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Gels
Special Issues
Organogels: State of the Art
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Organogels: State of the Art

A special issue of Gels (ISSN 2310-2861).

Deadline for manuscript submissions: closed (31 May 2021) | Viewed by 19495

Special Issue Editor

Prof. Dr. Pablo H. Di Chenna

E-Mail Website
Guest Editor
Departamento de Química Orgánica, UMYMFOR (CONICET-FCEN), Universidad de Buenos Aires, Piso 3, pabellón 2, Ciudad Universitaria, C1428EGA, Buenos Aires, Argentina
Interests: development and study of new physical gels; organogels as template for the preparation of nanoparticles; supramolecular chemistry; structure-gelating property relationship; steroid-derived physical gels; development of functional soft materials
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Organogels are a very diverse and fascinating class of soft material that over the years have evolved to be one of the most attractive subjects in materials science. All organogels have in common an organic liquid phase immobilized within a three-dimensional structured network, but the nature of the organic liquid, together with the gelator, determines the physicochemical and mechanical properties, as well as the functionality of these gels. Classic polymeric organogels, where the organic liquid phase is a classic organic solvent or oil trapped within an organic polymer, have found very important applications in the pharmaceutical, food, and cosmetics industries, and are still under development. In the last several years, supramolecular organogels have also attracted increasing attention because of their special properties (e.g., reversibility, self-healing, and functionality), being the focus of several high-tech applications. Very recently, organic ionic liquids and deep eutectic solvents have been used to prepare ionic organogels with very interesting properties such as high ionic conductivity and many potential applications in drug delivery. Despite the many industrial and high-tech potential applications of these materials, the organogelling process is not fully understood and is continuously under investigation.

This Special Issue is dedicated to overviewing the current state of the art in the area of organogels as well as future challenges, covering all aspects of these diverse materials:

  1. Design, synthesis, and preparation of organogels;
  2. Mechanism of gelation;
  3. Characterization of organogels;
  4. Properties and applications.

I hope this Special Issue will provide the possibility for researchers around the world to present and discuss their most recent findings and developments on organogels.

Prof. Dr. Pablo H. Di Chenna
Guest Editor

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. Gels is an international peer-reviewed open access monthly 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 2600 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

  • Polymeric organogels
  • Supramolecular organogels
  • Gelation mechanism
  • Organogel characterization
  • Responsive organogels
  • Organogel applications
  • Ionic organogels
  • Eutectogels

Published Papers (7 papers)

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Editorial

Jump to: Research, Review

2 pages, 188 KiB  
Editorial
Editorial on Special Issue “Organogels: State of the Art”
by Pablo Héctor Di Chenna
Gels 2022, 8(3), 157; https://0-doi-org.brum.beds.ac.uk/10.3390/gels8030157 - 04 Mar 2022
Viewed by 1450
Abstract
Organogels are a very diverse and fascinating class of soft materials that, over the last 30 years, have evolved to be one of the most interesting subjects in materials science [...] Full article
(This article belongs to the Special Issue Organogels: State of the Art)

Research

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12 pages, 20671 KiB  
Article
Investigation of an Organogel by Micro-Differential Scanning Calorimetry: Quantitative Relationship between the Shapes of the Thermograms and the Phase Diagram
by Duncan Schwaller, Elliot Christ, Mélanie Legros, Dominique Collin and Philippe J. Mésini
Gels 2021, 7(3), 93; https://0-doi-org.brum.beds.ac.uk/10.3390/gels7030093 - 14 Jul 2021
Cited by 3 | Viewed by 2441
Abstract
The phase diagrams of organogels are necessary for applications and fundamental aspects, for instance to understand their thermodynamics. Differential scanning calorimetry is one of the techniques implemented to map these diagrams. The thermograms of organogels upon heating show broad endotherms, increasing gradually to [...] Read more.
The phase diagrams of organogels are necessary for applications and fundamental aspects, for instance to understand their thermodynamics. Differential scanning calorimetry is one of the techniques implemented to map these diagrams. The thermograms of organogels upon heating show broad endotherms, increasing gradually to a maximum, at a temperature Tmax, and decreasing back to the baseline, sometimes 10 °C above. This broadening can lead to uncertainty in determining the molar enthalpies and the melting temperatures Tm of the gels. Herein, we have measured the thermograms of the 12-hydroxystearic acid/nitrobenzene gels for weight fractions ranging from 0.0015 to 0.04. Compared with transition temperatures measured by other techniques, the inflection points of the thermograms provide a measurement of Tm with less bias than Tmax. The phase diagram explains why the molar melting enthalpies derived from the thermograms for samples of low concentration are lower than expected. The shapes of the heat flows below the peak correlate quantitatively with the diagrams: after suitable correction and normalization, the integral curves superimpose with the phase diagram in their ascending branch and reach a plateau when the gel is fully melted. The shape of the thermograms upon cooling is also qualitatively explained within the frame of the diagrams. Full article
(This article belongs to the Special Issue Organogels: State of the Art)
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11 pages, 2001 KiB  
Article
Decoupling of Mechanical and Transport Properties in Organogels via Solvent Variation
by Kenneth P. Mineart, Cameron Hong and Lucas A. Rankin
Gels 2021, 7(2), 61; https://0-doi-org.brum.beds.ac.uk/10.3390/gels7020061 - 21 May 2021
Cited by 3 | Viewed by 2098
Abstract
Organogels have recently been considered as materials for transdermal drug delivery media, wherein their transport and mechanical properties are among the most important considerations. Transport through organogels has only recently been investigated and findings highlight an inextricable link between gels’ transport and mechanical [...] Read more.
Organogels have recently been considered as materials for transdermal drug delivery media, wherein their transport and mechanical properties are among the most important considerations. Transport through organogels has only recently been investigated and findings highlight an inextricable link between gels’ transport and mechanical properties based upon the formulated polymer concentration. Here, organogels composed of styrenic triblock copolymer and different aliphatic mineral oils, each with a unique dynamic viscosity, are characterized in terms of their quasi-static uniaxial mechanical behavior and the internal diffusion of two unique solute penetrants. Mechanical testing results indicate that variation of mineral oil viscosity does not affect gel mechanical behavior. This likely stems from negligible changes in the interactions between mineral oils and the block copolymer, which leads to consistent crosslinked network structure and chain entanglement (at a fixed polymer concentration). Conversely, results from diffusion experiments highlight that two penetrants—oleic acid (OA) and aggregated aerosol-OT (AOT)—diffuse through gels at a rate inversely proportional to mineral oil viscosity. The inverse dependence is theoretically supported by the hydrodynamic model of solute diffusion through gels. Collectively, our results show that organogel solvent variation can be used as a design parameter to tailor solute transport through gels while maintaining fixed mechanical properties. Full article
(This article belongs to the Special Issue Organogels: State of the Art)
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Graphical abstract

12 pages, 3841 KiB  
Article
Supramolecular Fractal Growth of Self-Assembled Fibrillar Networks
by Pedram Nasr, Hannah Leung, France-Isabelle Auzanneau and Michael A. Rogers
Gels 2021, 7(2), 46; https://0-doi-org.brum.beds.ac.uk/10.3390/gels7020046 - 14 Apr 2021
Cited by 5 | Viewed by 2657
Abstract
Complex morphologies, as is the case in self-assembled fibrillar networks (SAFiNs) of 1,3:2,4-Dibenzylidene sorbitol (DBS), are often characterized by their Fractal dimension and not Euclidean. Self-similarity presents for DBS-polyethylene glycol (PEG) SAFiNs in the Cayley Tree branching pattern, similar box-counting fractal dimensions across [...] Read more.
Complex morphologies, as is the case in self-assembled fibrillar networks (SAFiNs) of 1,3:2,4-Dibenzylidene sorbitol (DBS), are often characterized by their Fractal dimension and not Euclidean. Self-similarity presents for DBS-polyethylene glycol (PEG) SAFiNs in the Cayley Tree branching pattern, similar box-counting fractal dimensions across length scales, and fractals derived from the Avrami model. Irrespective of the crystallization temperature, fractal values corresponded to limited diffusion aggregation and not ballistic particle–cluster aggregation. Additionally, the fractal dimension of the SAFiN was affected more by changes in solvent viscosity (e.g., PEG200 compared to PEG600) than crystallization temperature. Most surprising was the evidence of Cayley branching not only for the radial fibers within the spherulitic but also on the fiber surfaces. Full article
(This article belongs to the Special Issue Organogels: State of the Art)
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Review

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18 pages, 3485 KiB  
Review
Computational Tools to Rationalize and Predict the Self-Assembly Behavior of Supramolecular Gels
by Ruben Van Lommel, Wim M. De Borggraeve, Frank De Proft and Mercedes Alonso
Gels 2021, 7(3), 87; https://0-doi-org.brum.beds.ac.uk/10.3390/gels7030087 - 09 Jul 2021
Cited by 11 | Viewed by 4138
Abstract
Supramolecular gels form a class of soft materials that has been heavily explored by the chemical community in the past 20 years. While a multitude of experimental techniques has demonstrated its usefulness when characterizing these materials, the potential value of computational techniques has [...] Read more.
Supramolecular gels form a class of soft materials that has been heavily explored by the chemical community in the past 20 years. While a multitude of experimental techniques has demonstrated its usefulness when characterizing these materials, the potential value of computational techniques has received much less attention. This review aims to provide a complete overview of studies that employ computational tools to obtain a better fundamental understanding of the self-assembly behavior of supramolecular gels or to accelerate their development by means of prediction. As such, we hope to stimulate researchers to consider using computational tools when investigating these intriguing materials. In the concluding remarks, we address future challenges faced by the field and formulate our vision on how computational methods could help overcoming them. Full article
(This article belongs to the Special Issue Organogels: State of the Art)
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23 pages, 8440 KiB  
Review
Physical Aspects of Organogelation: A Point of View
by Jean-Michel Guenet
Gels 2021, 7(2), 65; https://0-doi-org.brum.beds.ac.uk/10.3390/gels7020065 - 01 Jun 2021
Cited by 14 | Viewed by 3110
Abstract
The physics side of organogelation is broached through three main aspects, thermodynamics (formation and melting), structure (morphology and molecular organization), and rheology. A definition of a gel is first discussed so as to delimit the field of investigation; namely, systems constituted of fibril-like [...] Read more.
The physics side of organogelation is broached through three main aspects, thermodynamics (formation and melting), structure (morphology and molecular organization), and rheology. A definition of a gel is first discussed so as to delimit the field of investigation; namely, systems constituted of fibril-like entities. It is again highlighted that gel formation occurs through first-order transitions, chiefly by homogeneous nucleation. A deeper knowledge of the system is thus achieved by mapping out the temperature–concentration phase diagram. Some experimental diagrams are shown, while diagrams likely to pertain to these systems are presented. The molecular arrangement is basically crystallization that occurs in a preferred direction, hence the formation of fibrils. The effects of the solvent type, the quenching process of the solution are discussed with respect to the morphology and the crystal structure. Finally, the rheological properties are tackled. Notions of critical gelation concentration and percolation are debated. The interest of mapping out the temperature–concentration phase diagram is emphasized, particularly for understanding the variation of the gel modulus with temperature. Full article
(This article belongs to the Special Issue Organogels: State of the Art)
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24 pages, 11552 KiB  
Review
Carbocycle-Based Organogelators: Influence of Chirality and Structural Features on Their Supramolecular Arrangements and Properties
by Rosa M. Ortuño
Gels 2021, 7(2), 54; https://0-doi-org.brum.beds.ac.uk/10.3390/gels7020054 - 01 May 2021
Cited by 7 | Viewed by 2311
Abstract
The rational design and engineer of organogel-based smart materials and stimuli-responsive materials with tuned properties requires the control of the non-covalent forces driving the hierarchical self-assembly. Chirality, as well as cis/trans relative configuration, also plays a crucial role promoting the morphology and characteristics [...] Read more.
The rational design and engineer of organogel-based smart materials and stimuli-responsive materials with tuned properties requires the control of the non-covalent forces driving the hierarchical self-assembly. Chirality, as well as cis/trans relative configuration, also plays a crucial role promoting the morphology and characteristics of the aggregates. Cycloalkane derivatives can provide chiral chemical platforms allowing the incorporation of functional groups and hydrophobic structural units able for a convenient molecular stacking leading to gels. Restriction of the conformational freedom imposed by the ring strain is also a contributing issue that can be modulated by the inclusion of flexible segments. In addition, donor/acceptor moieties can also be incorporated favoring the interactions with light or with charged species. This review offers a perspective on the abilities and properties of carbocycle-based organogelators starting from simple cycloalkane derivatives, which were the key to establish the basis for an effective self-assembling, to sophisticated polycyclic compounds with manifold properties and applications. Full article
(This article belongs to the Special Issue Organogels: State of the Art)
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