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Rational Design and Application of Functional Hydrogels

A special issue of International Journal of Molecular Sciences (ISSN 1422-0067). This special issue belongs to the section "Materials Science".

Deadline for manuscript submissions: 31 August 2024 | Viewed by 12698

Special Issue Editors

Department of Biophysics, School of Physics, Nanjing University, Nanjing 210093, China
Interests: hydrogels; biomimetic nanomaterials; peptide self-assembly; biomechanics; molecular engineering
Special Issues, Collections and Topics in MDPI journals
School of Physics, Nanjing University, Nanjing 210093, China
Interests: protein; peptide; hydrogel; single molecule; mechanical properties; self-assembly; force spectroscopy; biomaterials
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues, 

As the superstar of attractive soft materials, hydrogels have been developed and widely studied for the last decades. Due to the advantages of high water contents, tunable mechanical properties and excellent biocompatibility, hydrogels are materials choice for many biomedical applications, such as synthetic extracellular matrix (ECM) for cell culture, synthetic tissues, regenerative medicine and drug delivery. Recently, hydrogel materials were further endowed with more abundant functions including strain sensors, biomedical actuators and soft robotics. In order to achieve the various functionality, the building blocks of the hydrogels, as well as the hydrogel network, need to be designed and fabricated accordingly, following the principle of bottom-up which means that the design and structure of bottom molecules may significantly determine the bulk properties.  

The goal of this Special Issue is to focus attention on the rational design and functionalization of hydrogels. We invite to contributions of reviews and/or original papers reporting new results about the building blocks design, network design and functional design of hydrogels as well as the applications in the field including cell culture, tissue engineering, interfacial adhesion, flexible electronics and so on. Hydrogels formed using various building blocks such as polymers, peptides, proteins, DNA/RNA and composites of them were all acceptable. Manuscripts that address recent advances in the design principle of hydrogels with special properties and approaches to endow hydrogels with new functions are especially welcome.

Dr. Bin Xue
Dr. Yi Cao
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.

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Keywords

  • hydrogel network
  • mechanical property
  • material engineering
  • biomedical engineering
  • soft actuator
  • biosensing
  • tissue engineering

Published Papers (5 papers)

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Research

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15 pages, 3304 KiB  
Article
Comparison of Osteoconductive Ability of Two Types of Cholesterol-Bearing Pullulan (CHP) Nanogel-Hydrogels Impregnated with BMP-2 and RANKL-Binding Peptide: Bone Histomorphometric Study in a Murine Calvarial Defect Model
by Cangyou Xie, Fatma Rashed, Yosuke Sasaki, Masud Khan, Jia Qi, Yuri Kubo, Yoshiro Matsumoto, Shinichi Sawada, Yoshihiro Sasaki, Takashi Ono, Tohru Ikeda, Kazunari Akiyoshi and Kazuhiro Aoki
Int. J. Mol. Sci. 2023, 24(11), 9751; https://doi.org/10.3390/ijms24119751 - 5 Jun 2023
Viewed by 1955
Abstract
The receptor activator of NF-κB ligand (RANKL)-binding peptide is known to accelerate bone morphogenetic protein (BMP)-2-induced bone formation. Cholesterol-bearing pullulan (CHP)-OA nanogel-crosslinked PEG gel (CHP-OA nanogel-hydrogel) was shown to release the RANKL-binding peptide sustainably; however, an appropriate scaffold for peptide-accelerated bone formation is [...] Read more.
The receptor activator of NF-κB ligand (RANKL)-binding peptide is known to accelerate bone morphogenetic protein (BMP)-2-induced bone formation. Cholesterol-bearing pullulan (CHP)-OA nanogel-crosslinked PEG gel (CHP-OA nanogel-hydrogel) was shown to release the RANKL-binding peptide sustainably; however, an appropriate scaffold for peptide-accelerated bone formation is not determined yet. This study compares the osteoconductivity of CHP-OA hydrogel and another CHP nanogel, CHP-A nanogel-crosslinked PEG gel (CHP-A nanogel–hydrogel), in the bone formation induced by BMP-2 and the peptide. A calvarial defect model was performed in 5-week-old male mice, and scaffolds were placed in the defect. In vivo μCT was performed every week. Radiological and histological analyses after 4 weeks of scaffold placement revealed that the calcified bone area and the bone formation activity at the defect site in the CHP-OA hydrogel were significantly lower than those in the CHP-A hydrogel when the scaffolds were impregnated with both BMP-2 and the RANKL-binding peptide. The amount of induced bone was similar in both CHP-A and CHP-OA hydrogels when impregnated with BMP-2 alone. In conclusion, CHP-A hydrogel could be an appropriate scaffold compared to the CHP-OA hydrogel when the local bone formation was induced by the combination of RANKL-binding peptide and BMP-2, but not by BMP-2 alone. Full article
(This article belongs to the Special Issue Rational Design and Application of Functional Hydrogels)
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12 pages, 3003 KiB  
Article
Engineering Bio-Adhesives Based on Protein–Polysaccharide Phase Separation
by Zoobia Bashir, Wenting Yu, Zhengyu Xu, Yiran Li, Jiancheng Lai, Ying Li, Yi Cao and Bin Xue
Int. J. Mol. Sci. 2022, 23(17), 9987; https://doi.org/10.3390/ijms23179987 - 1 Sep 2022
Cited by 7 | Viewed by 2279
Abstract
Glue-type bio-adhesives are in high demand for many applications, including hemostasis, wound closure, and integration of bioelectronic devices, due to their injectable ability and in situ adhesion. However, most glue-type bio-adhesives cannot be used for short-term tissue adhesion due to their weak instant [...] Read more.
Glue-type bio-adhesives are in high demand for many applications, including hemostasis, wound closure, and integration of bioelectronic devices, due to their injectable ability and in situ adhesion. However, most glue-type bio-adhesives cannot be used for short-term tissue adhesion due to their weak instant cohesion. Here, we show a novel glue-type bio-adhesive based on the phase separation of proteins and polysaccharides by functionalizing polysaccharides with dopa. The bio-adhesive exhibits increased adhesion performance and enhanced phase separation behaviors. Because of the cohesion from phase separation and adhesion from dopa, the bio-adhesive shows excellent instant and long-term adhesion performance for both organic and inorganic substrates. The long-term adhesion strength of the bio-glue on wet tissues reached 1.48 MPa (shear strength), while the interfacial toughness reached ~880 J m−2. Due to the unique phase separation behaviors, the bio-glue can even work normally in aqueous environments. At last, the feasibility of this glue-type bio-adhesive in the adhesion of various visceral tissues in vitro was demonstrated to have excellent biocompatibility. Given the convenience of application, biocompatibility, and robust bio-adhesion, we anticipate the bio-glue may find broad biomedical and clinical applications. Full article
(This article belongs to the Special Issue Rational Design and Application of Functional Hydrogels)
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12 pages, 2049 KiB  
Article
Gradual Stress-Relaxation of Hydrogel Regulates Cell Spreading
by Wenting Yu, Wenxu Sun, Huiyan Chen, Juan Wang, Bin Xue and Yi Cao
Int. J. Mol. Sci. 2022, 23(9), 5170; https://doi.org/10.3390/ijms23095170 - 5 May 2022
Cited by 6 | Viewed by 3224
Abstract
There is growing evidence that the mechanical properties of extracellular matrices (ECMs), including elasticity and stress-relaxation, greatly influence the function and form of the residing cells. However, the effects of elasticity and stress-relaxation are often correlated, making the study of the effect of [...] Read more.
There is growing evidence that the mechanical properties of extracellular matrices (ECMs), including elasticity and stress-relaxation, greatly influence the function and form of the residing cells. However, the effects of elasticity and stress-relaxation are often correlated, making the study of the effect of stress-relaxation on cellular behaviors difficult. Here, we designed a hybrid network hydrogel with a controllable stress-relaxation gradient and a constant elasticity. The hydrogel is crosslinked by covalent bonds and dynamic peptide-metal ion coordination interactions. The stress-relaxation gradient is controlled by spatially controlling the coordination and covalent crosslinker ratios. The different parts of the hydrogel exhibit distinct stress-relaxation amplitudes but the have same stress-relaxation timescale. Based on this hydrogel, we investigate the influence of hydrogel stress-relaxation on cell spreading. Our results show that the spreading of cells is suppressed at an increasing stress-relaxation amplitude with a fixed elasticity and stress-relaxation timescale. Our study provides a universal route to tune the stress-relaxation of hydrogels without changing their components and elasticity, which may be valuable for systematic investigations of the stress-relaxation gradient in cell cultures and organoid constructions. Full article
(This article belongs to the Special Issue Rational Design and Application of Functional Hydrogels)
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12 pages, 2360 KiB  
Article
Tuning Strain Stiffening of Protein Hydrogels by Charge Modification
by Jie Gu, Yu Guo, Yiran Li, Juan Wang, Wei Wang, Yi Cao and Bin Xue
Int. J. Mol. Sci. 2022, 23(6), 3032; https://doi.org/10.3390/ijms23063032 - 11 Mar 2022
Cited by 5 | Viewed by 2862
Abstract
Strain-stiffening properties derived from biological tissue have been widely observed in biological hydrogels and are essential in mimicking natural tissues. Although strain-stiffening has been studied in various protein-based hydrogels, effective approaches for tuning the strain-stiffening properties of protein hydrogels have rarely been explored. [...] Read more.
Strain-stiffening properties derived from biological tissue have been widely observed in biological hydrogels and are essential in mimicking natural tissues. Although strain-stiffening has been studied in various protein-based hydrogels, effective approaches for tuning the strain-stiffening properties of protein hydrogels have rarely been explored. Here, we demonstrated a new method to tune the strain-stiffening amplitudes of protein hydrogels. By adjusting the surface charge of proteins inside the hydrogel using negatively/positively charged molecules, the strain-stiffening amplitudes could be quantitively regulated. The strain-stiffening of the protein hydrogels could even be enhanced 5-fold under high deformations, while the bulk property, recovery ability and biocompatibility remained almost unchanged. The tuning of strain-stiffening amplitudes using different molecules or in different protein hydrogels was further proved to be feasible. We anticipate that surface charge adjustment of proteins in hydrogels represents a general principle to tune the strain-stiffening property and can find wide applications in regulating the mechanical behaviors of protein-based hydrogels. Full article
(This article belongs to the Special Issue Rational Design and Application of Functional Hydrogels)
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Review

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53 pages, 3493 KiB  
Review
Advancements in Regenerative Hydrogels in Skin Wound Treatment: A Comprehensive Review
by Gabriel Olteanu, Sorinel Marius Neacșu, Florin Alexandru Joița, Adina Magdalena Musuc, Elena Carmen Lupu, Corina-Bianca Ioniță-Mîndrican, Dumitru Lupuliasa and Magdalena Mititelu
Int. J. Mol. Sci. 2024, 25(7), 3849; https://doi.org/10.3390/ijms25073849 - 29 Mar 2024
Viewed by 1122
Abstract
This state-of-the-art review explores the emerging field of regenerative hydrogels and their profound impact on the treatment of skin wounds. Regenerative hydrogels, composed mainly of water-absorbing polymers, have garnered attention in wound healing, particularly for skin wounds. Their unique properties make them well [...] Read more.
This state-of-the-art review explores the emerging field of regenerative hydrogels and their profound impact on the treatment of skin wounds. Regenerative hydrogels, composed mainly of water-absorbing polymers, have garnered attention in wound healing, particularly for skin wounds. Their unique properties make them well suited for tissue regeneration. Notable benefits include excellent water retention, creating a crucially moist wound environment for optimal healing, and facilitating cell migration, and proliferation. Biocompatibility is a key feature, minimizing adverse reactions and promoting the natural healing process. Acting as a supportive scaffold for cell growth, hydrogels mimic the extracellular matrix, aiding the attachment and proliferation of cells like fibroblasts and keratinocytes. Engineered for controlled drug release, hydrogels enhance wound healing by promoting angiogenesis, reducing inflammation, and preventing infection. The demonstrated acceleration of the wound healing process, particularly beneficial for chronic or impaired healing wounds, adds to their appeal. Easy application and conformity to various wound shapes make hydrogels practical, including in irregular or challenging areas. Scar minimization through tissue regeneration is crucial, especially in cosmetic and functional regions. Hydrogels contribute to pain management by creating a protective barrier, reducing friction, and fostering a soothing environment. Some hydrogels, with inherent antimicrobial properties, aid in infection prevention, which is a crucial aspect of successful wound healing. Their flexibility and ability to conform to wound contours ensure optimal tissue contact, enhancing overall treatment effectiveness. In summary, regenerative hydrogels present a promising approach for improving skin wound healing outcomes across diverse clinical scenarios. This review provides a comprehensive analysis of the benefits, mechanisms, and challenges associated with the use of regenerative hydrogels in the treatment of skin wounds. In this review, the authors likely delve into the application of rational design principles to enhance the efficacy and performance of hydrogels in promoting wound healing. Through an exploration of various methodologies and approaches, this paper is poised to highlight how these principles have been instrumental in refining the design of hydrogels, potentially revolutionizing their therapeutic potential in addressing skin wounds. By synthesizing current knowledge and highlighting potential avenues for future research, this review aims to contribute to the advancement of regenerative medicine and ultimately improve clinical outcomes for patients with skin wounds. Full article
(This article belongs to the Special Issue Rational Design and Application of Functional Hydrogels)
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