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Supramolecular Gel II
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Supramolecular Gel II

A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Macromolecular Chemistry".

Deadline for manuscript submissions: closed (31 March 2023) | Viewed by 16579

Special Issue Editors

Prof. Dr. Francesca D’Anna

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Guest Editor
Dipartimento di Scienze e Tecnologie Biologiche, Università degli Studi di Palermo, Palermo, Italy
Interests: supramolecular chemistry; ionic liquids; supramolecular gels; hybrid supramolecular gels; biomass transformation; self-assembly processes
Special Issues, Collections and Topics in MDPI journals
Dr. Salvatore Marullo

E-Mail Website
Guest Editor
Dipartimento di Scienze e Tecnologie Biologiche, Università degli Studi di Palermo, Palermo, Italy
Interests: ionic liquids; supramolecular gels; biomass transformation; self-assembly processes
Special Issues, Collections and Topics in MDPI journals
Dr. Carla Rizzo

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Guest Editor
Dipartimento di Scienze e Tecnologie Biologiche, Università degli Studi di Palermo, Palermo, Italy
Interests: ionic liquids; supramolecular gels; hybrid supramolecular gels; biomass transformation
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Supramolecular gels represent one of the new frontiers of materials chemistry. Built by the feeble and cooperative supramolecular interactions occurring among low molecular weight compounds (gelators), they are featured in 3D networks which are able to immobilize solvents through the occurrence of capillary forces.

Their classification is solvent-based and together with more common organo- and hydrogels, i.e., gels formed in organic solvents or water; more recently, ionogels, i.e., gels formed in ionic liquids, have also attracted research attention. In all cases, the gel texture proves more porous with respect to polymeric gels. Furthermore, they are frequently able to be restored after the action of external stimuli, such as pH changes, UV-vis irradiation, magnetic stirring or ultrasound irradiation. These abilities have significantly favored their application, and they are currently applied in different fields, such as the pharmaceutical (as a drug carrier and matrix for drug crystallization), environmental (as a sorbent for pollutant removal), synthetic (as a reaction media) fields, etc.

This issue is aimed at collecting contributions on studies on the obtaining of gel phases and their characterization, in the attempt to better clarify the relationship between gelator, solvent nature, and gel phase formation. On the other hand, investigations of the plethora of supramolecular gels applications will also be taken into account. The main goal of the Special Issue is to shed light on the ongoing research on this topic.

Prof. Dr. Francesca D’Anna
Dr. Salvatore Marullo
Dr. Carla Rizzo
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. Molecules 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

  • Hydrogels
  • Organogels
  • Ionogels
  • Hybrid supramolecular gels
  • Gel properties
  • Gel applications

Related Special Issue

Published Papers (6 papers)

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Research

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19 pages, 6044 KiB  
Article
Silver Is Not Equal to Silver: Synthesis and Evaluation of Silver Nanoparticles with Low Biological Activity, and Their Incorporation into C12Alanine-Based Hydrogel
by Konrad Kubiński, Kamila Górka, Monika Janeczko, Aleksandra Martyna, Mateusz Kwaśnik, Maciej Masłyk, Emil Zięba, Joanna Kowalczuk, Piotr Kuśtrowski, Mariusz Borkowski, Anna Boguszewska-Czubara, Agnieszka Klimeczek and Oleg M. Demchuk
Molecules 2023, 28(3), 1194; https://doi.org/10.3390/molecules28031194 - 25 Jan 2023
Cited by 5 | Viewed by 2081
Abstract
A new type of silver nanoparticles (AgNPs) was prepared and comprehensively studied. Scanning electron microscopy (SEM) and dynamic light scattering (DLS) analyses indicated that 24 nm AgNPs with narrow size distribution were obtained while Z-potential confirms their good stability. The composites of the [...] Read more.
A new type of silver nanoparticles (AgNPs) was prepared and comprehensively studied. Scanning electron microscopy (SEM) and dynamic light scattering (DLS) analyses indicated that 24 nm AgNPs with narrow size distribution were obtained while Z-potential confirms their good stability. The composites of the obtained AgNPs with nontoxic-nature-inspired hydrogel were formed upon cooling of the aqueous solution AgNPs and C12Ala. The thermal gravimetric analysis (TGA) and the differential scanning calorimetry (DSC) do not show significant shifts in the characteristic temperature peaks for pure and silver-enriched gels, which indicates that AgNPs do not strongly interact with C12Ala fibers, which was also confirmed by SEM. Both AgNPs alone and in the assembly with the gelator C12Ala were almost biologically passive against bacteria, fungus, cancer, and nontumor human cells, as well as zebra-fish embryos. These studies proved that the new inactive AgNPs-doped hydrogels have potential for the application in therapy as drug delivery media. Full article
(This article belongs to the Special Issue Supramolecular Gel II)
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13 pages, 2985 KiB  
Article
Anion-Responsive Fluorescent Supramolecular Gels
by Giacomo Picci, Matthew T. Mulvee, Claudia Caltagirone, Vito Lippolis, Antonio Frontera, Rosa M. Gomila and Jonathan W. Steed
Molecules 2022, 27(4), 1257; https://doi.org/10.3390/molecules27041257 - 13 Feb 2022
Cited by 10 | Viewed by 2465
Abstract
Three novel bis-urea fluorescent low-molecular-weight gelators (LMWGs) based on the tetraethyl diphenylmethane spacer—namely, L1, L2, and L3, bearing indole, dansyl, and quinoline units as fluorogenic fragments, respectively, are able to form gel in different solvents. L2 and L3 gel in [...] Read more.
Three novel bis-urea fluorescent low-molecular-weight gelators (LMWGs) based on the tetraethyl diphenylmethane spacer—namely, L1, L2, and L3, bearing indole, dansyl, and quinoline units as fluorogenic fragments, respectively, are able to form gel in different solvents. L2 and L3 gel in apolar solvents such as chlorobenzene and nitrobenzene. Gelator L1 is able to gel in the polar solvent mixture DMSO/H2O (H2O 15% v/v). This allowed the study of gel formation in the presence of anions as a third component. An interesting anion-dependent gel formation was observed with fluoride and benzoate inhibiting the gelation process and H2PO4−, thus causing a delay of 24 h in the gel formation. The interaction of L1 with the anions in solution was clarified by 1H-NMR titrations and the differences in the cooperativity of the two types of NH H-bond donor groups (one indole NH and two urea NHs) on L1 when binding BzO− or H2PO4− were taken into account to explain the inhibition of the gelation in the presence of BzO−. DFT calculations corroborate this hypothesis and, more importantly, demonstrate considering a trimeric model of the L1 gel that BzO− favours its disruption into monomers inhibiting the gel formation. Full article
(This article belongs to the Special Issue Supramolecular Gel II)
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10 pages, 1164 KiB  
Article
The Effect of Supramolecular Humic Acids on the Diffusivity of Metal Ions in Agarose Hydrogel
by Martina Klučáková
Molecules 2022, 27(3), 1019; https://doi.org/10.3390/molecules27031019 - 2 Feb 2022
Cited by 5 | Viewed by 1590
Abstract
Humic acids are known as natural substances of a supramolecular nature. Their self-assembly ability can affect the migration of heavy metals and other pollutants in nature. The formation of metal-humic complexes can decrease their mobility and bioavailability. This study focuses on metal ions [...] Read more.
Humic acids are known as natural substances of a supramolecular nature. Their self-assembly ability can affect the migration of heavy metals and other pollutants in nature. The formation of metal-humic complexes can decrease their mobility and bioavailability. This study focuses on metal ions diffusion and immobilization in humic hydrogels. Humic acids were purchased from International Humic Substances Society (isolated from different matrices—peat, soil, leonardite, water) and extracted from lignite mined in Czech Republic. Copper(II) ions were chosen as a model example of reactive metals for the diffusion experiments. The model of instantaneous planar source was used for experimental data obtained from monitoring the time development of copper(II) ions distribution in hydrogel. The effective diffusion coefficients of copper(II) ions showed the significant dependence on reaction ability of humic hydrogels. Lower amounts of the acidic functional groups caused an increase in the effective diffusion coefficient. In general, diffusion experiments seem to act as a valuable method for reactivity mapping studies on humic substances. Full article
(This article belongs to the Special Issue Supramolecular Gel II)
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21 pages, 3956 KiB  
Article
Making and Breaking of Gels: Stimuli-Responsive Properties of Bis(Pyridyl-N-oxide Urea) Gelators
by Sreejith Sudhakaran Jayabhavan, Dipankar Ghosh and Krishna K. Damodaran
Molecules 2021, 26(21), 6420; https://doi.org/10.3390/molecules26216420 - 24 Oct 2021
Cited by 6 | Viewed by 2811
Abstract
The structural modification of existing supramolecular architecture is an efficient strategy to design and synthesize supramolecular gels with tunable and predictable properties. In this work, we have modified bis(pyridyl urea) compounds with different linkers, namely hexylene and butylene, to their corresponding bis(pyridyl-N [...] Read more.
The structural modification of existing supramolecular architecture is an efficient strategy to design and synthesize supramolecular gels with tunable and predictable properties. In this work, we have modified bis(pyridyl urea) compounds with different linkers, namely hexylene and butylene, to their corresponding bis(pyridyl-N-oxide urea). The gelation properties of both the parent and the modified compounds were studied, and the results indicated that modification of the 3-pyridyl moieties to the corresponding 3-pyridyl-N-oxides induced hydrogelation. The stability of the parent and modified compounds were evaluated by sol-gel transition temperature (Tgel) and rheological measurements, and single-crystal X-ray diffraction was used to analyze the solid-state interactions of the gelators. The morphologies of the dried gels were analyzed by scanning electron microscopy (SEM), which revealed that the structural modification did not induce any prominent effect on the gel morphology. The stimuli-responsive behavior of these gels in the presence of salts in DMSO/water was evaluated by rheological experiments, which indicated that the modified compounds displayed enhanced gel strength in most cases. However, the gel network collapsed in the presence of the chloride salts of aluminum(III), zinc(II), copper(II), and cadmium(II). The mechanical strength of the parent gels decreased in the presence of salts, indicating that the structural modification resulted in robust gels in most cases. The modified compounds formed gels below minimum gel concentration in the presence of various salts, indicating salt-induced gelation. These results show the making and breaking ability of the gel network in the presence of external stimuli (salts), which explains the potential of using LMWGs based on N-oxide moieties as stimuli-responsive materials. Full article
(This article belongs to the Special Issue Supramolecular Gel II)
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11 pages, 8442 KiB  
Article
Effect of Process Conditions and Colloidal Properties of Cellulose Nanocrystals Suspensions on the Production of Hydrogel Beads
by Nicola Ferrari, Cecilia Ada Maestri, Paolo Bettotti, Mario Grassi, Michela Abrami and Marina Scarpa
Molecules 2021, 26(9), 2552; https://doi.org/10.3390/molecules26092552 - 27 Apr 2021
Cited by 3 | Viewed by 2019
Abstract
The influence of the physical, rheological, and process parameters on the cellulose nanocrystal (CNC) drops before and after external gelation in a CaCl2 solution was investigated. The dominant role of the CNC’s colloidal suspension properties, such as the viscous force, inertial, and [...] Read more.
The influence of the physical, rheological, and process parameters on the cellulose nanocrystal (CNC) drops before and after external gelation in a CaCl2 solution was investigated. The dominant role of the CNC’s colloidal suspension properties, such as the viscous force, inertial, and surface tension forces in the fluid dynamics was quantitatively evaluated in the formation of drops and jellified beads. The similarity and difference between the behavior of carbohydrate polymers and rod-like crystallites such as CNC were enlightened. Pump-driven and centrifugally-driven external gelation approaches were followed to obtain CNC hydrogel beads with tunable size and regular shape. A superior morphological control—that is, a more regular shape and smaller dimension of the beads—were obtained by centrifugal force-driven gelation. These results suggest that even by using a simple set-up and a low-speed centrifuge device, the extrusion of a colloidal solution through a small nozzle under a centrifugal field is an efficient approach for the production of CNC hydrogel beads with good reproducibility, control over the bead morphology and size monodispersion. Full article
(This article belongs to the Special Issue Supramolecular Gel II)
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Review

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17 pages, 3126 KiB  
Review
Diketopiperazine Gels: New Horizons from the Self-Assembly of Cyclic Dipeptides
by Marco Scarel and Silvia Marchesan
Molecules 2021, 26(11), 3376; https://doi.org/10.3390/molecules26113376 - 3 Jun 2021
Cited by 28 | Viewed by 4652
Abstract
Cyclodipeptides (CDPs) or 2,5-diketopiperazines (DKPs) can exert a variety of biological activities and display pronounced resistance against enzymatic hydrolysis as well as a propensity towards self-assembly into gels, relative to the linear-dipeptide counterparts. They have attracted great interest in a variety of fields [...] Read more.
Cyclodipeptides (CDPs) or 2,5-diketopiperazines (DKPs) can exert a variety of biological activities and display pronounced resistance against enzymatic hydrolysis as well as a propensity towards self-assembly into gels, relative to the linear-dipeptide counterparts. They have attracted great interest in a variety of fields spanning from functional materials to drug discovery. This concise review will analyze the latest advancements in their synthesis, self-assembly into gels, and their more innovative applications. Full article
(This article belongs to the Special Issue Supramolecular Gel II)
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