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Gels
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Advance in Supramolecular Gels
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Advance in Supramolecular Gels

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

Deadline for manuscript submissions: closed (30 July 2023) | Viewed by 19098

Special Issue Editors

Prof. Dr. Yiming Wang

E-Mail Website
Guest Editor
State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
Interests: out-of-equilibrium systems; supramolecular gels; systems chemistry; dynamic smart materials
Special Issues, Collections and Topics in MDPI journals
Dr. Yutao Sang

E-Mail Website
Guest Editor
Department of Chemical and Biological Physics, Weizmann Institute of Science, Rehovot 7610001, Israel
Interests: supramolecular chirality; gels; chiral self-assembly; spin-dependent electron transfer

Special Issue Information

Dear Colleagues,

Supramolecular gels, which are generally formed by the self-assembly of small molecules through various non-covalent interactions, are currently an important class of soft materials attracting considerable interest in the field of sensing, catalysis, cell culturing, drug delivery, tissue engineering, environmental remediation, and optoelectronics. Due to the dynamic nature of non-covalent bonds, supramolecular gels show inherent dynamic and reversibility, differing from covalently cross-linked polymer gels which are usually static without additional tunability. Inspired by nature, the development of supramolecular gels has evolved into a much broader discipline, which makes it possible for gel materials to have more interesting and emergent functions. For instance, the interests in the field of supramolecular gels have been shifting from traditional thermodynamic control to non-equilibrium self-assembly, and from single-component systems to more complex multicomponent systems. As a result, a more elaborate structural and functional diversity of supramolecular gel systems has been created.

On the basis of the great progress in the field of supramolecular gels in recent years, we organize this Special Issue on “Advance in Supramolecular Gels” with the aim to summarize the recent achievements in the design of gelators, the investigation of self-assembly mechanisms, self-assembly control, and the functionalization and potential applications of supramolecular gels, among other relevant topics. We look forward to the submission of new results and reviews associated with supramolecular gels from experimental and theoretical perspectives.

Prof. Dr. Yiming Wang
Dr. Yutao Sang
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. 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

  • soft materials
  • supramolecular gels
  • gelator design
  • gelation mechanism
  • thermodynamic stability
  • pathway control
  • out-of-equilibrium system
  • properties studies
  • functional gels
  • potential applications
  • systems chemistry

Published Papers (10 papers)

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Research

12 pages, 2924 KiB  
Article
Synthesis and Cytotoxicity Studies of Poly(1,4-butanediol citrate) Gels for Cell Culturing
by Aleksandra Bandzerewicz, Klara Niebuda and Agnieszka Gadomska-Gajadhur
Gels 2023, 9(8), 628; https://doi.org/10.3390/gels9080628 - 04 Aug 2023
Cited by 1 | Viewed by 799
Abstract
One of the main branches of regenerative medicine is biomaterials research, which is designed to develop and study materials for regenerative therapies, controlled drug delivery systems, wound dressings, etc. Research is continually being conducted to find biomaterials—especially polymers—with better biocompatibility, broader modification possibilities [...] Read more.
One of the main branches of regenerative medicine is biomaterials research, which is designed to develop and study materials for regenerative therapies, controlled drug delivery systems, wound dressings, etc. Research is continually being conducted to find biomaterials—especially polymers—with better biocompatibility, broader modification possibilities and better application properties. This study describes a potential biomaterial, poly(1,4-butanediol citrate). The gelation time of poly(1,4-butanediol citrate) was estimated. Based on this, the limiting reaction time and temperature were determined to avoid gelling of the reaction mixture. Experiments with different process conditions were carried out, and the products were characterised through NMR spectra analysis. Using statistical methods, the functions were defined, describing the dependence of the degree of esterification of the acid groups on the following process parameters: temperature and COOH/OH group ratio. Polymer films from the synthesised polyester were prepared and characterised. The main focus was assessing the initial biocompatibility of the materials. Full article
(This article belongs to the Special Issue Advance in Supramolecular Gels)
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29 pages, 5503 KiB  
Article
Unveiling the Role of Capping Groups in Naphthalene N-Capped Dehydrodipeptide Hydrogels
by Helena Vilaça, André Carvalho, Tarsila Castro, Elisabete M. S. Castanheira, Loic Hilliou, Ian Hamley, Manuel Melle-Franco, Paula M. T. Ferreira and José A. Martins
Gels 2023, 9(6), 464; https://doi.org/10.3390/gels9060464 - 06 Jun 2023
Viewed by 1311
Abstract
Self-assembled peptide-based hydrogels are archetypical nanostructured materials with a plethora of foreseeable applications in nanomedicine and as biomaterials. N-protected di- and tri-peptides are effective minimalist (molecular) hydrogelators. Independent variation of the capping group, peptide sequence and side chain modifications allows a wide chemical [...] Read more.
Self-assembled peptide-based hydrogels are archetypical nanostructured materials with a plethora of foreseeable applications in nanomedicine and as biomaterials. N-protected di- and tri-peptides are effective minimalist (molecular) hydrogelators. Independent variation of the capping group, peptide sequence and side chain modifications allows a wide chemical space to be explored and hydrogel properties to be tuned. In this work, we report the synthesis of a focused library of dehydrodipeptides N-protected with 1-naphthoyl and 2-naphthylacetyl groups. The 2-naphthylacetyl group was extensively reported for preparation of peptide-based self-assembled hydrogels, whereas the 1-naphthaloyl group was largely overlooked, owing presumably to the lack of a methylene linker between the naphthalene aromatic ring and the peptide backbone. Interestingly, dehydrodipeptides N-capped with the 1-naphthyl moiety afford stronger gels, at lower concentrations, than the 2-naphthylacetyl-capped dehydrodipeptides. Fluorescence and circular dichroism spectroscopy showed that the self-assembly of the dehydrodipeptides is driven by intermolecular aromatic π–π stacking interactions. Molecular dynamics simulations revealed that the 1-naphthoyl group allows higher order aromatic π–π stacking of the peptide molecules than the 2-naphthylacetyl group, together with hydrogen bonding of the peptide scaffold. The nanostructure of the gel networks was studied by TEM and STEM microscopy and was found to correlate well with the elasticity of the gels. This study contributes to understanding the interplay between peptide and capping group structure on the formation of self-assembled low-molecular-weight peptide hydrogels. Moreover, the results presented here add the 1-naphthoyl group to the palette of capping groups available for the preparation of efficacious low-molecular-weight peptide-based hydrogels. Full article
(This article belongs to the Special Issue Advance in Supramolecular Gels)
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20 pages, 5200 KiB  
Article
The Effect of Branched Alkyl Chain Length on the Properties of Supramolecular Organogels from Mono-N-Alkylated Primary Oxalamides
by Khalid Azyat, Darren Makeiff, Bradley Smith, Mickie Wiebe, Steve Launspach, Ashley Wagner, Marianna Kulka and Nicolas Godbert
Gels 2023, 9(1), 5; https://doi.org/10.3390/gels9010005 - 22 Dec 2022
Cited by 3 | Viewed by 1308
Abstract
Mono-N-alkylated primary oxalamide derivatives with different sized branched alkyl tail-groups were excellent low molecular weight gelators for a variety of different organic solvents with different polarities and hydrogen-bonding abilities. Solvent-gelator interactions were analyzed using Hansen solubility parameters, while 1H NMR [...] Read more.
Mono-N-alkylated primary oxalamide derivatives with different sized branched alkyl tail-groups were excellent low molecular weight gelators for a variety of different organic solvents with different polarities and hydrogen-bonding abilities. Solvent-gelator interactions were analyzed using Hansen solubility parameters, while 1H NMR and FTIR spectroscopy were used to probe the driving forces for the supramolecular gelation. The molecular structures of the twin tail-groups did not significantly affect the supramolecular gelation behavior in different solvents. However, for select solvents, the molecular structures of the tail-groups did have a significant effect on gel properties such as the critical gelator concentration, thermal stability, gel stiffness, gel strength, network morphology, and molecular packing. Finally, metabolic activity studies showed that the primary alkyl oxalamide gelators had no effect on the metabolic activity of mouse immune cells, which suggests that the compounds are not cytotoxic and are suitable for use in biomedical applications. Full article
(This article belongs to the Special Issue Advance in Supramolecular Gels)
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24 pages, 8457 KiB  
Article
A Pharmaco-Technical Investigation of Thymoquinone and Peat-Sourced Fulvic Acid Nanoemulgel: A Combination Therapy
by Rahmuddin Khan, Mohd Aamir Mirza, Mohd Aqil, Nazia Hassan, Foziyah Zakir, Mohammad Javed Ansari and Zeenat Iqbal
Gels 2022, 8(11), 733; https://doi.org/10.3390/gels8110733 - 10 Nov 2022
Cited by 10 | Viewed by 1887
Abstract
Thymoquinone has a multitude of pharmacological effects and has been researched for a wide variety of indications, but with limited clinical success. It is associated with pharmaco-technical caveats such as hydrophobicity, high degradation, and a low oral bioavailability. A prudent approach warrants its [...] Read more.
Thymoquinone has a multitude of pharmacological effects and has been researched for a wide variety of indications, but with limited clinical success. It is associated with pharmaco-technical caveats such as hydrophobicity, high degradation, and a low oral bioavailability. A prudent approach warrants its usage through an alternative dermal route in combination with functional excipients to harness its potential for treating dermal afflictions, such as psoriasis. Henceforth, the present study explores a nanoformulation approach for designing a fulvic acid (peat-sourced)-based thymoquinone nanoemulsion gel (FTQ-NEG) for an enhanced solubility and improved absorption. The excipients, surfactant/co-surfactant, and oil selected for the o/w nanoemulsion (FTQ-NE) are Tween 80/Transcutol-P and kalonji oil. The formulation methodology includes high-energy ultrasonication complemented with a three-dimensional/factorial Box–Behnken design for guided optimization. The surface morphology assessment through scanning/transmission electron microscopy and fluorescence microscopy revealed a 100 nm spherical, globule-like structure of the prepared nanoemulsion. Furthermore, the optimized FTQ-NE had a zeta potential of −2.83 ± 0.14 Mv, refractive index of 1.415 ± 0.036, viscosity of 138.5 ± 3.08 mp, and pH of 5.8 ± 0.16, respectively. The optimized FTQ-NE was then formulated as a gel using Carbopol 971® (1%). The in vitro release analysis of the optimized FTQ-NEG showed a diffusion-dominant drug release (Higuchi model) for 48 h. The drug permeation flux observed for FTQ-NEG (3.64 μg/cm2/h) was much higher compared to that of the pure drug (1.77 mg/cm2/h). The results were further confirmed by confocal microscopy studies, which proved the improved penetration of thymoquinone through mice skin. Long-term stability studies of the purported formulation were also conducted and yielded satisfactory results. Full article
(This article belongs to the Special Issue Advance in Supramolecular Gels)
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16 pages, 6906 KiB  
Article
Fluorescent Quinoline-Based Supramolecular Gel for Selective and Ratiometric Sensing Zinc Ion with Multi-Modes
by Qingqing Han, Qingqing Wang, Aiping Gao, Xuefei Ge, Rong Wan and Xinhua Cao
Gels 2022, 8(10), 605; https://doi.org/10.3390/gels8100605 - 21 Sep 2022
Cited by 4 | Viewed by 1769
Abstract
A gelator 1 containing functional quinoline and Schiff base groups that could form organogels in DMF, DMSO, acetone, ethanol and 1,4-dioxane was designed and synthesized. The self-assembly process of geator 1 was characterized by field emission scanning electron microscopy (FESEM), UV-vis absorption spectroscopy, [...] Read more.
A gelator 1 containing functional quinoline and Schiff base groups that could form organogels in DMF, DMSO, acetone, ethanol and 1,4-dioxane was designed and synthesized. The self-assembly process of geator 1 was characterized by field emission scanning electron microscopy (FESEM), UV-vis absorption spectroscopy, fluorescence emission spectroscopy, Fourier transform infrared spectroscopy(FTIR), X-ray powder diffraction (XRD) and water contact angle. Under non-covalent interactions, gelator 1 self-assembled into microbelts and nanofiber structures with different surface wettability. Weak fluorescence was emitted from the solution and gel state of 1. Interestingly, gelator 1 exhibited good selectivity and sensitivity towards Zn2+ in solution and gel states along with its emission enhancement and change. The emission intensity at 423 nm of solution 1 in 1,4-dioxane was slightly enhanced, and a new emission peak appeared at 545 nm along with its intensity sequentially strengthened in the titration process. The obvious ratiometric detection process was presented with a limit of detection (LOD) of 5.51 μM. The detection mechanism was revealed by a theoretical calculation and NMR titration experiment, which was that Zn2+ induced the transition from trans- to cis- of molecule 1 and further coordinated with 1. This study will introduce a new method for the construction of functional self-assembly gel sensors for the detection of Zn2+. Full article
(This article belongs to the Special Issue Advance in Supramolecular Gels)
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15 pages, 2223 KiB  
Article
New Carbamates and Ureas: Comparative Ability to Gel Organic Solvents
by Gabriela Martínez-Mejía, Brenda Afrodita Bermeo-Solórzano, Silvia González, José Manuel del Río, Mónica Corea and Rogelio Jiménez-Juárez
Gels 2022, 8(7), 440; https://doi.org/10.3390/gels8070440 - 14 Jul 2022
Cited by 1 | Viewed by 1460
Abstract
Two series of novel amphiphilic compounds were synthesized based on carbamates and ureas structures, using a modification of the synthesis methods reported by bibliography. The compounds were tested for organic solvent removal in a model wastewater. The lipophilic group of all compounds was [...] Read more.
Two series of novel amphiphilic compounds were synthesized based on carbamates and ureas structures, using a modification of the synthesis methods reported by bibliography. The compounds were tested for organic solvent removal in a model wastewater. The lipophilic group of all compounds was a hexadecyl chain, while the hydrophilic substituent was changed with the same modifications in both series. The structures were confirmed by FT-IR, NMR, molecular dynamic simulation and HR-MS and their ability to gel organic solvents were compared. The SEM images showed the ureas had a greater ability to gel organic solvents than the carbamates and formed robust supramolecular networks, with surfaces of highly interwoven fibrillar spheres. The carbamates produced corrugated and smooth surfaces. The determination of the minimum gelation concentration demonstrated that a smaller quantity of the ureas (compared to the carbamates, measured as the weight percentage) was required to gel each solvent. This advantage of the ureas was attributed to their additional N-H bond, which is the only structural difference between the two types of compounds, and their structures were corroborated by molecular dynamic simulation. The formation of weak gels was demonstrated by rheological characterization, and they demonstrated to be good candidates for the removal organic solvents. Full article
(This article belongs to the Special Issue Advance in Supramolecular Gels)
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9 pages, 2122 KiB  
Article
Polyaniline Functionalized Peptide Self-Assembled Conductive Hydrogel for 3D Cell Culture
by Jieling Li, Yan Xue, Anhe Wang, Shaonan Tian, Qi Li and Shuo Bai
Gels 2022, 8(6), 372; https://doi.org/10.3390/gels8060372 - 13 Jun 2022
Cited by 5 | Viewed by 2403
Abstract
The functionalization of self-assembled peptide hydrogel is of great importance to broaden its applications in the field of biomedicine. In this work, conductive hydrogel is fabricated by introducing conductive polymer polyaniline into peptide self-assembled hydrogel. Compared with pure peptide formed hydrogel, the conductive [...] Read more.
The functionalization of self-assembled peptide hydrogel is of great importance to broaden its applications in the field of biomedicine. In this work, conductive hydrogel is fabricated by introducing conductive polymer polyaniline into peptide self-assembled hydrogel. Compared with pure peptide formed hydrogel, the conductive hydrogel exhibits enhanced conductivity, mechanical property and stability. In addition, the hydrogel is tested to be of great injectability and 3D bio-printability and could support the viability of encapsulated cells that are sensitive to electrical signals. It should have great application prospects in the preparation of tissue engineering scaffolds. Full article
(This article belongs to the Special Issue Advance in Supramolecular Gels)
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11 pages, 725 KiB  
Article
New Directions in Aesthetic Medicine: A Novel and Hybrid Filler Based on Hyaluronic Acid and Lactose Modified Chitosan
by Eva Daminato, Giulio Bianchini and Valerio Causin
Gels 2022, 8(5), 326; https://doi.org/10.3390/gels8050326 - 23 May 2022
Cited by 3 | Viewed by 2382
Abstract
Fillers based on crosslinked hyaluronic acid (HA) are becoming increasingly important in the field of aesthetic medicine, for example for treating wrinkles or for volumizing purposes. However, crosslinking agents are usually associated with toxicity and adverse reactions. The aim of this study is [...] Read more.
Fillers based on crosslinked hyaluronic acid (HA) are becoming increasingly important in the field of aesthetic medicine, for example for treating wrinkles or for volumizing purposes. However, crosslinking agents are usually associated with toxicity and adverse reactions. The aim of this study is the development of an innovative technology to manufacture high performance HA-based fillers using minimal amounts of crosslinking agent. In this work, new fillers based on HA, functionalized with different amounts of 1,4-butanediol diglycidyl ether (BDDE) (degree of modification ranging between 3.5% and 8.8%) and formulated with a lactose modified chitosan (CTL), were investigated. The relative quantities of these polymeric building blocks in the formulations were 20–25 and 5 mg/mL for HA and CTL, respectively. Due to its cationic nature, CTL could interact with the anionic HA and enhance the elastic properties of the filler. Fillers manufactured with this novel technology (HACL-CTL) were characterized and compared with several fillers available in the market. In particular, resistance against hyaluronidase, swelling, cohesivity and rheological properties were investigated. Cohesivity, resistance to hydrolysis and swelling of HACL-CTL were comparable to commercial products. However, HACL-CTL fillers showed excellent elastic performance that reached 94% of elasticity in response to shear stresses. Surprisingly, these fillers also showed a resistance to compression higher than that of currently marketed products, making them very promising for their lifting effect. Full article
(This article belongs to the Special Issue Advance in Supramolecular Gels)
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13 pages, 3344 KiB  
Article
Supramolecular Thixotropic Ionogel Electrolyte for Sodium Batteries
by Shipeng Chen, Li Feng, Xiaoji Wang, Yange Fan, Yubin Ke, Lin Hua, Zheng Li, Yimin Hou and Baoyu Xue
Gels 2022, 8(3), 193; https://doi.org/10.3390/gels8030193 - 20 Mar 2022
Cited by 1 | Viewed by 2325
Abstract
Owing to the potential of sodium as an alternative to lithium as charge carrier, increasing attention has been focused on the development of high-performance electrolytes for Na batteries in recent years. In this regard, gel-type electrolytes, which combine the outstanding ionic conductivity of [...] Read more.
Owing to the potential of sodium as an alternative to lithium as charge carrier, increasing attention has been focused on the development of high-performance electrolytes for Na batteries in recent years. In this regard, gel-type electrolytes, which combine the outstanding ionic conductivity of liquid electrolytes and the safety of solid electrolytes, demonstrate immense application prospects. However, most gel electrolytes not only need a number of specific techniques for molding, but also typically suffer from breakage, leading to a short service life and severe safety issues. In this study, a supramolecular thixotropic ionogel electrolyte is proposed to address these problems. This thixotropic electrolyte is formed by the supramolecular self-assembly of D-gluconic acetal-based gelator (B8) in an ionic liquid solution of a Na salt, which exhibits moldability, a high ionic conductivity, and a rapid self-healing property. The ionogel electrolyte is chemically stable to Na and exhibits a good Na+ transference number. In addition, the self-assembly mechanism of B8 and thixotropic mechanism of ionogel are investigated. The safe, low-cost and multifunctional ionogel electrolyte developed herein supports the development of future high-performance Na batteries. Full article
(This article belongs to the Special Issue Advance in Supramolecular Gels)
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12 pages, 5760 KiB  
Article
Novel Natural Glycyrrhetinic Acid-Derived Super Metal Gel and Its Highly Selective Dyes Removal
by Shengzhu Guo, Kaize Su, Huiji Yang, Wende Zheng, Zhen Zhang, Song Ang, Kun Zhang and Panpan Wu
Gels 2022, 8(3), 188; https://doi.org/10.3390/gels8030188 - 19 Mar 2022
Cited by 5 | Viewed by 1933
Abstract
Hydrogels play important roles in function materials, especially in wastewater treatment, that could solve the problems of microbial infections and dye pollutions. Herein, a natural glycyrrhetinic acid-derived gel was successfully constructed by forming hierarchical assemblies of the glycyrrhetinic acid derivatives (GA-O-09) with Cu [...] Read more.
Hydrogels play important roles in function materials, especially in wastewater treatment, that could solve the problems of microbial infections and dye pollutions. Herein, a natural glycyrrhetinic acid-derived gel was successfully constructed by forming hierarchical assemblies of the glycyrrhetinic acid derivatives (GA-O-09) with Cu2+. Interestingly, the GA-O-09/Cu2+ gel exhibited Cu2+-triggered shrinkage, which was helpful for spontaneous self-demolding through the shrinkage process with a precise amount of Cu2+. Moreover, the gel showed excellent antimicrobial activity against Staphylococcus aureus and methicillin-resistant Staphylococcus aureus (MRSA) with minimum inhibitory concentrations (MICs) at 2.5 μg/mL and 5.0 μg/mL, respectively. Furthermore, the resultant GA-O-09/Cu2+ gel showed an excellent performance in dyes removal; the adsorption capacity at equilibrium (qe) could reach 82.91 mg/g according to a pseudo-second-order model, and it was better than most reported dye adsorbent materials. The experimental result suggested that the electrostatic interactions of the hydrogel with the cationic dyes and the hydrogel swelling were responsible for the possible dye removal mechanism of GA-O-09/Cu2+ gel. Therefore, our study holds the promise of a better future, for such a hydrogel could be used as an antibacterial and dye removal material. Full article
(This article belongs to the Special Issue Advance in Supramolecular Gels)
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