evaluated on a metal specimen treated with various apolar protective coatings used commonly in the restoration of metallic artifacts, such as microcrystalline waxes (Reswax, Soter), acrylic resins (Paraloid B44), and protective varnishes (Incral, Regalrez). Multispectral analysis, digital optical microscopy, FTIR spectroscopy, and spectrocolorimetry allowed for the assessment of the gels’ ability to remove the different protective coatings, the degree of cleaning achieved, and the presence of any residues. The results obtained highlight the ability of the formulated gels to effectively remove protective coatings from metallic artifacts. Cetyl Alcohol proved to be the most versatile surfactant to realize a stable and efficient gel. The gels based on Methyl Myristate and Isopropyl Palmitate showed promising results as “green” alternatives to Ligroin, although in some cases, they exhibited less selectivity in the removal of protective coatings. Full article
(This article belongs to the Special Issue Design of Supramolecular Hydrogels)
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15 pages, 4341 KiB  
Article
Effect of Silk Fibroin on the Mechanical and Transport Properties of Agarose Hydrogels
by Veronika Richterová and Miloslav Pekař
Gels 2024, 10(10), 611; https://doi.org/10.3390/gels10100611 - 24 Sep 2024
Viewed by 743
Abstract
In this work, the effect of incorporating silk fibroin, a fibrous biocompatible protein, into physically cross-linked agarose hydrogels was investigated as a simple model study to examine how supramolecular fibrous structures influence the properties of the hydrogels. The rheological and transport properties were [...] Read more.
In this work, the effect of incorporating silk fibroin, a fibrous biocompatible protein, into physically cross-linked agarose hydrogels was investigated as a simple model study to examine how supramolecular fibrous structures influence the properties of the hydrogels. The rheological and transport properties were studied. Fibroin did not change the general viscoelastic properties of the investigated hydrogels but changed the viscoelastic moduli values and also the mesh size, as calculated from rheometry data. Fibroin influenced the mechanical properties depending on its concentration: at lower concentrations, it increased the mesh size, while at higher concentrations, it acted as a filler, decreasing the mesh size. Similarly, the storage and loss moduli were affected, either increasing or decreasing based on the fibroin concentration. The fibroin effect on the diffusion of two dyes differing in their charge was the result of a combination of structural effects, responsible also for changes in the rheological properties, and a result of electrostatic interactions between the charged groups. For positively charged methylene blue, low fibroin concentrations accelerated diffusion, while higher concentrations slowed it by filling network vacancies. In contrast, for negatively charged eosin-B, fibroin strongly impeded diffusion at all concentrations due to electrostatic repulsion, leading to its accumulation at the hydrogel interface. The findings of this work may contribute to an understanding of the behavior of the extracellular matrix or soft tissues as well as to the development of the tailored design of hydrogel materials. Full article
(This article belongs to the Special Issue Design of Supramolecular Hydrogels)
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18 pages, 3239 KiB  
Article
Designing Stimuli-Responsive Supramolecular Gels by Tuning the Non-Covalent Interactions of the Functional Groups
by Geethanjali Kuppadakkath, Ira Volkova and Krishna K. Damodaran
Gels 2024, 10(9), 584; https://doi.org/10.3390/gels10090584 - 11 Sep 2024
Viewed by 668
Abstract
The physical characteristics of a supramolecular gel are greatly influenced by the nature and arrangement of functional groups in the gelator. This work focuses on the impact of the functional groups, specifically the hydroxyl group, on the stimuli-responsive properties of a gel. We [...] Read more.
The physical characteristics of a supramolecular gel are greatly influenced by the nature and arrangement of functional groups in the gelator. This work focuses on the impact of the functional groups, specifically the hydroxyl group, on the stimuli-responsive properties of a gel. We used a C3-symmetric benzene-1,3,5-tricarboxamide (BTA) platform, which was attached to the methyl ester of phenylalanine (MPBTA) and tyrosine (MTBTA). The gelation studies revealed that MPBTA gelled in alcohols, non-polar aromatic solvents, and aqueous mixtures (1:1, v/v) of high-polar solvents, whereas MTBTA gelled only in an aqueous mixture of DMF (1:1, v/v). The mechanical and thermal strength of the gels were evaluated by rheological and Tgel studies, and the results indicated that MPBTA gels were stronger than MTBTA gels. The gels were characterized by powder X-ray diffraction and scanning electron microscopy (SEM). The analysis of stimuli-responsive properties revealed that MPBTA gels were intact in the presence of sodium/potassium salts, but the MTBTA gel network was disrupted. These results indicate that the elegant choice of functional groups could be used to tune the constructive or destructive stimuli-responsive behavior of gels. This study highlights the significant role of functional groups in modulating the stimuli-responsive properties of supramolecular gels. Full article
(This article belongs to the Special Issue Design of Supramolecular Hydrogels)
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