Properties and Structure of Hydrogel-Related Materials

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

Deadline for manuscript submissions: 30 June 2024 | Viewed by 7563

Special Issue Editors


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Guest Editor
State Key Laboratory of Separation Membranes and Membrane Processes, School of Materials Science and Engineering, Tiangong University, Tianjin 300387, China
Interests: nanocomposite hydrogel; hydrogel nanofiber; photonic crystal hydrogel sensor; biomedical hydrogel

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Guest Editor
College of Polymer Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, China
Interests: polymer rheology; tough gel; flexible device
College of Polymer Science and Engineering, Sichuan University, Chengdu 610065, China
Interests: fracture mechanics; adhesion; tough gel
Institute for Chemical Reaction Design and Discovery (WPI-ICReDD), Hokkaido University, Sapporo 001-0021, Japan
Interests: polymer gel; functional material; fracture mechanics
Special Issues, Collections and Topics in MDPI journals
Faculty of Advanced Life Science, Hokkaido University, Sapporo 001-0021, Japan
Interests: tough gel; mechanochemistry in gel; self-growing material; polymer physics

Special Issue Information

Dear Colleagues,

It is now well recognized that the birth of synthetic hydrogels in 1960, by O. Wichterle and D. Lim, marked the beginning of a new era in the science and technology of hydrogels. Hydrogels are made of hydrophilic polymer networks swollen in water or other fluids, integrating solid (elastic) and liquid (viscous) properties. Especially in the past three decades, hydrogels have also been extensively explored and widely used in diverse interdisciplinary science and engineering applications such as fracture mechanics, mechanochemistry, wound dressings, scaffolds for tissue engineering, contact lenses, absorbents in waste management, coating, drug delivery, water treatment, sensors, flexible electronics, and soft robots. However, most of the conventional hydrogels composed of a single network (SN) usually suffer from mechanical weakness (toughness < 10 J m−2, strength < 50 kPa, stiffness < 10 kPa), which greatly limits their extensive uses for engineering applications requiring high mechanical properties. Over the last few decades, intensive efforts have led to synthesizing hydrogels that possess extreme mechanical properties, such as double-network (DN) gels, slide-ring (SR) gels, tetra-PEG gels, nanocomposite (NC) gels, hybrid gels, polyampholytes gels, phase-separated gels, and freeze-casting gels. As a landmark tough material, DN gel has intrinsic tough mechanical properties due to its unique two contrasting network structures. The theory of sacrificial bond and energy dissipation adequately demonstrates the universality of the toughing gel and can be easily understood by a general audience. Although many aspects of the bridging relationship between the structure and properties of gel have been clarified so far, many phenomena and underlying mechanisms are still left unsolved. We believe it is time to revisit the mechanical properties and network of gels in marking a possible second beginning of a new era in the science of gels. We look forward to the submission of new results on the properties and structure of gels. The submission of both theoretical and experimental studies is welcome.

Prof. Dr. Qingsong Zhang
Prof. Dr. Yanan Ye
Dr. Wei Cui
Dr. Yong Zheng
Dr. Qifeng Mu
Guest Editors

Manuscript Submission Information

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Keywords

  • gel and network
  • tough gel
  • gel rheology
  • gel adhesion
  • photonic crystal hydrogel sensor

Published Papers (4 papers)

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Research

20 pages, 5319 KiB  
Article
Modulation of Methacrylated Hyaluronic Acid Hydrogels Enables Their Use as 3D Cultured Model
by Ornella Ursini, Maddalena Grieco, Carla Sappino, Agostina Lina Capodilupo, Sara Maria Giannitelli, Emanuele Mauri, Alessio Bucciarelli, Chiara Coricciati, Valeria de Turris, Giuseppe Gigli, Lorenzo Moroni and Barbara Cortese
Gels 2023, 9(10), 801; https://doi.org/10.3390/gels9100801 - 05 Oct 2023
Viewed by 1783
Abstract
Bioengineered hydrogels represent physiologically relevant platforms for cell behaviour studies in the tissue engineering and regenerative medicine fields, as well as in in vitro disease models. Hyaluronic acid (HA) is an ideal platform since it is a natural biocompatible polymer that is widely [...] Read more.
Bioengineered hydrogels represent physiologically relevant platforms for cell behaviour studies in the tissue engineering and regenerative medicine fields, as well as in in vitro disease models. Hyaluronic acid (HA) is an ideal platform since it is a natural biocompatible polymer that is widely used to study cellular crosstalk, cell adhesion and cell proliferation, and is one of the major components of the extracellular matrix (ECM). We synthesised chemically modified HA with photo-crosslinkable methacrylated groups (HA-MA) in aqueous solutions and in strictly monitored pH and temperature conditions to obtain hydrogels with controlled bulk properties. The physical and chemical properties of the different HA-MA hydrogels were investigated via rheological studies, mechanical testing and scanning electron microscopy (SEM) imaging, which allowed us to determine the optimal biomechanical properties and develop a biocompatible scaffold. The morphological evolution processes and proliferation rates of glioblastoma cells (U251-MG) cultured on HA-MA surfaces were evaluated by comparing 2D structures with 3D structures, showing that the change in dimensionality impacted cell functions and interactions. The cell viability assays and evaluation of mitochondrial metabolism showed that the hydrogels did not interfere with cell survival. In addition, morphological studies provided evidence of cell–matrix interactions that promoted cell budding from the spheroids and the invasiveness in the surrounding environment. Full article
(This article belongs to the Special Issue Properties and Structure of Hydrogel-Related Materials)
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16 pages, 3301 KiB  
Article
Synthesis and Characterization of Sulfur Nanoparticles of Citrus limon Extract Embedded in Nanohydrogel Formulation: In Vitro and In Vivo Studies
by Hadia Baloch, Aisha Siddiqua, Asif Nawaz, Muhammad Shahid Latif, Syeda Qurbat Zahra, Suliman Yousef Alomar, Naushad Ahmad and Tarek M. Elsayed
Gels 2023, 9(4), 284; https://doi.org/10.3390/gels9040284 - 01 Apr 2023
Cited by 4 | Viewed by 2176
Abstract
The study aimed to synthesize non-noxious, clean, reliable, and green sulfur nanoparticles (SNPs) from Citrus limon leaves. The synthesized SNPs were used to analyze particle size, zeta potential, UV–visible spectroscopy, SEM, and ATR-FTIR. The prepared SNPs exhibited a globule size of 55.32 ± [...] Read more.
The study aimed to synthesize non-noxious, clean, reliable, and green sulfur nanoparticles (SNPs) from Citrus limon leaves. The synthesized SNPs were used to analyze particle size, zeta potential, UV–visible spectroscopy, SEM, and ATR-FTIR. The prepared SNPs exhibited a globule size of 55.32 ± 2.15 nm, PDI value of 0.365 ± 0.06, and zeta potential of −12.32 ± 0.23 mV. The presence of SNPs was confirmed by UV–visible spectroscopy in the range of 290 nm. The SEM image showed that the particles were spherical with a size of 40 nm. The ATR-FTIR study showed no interaction, and all the major peaks were preserved in the formulations. An antimicrobial and antifungal study of SNPs was carried out against Gram-positive bacteria (Staph. aureus, Bacillus), Gram-negative bacteria (E. coli and Bordetella), and fungal strains (Candida albicans). The study showed that Citrus limon extract SNPs exhibited better antimicrobial and antifungal activities against Staph. aureus, Bacillus, E. coli, Bordetella, and Candida albicans at a minimal inhibitory concentration of 50 μg/mL. Different antibiotics were used alone and in combination with SNPs of Citrus limon extract to evaluate their activity against various strains of bacteria and fungal strains. The study showed that using SNPs of Citrus limon extract with antibiotics has a synergistic effect against Staph.aureus, Bacillus, E. coli, Bordetella, and Candida albicans. SNPs were embedded in nanohydrogel formulations for in vivo (wound healing) studies. In preclinical studies, SNPs of Citrus limon extract embedded within a nanohydrogel formulation (NHGF4) have shown promising results. To be widely used in clinical settings, further studies are needed to evaluate their safety and efficacy in human volunteers. Full article
(This article belongs to the Special Issue Properties and Structure of Hydrogel-Related Materials)
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13 pages, 3833 KiB  
Article
Enhanced Rupture Force in a Cut-Dispersed Double-Network Hydrogel
by Shilei Zhu, Dongdong Yan, Lin Chen, Yan Wang, Fengbo Zhu, Yanan Ye, Yong Zheng, Wenwen Yu and Qiang Zheng
Gels 2023, 9(2), 158; https://doi.org/10.3390/gels9020158 - 16 Feb 2023
Cited by 1 | Viewed by 1373
Abstract
The Kirigami approach is an effective way to realize controllable deformation of intelligent materials via introducing cuts into bulk materials. For materials ranging from ordinary stiff materials such as glass, ceramics, and metals to soft materials, including ordinary hydrogels and elastomers, all of [...] Read more.
The Kirigami approach is an effective way to realize controllable deformation of intelligent materials via introducing cuts into bulk materials. For materials ranging from ordinary stiff materials such as glass, ceramics, and metals to soft materials, including ordinary hydrogels and elastomers, all of them are all sensitive to the presence of cuts, which usually act as defects to deteriorate mechanical properties. Herein, we study the influence of the cuts on the mechanical properties by introducing “dispersed macro-scale cuts” into a model tough double network (DN) hydrogel (named D-cut gel), which consists of a rigid and brittle first network and a ductile stretchable second network. For comparison, DN gels with “continuous cuts” having the same number of interconnected cuts (named C-cut gel) were chosen. The fracture tests of D-cut gel and C-cut gel with different cut patterns were performed. The fracture observation revealed that crack blunting occurred at each cut tip, and a large wrinkle-like zone was formed where the wrinkles were parallel to the propagation direction of the cut. By utilizing homemade circular polarizing optical systems, we found that introducing dispersed cuts increases the rupture force by homogenizing the stress around the crack tip surrounding every cut, which reduces stress concentration in one certain cut. We believe this work reveals the fracture mechanism of tough soft materials with a kirigami cut structure, which should guide the design of advanced soft and tough materials along this line. Full article
(This article belongs to the Special Issue Properties and Structure of Hydrogel-Related Materials)
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19 pages, 5877 KiB  
Article
Metal-Coordinated Dynamics and Viscoelastic Properties of Double-Network Hydrogels
by Shilei Zhu, Yan Wang, Zhe Wang, Lin Chen, Fengbo Zhu, Yanan Ye, Yong Zheng, Wenwen Yu and Qiang Zheng
Gels 2023, 9(2), 145; https://doi.org/10.3390/gels9020145 - 09 Feb 2023
Cited by 2 | Viewed by 1578
Abstract
Biological soft tissues are intrinsically viscoelastic materials which play a significant role in affecting the activity of cells. As potential artificial alternatives, double-network (DN) gels, however, are pure elastic and mechanically time independent. The viscoelasticization of DN gels is an urgent challenge in [...] Read more.
Biological soft tissues are intrinsically viscoelastic materials which play a significant role in affecting the activity of cells. As potential artificial alternatives, double-network (DN) gels, however, are pure elastic and mechanically time independent. The viscoelasticization of DN gels is an urgent challenge in enabling DN gels to be used for advanced development of biomaterial applications. Herein, we demonstrate a simple approach to regulate the viscoelasticity of tough double-network (DN) hydrogels by forming sulfonate–metal coordination. Owing to the dynamic nature of the coordination bonds, the resultant hydrogels possess highly viscoelastic, mechanical time-dependent, and self-recovery properties. Rheological measurements are performed to investigate the linear dynamic mechanical behavior at small strains. The tensile tests and cyclic tensile tests are also systematically performed to evaluate the rate-dependent large deformation mechanical behaviors and energy dissipation behaviors of various ion-loaded DN hydrogels. It has been revealed based on the systematic analysis that robust strong sulfonate–Zr4+ coordination interactions not only serve as dynamic crosslinks imparting viscoelastic rate-dependent mechanical performances, but also strongly affect the relative strength of the first PAMPS network, thereby increasing the yielding stress σy and the fracture stress at break σb and reducing the stretch ratio at break λb. It is envisioned that the viscoelasticization of DN gels enables versatile applications in the biomedical and engineering fields. Full article
(This article belongs to the Special Issue Properties and Structure of Hydrogel-Related Materials)
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