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Polymers
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Composite Hydrogels towards Next-Generation Functional Materials and Devices
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Composite Hydrogels towards Next-Generation Functional Materials and Devices

A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Polymer Composites and Nanocomposites".

Deadline for manuscript submissions: 15 June 2024 | Viewed by 18238

Special Issue Editors

Prof. Dr. Boxin Zhao

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Guest Editor
Department of Chemical Engineering, University of Waterloo, Waterloo, ON N2L 3G1, Canada
Interests: surface science and bionanomaterials; interfacial materials engineering for advanced manufacturing; biomimicry and biomimetic materials; multifunctional polymers and nanocomposites; biopolymer; hydrogels and healthcare materials; advanced coating and adhesive bonding technology
Special Issues, Collections and Topics in MDPI journals
Prof. Dr. Bruce P. Lee

E-Mail Website
Guest Editor
Department of Biomedical Engineering, Michigan Technological University, Houghton, MI 49931, USA
Interests: biomimetic materials; antimicrobial polymers; tissue adhesives; biointerface; smart materials
Special Issues, Collections and Topics in MDPI journals
Prof. Dr. Wei Zhang

E-Mail Website
Guest Editor
School of Materials Science and Engineering, Southeast University, Nanjing, China
Interests: flexible energy storage materials; functional polymer hydrogels; interfacial phenomenon and surface properties; bio-inspired structures and materials

Special Issue Information

Dear Colleagues, 

Hydrogels are a unique class of functional materials that possess three-dimensional polymeric networks and contain a large amount of water; such special structure and property endow the hydrogels with great potentials in numerous applications, including chemical and biomedical engineering, electronics, energy storage and conversion, water purification and collection, adhesives, actuators, and so on.  Even though pristine hydrogels usually exhibit weak strength and have limited functionalities; they can be readily combined with a variety of other polymers and additives to make composite hydrogels so as to deliver many desired properties. For instance, double-network polymers have been exploited in hydrogels for desired toughness and strength; hydrogels with adhesive moieties are being actively developed for wet adhesives; furthermore, hydrogels in combination with conductive fillers, such as metal nanoparticles, carbon nanotubes, conductive polymers, have been actively investigated for the development of sensors, supercapacitors, wearable/implantable electronics and many other functional devices. 

Recognizing the importance and growing interests in composite hydrogels, we would like to invite you to submit your original work (a communication or a full paper) or a review article to this Special Issue. The topics of interest include but are not limited to biomedical hydrogels, conductive hydrogels, hydrogels for energy storage, sustainable hydrogels, hydrogel adhesives, hydrogel actuators, etc. All contributions on the design principles, chemistry, characterization, morphology, multifunctional properties, simulation and modeling relative to composite hydrogels, as well as those focused on the development of hydrogel-based or hydrogel-related functional materials and devices are welcome.

Prof. Dr. Boxin Zhao
Prof. Dr. Bruce P. Lee
Prof. Dr. Wei Zhang
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. Polymers 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

  • nanocomposite hydrogels
  • biomedical hydrogels
  • sustainable hydrogels
  • adhesive hydrogels
  • smart hydrogels
  • tough hydrogels
  • conductive hydrogels
  • hybrid hydrogels
  • hydrogel chemistry
  • hydrogel mechanical properties
  • hydrogel actuator
  • hydrogel for flexible electronics
  • hydrogel for energy storage

Published Papers (7 papers)

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Research

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23 pages, 6911 KiB  
Article
Utilizing Robust Design to Optimize Composite Bioadhesive for Promoting Dermal Wound Repair
by Rattapol Pinnaratip, Zhongtian Zhang, Ariana Smies, Pegah Kord Forooshani, Xiaoqing Tang, Rupak M Rajachar and Bruce P. Lee
Polymers 2023, 15(8), 1905; https://doi.org/10.3390/polym15081905 - 15 Apr 2023
Viewed by 1061
Abstract
Catechol-modified bioadhesives generate hydrogen peroxide (H2O2) during the process of curing. A robust design experiment was utilized to tune the H2O2 release profile and adhesive performance of a catechol-modified polyethylene glycol (PEG) containing silica particles (SiP). [...] Read more.
Catechol-modified bioadhesives generate hydrogen peroxide (H2O2) during the process of curing. A robust design experiment was utilized to tune the H2O2 release profile and adhesive performance of a catechol-modified polyethylene glycol (PEG) containing silica particles (SiP). An L9 orthogonal array was used to determine the relative contributions of four factors (the PEG architecture, PEG concentration, phosphate-buffered saline (PBS) concentration, and SiP concentration) at three factor levels to the performance of the composite adhesive. The PEG architecture and SiP wt% contributed the most to the variation in the results associated with the H2O2 release profile, as both factors affected the crosslinking of the adhesive matrix and SiP actively degraded the H2O2. The predicted values from this robust design experiment were used to select the adhesive formulations that released 40–80 µM of H2O2 and evaluate their ability to promote wound healing in a full-thickness murine dermal wound model. The treatment with the composite adhesive drastically increased the rate of the wound healing when compared to the untreated controls, while minimizing the epidermal hyperplasia. The release of H2O2 from the catechol and soluble silica from the SiP contributed to the recruitment of keratinocytes to the wound site and effectively promoted the wound healing. Full article
(This article belongs to the Special Issue Composite Hydrogels towards Next-Generation Functional Materials and Devices)
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13 pages, 20853 KiB  
Article
3D Printed Hydrogel Microneedle Arrays for Interstitial Fluid Biomarker Extraction and Colorimetric Detection
by Mahmood Razzaghi, Amir Seyfoori, Erik Pagan, Esfandyar Askari, Alireza Hassani Najafabadi and Mohsen Akbari
Polymers 2023, 15(6), 1389; https://doi.org/10.3390/polym15061389 - 10 Mar 2023
Cited by 10 | Viewed by 7148
Abstract
To treat and manage chronic diseases, it is necessary to continuously monitor relevant biomarkers and modify treatment as the disease state changes. Compared to other bodily fluids, interstitial skin fluid (ISF) is a good choice for identifying biomarkers because it has a molecular [...] Read more.
To treat and manage chronic diseases, it is necessary to continuously monitor relevant biomarkers and modify treatment as the disease state changes. Compared to other bodily fluids, interstitial skin fluid (ISF) is a good choice for identifying biomarkers because it has a molecular composition most similar to blood plasma. Herein, a microneedle array (MNA) is presented to extract ISF painlessly and bloodlessly. The MNA is made of crosslinked poly(ethylene glycol) diacrylate (PEGDA), and an optimal balance of mechanical properties and absorption capability is suggested. Besides, the effect of needles’ cross-section shape on skin penetration is studied. The MNA is integrated with a multiplexed sensor that provides a color change in a biomarker concentration-dependent manner based on the relevant reactions for colorimetric detection of pH and glucose biomarkers. The developed device enables diagnosis by visual inspection or quantitative red, green, and blue (RGB) analysis. The outcomes of this study show that MNA can successfully identify biomarkers in interstitial skin fluid in a matter of minutes. The home-based long-term monitoring and management of metabolic diseases will benefit from such practical and self-administrable biomarker detection. Full article
(This article belongs to the Special Issue Composite Hydrogels towards Next-Generation Functional Materials and Devices)
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13 pages, 3088 KiB  
Article
Hydrogel/β-FeOOH-Coated Poly(vinylidene fluoride) Membranes with Superhydrophilicity/Underwater Superoleophobicity Facilely Fabricated via an Aqueous Approach for Multifunctional Applications
by Yin Tang, Tang Zhu, Huichao Liu, Zheng Tang, Xingwen Kuang, Yongna Qiao, Hao Zhang and Caizhen Zhu
Polymers 2023, 15(4), 839; https://doi.org/10.3390/polym15040839 - 08 Feb 2023
Cited by 5 | Viewed by 1492
Abstract
Hydrogel coatings that can endow various substrates with superior properties (e.g., biocompatibility, hydrophilicity, and lubricity) have wide applications in the fields of oil/water separation, antifouling, anti-bioadhesion, etc. Currently, the engineering of multifunctional hydrogel-coated materials with superwettability and water purification property using a simple [...] Read more.
Hydrogel coatings that can endow various substrates with superior properties (e.g., biocompatibility, hydrophilicity, and lubricity) have wide applications in the fields of oil/water separation, antifouling, anti-bioadhesion, etc. Currently, the engineering of multifunctional hydrogel-coated materials with superwettability and water purification property using a simple and sustainable strategy is still largely uninvestigated but has a beneficial effect on the world. Herein, we successfully prepared poly(2-acrylamido-2-methyl-1-propanesulfonic acid) hydrogel/β-FeOOH-coated poly(vinylidene fluoride) (PVDF/PAMPS/β-FeOOH) membrane through free-radical polymerization and the in situ mineralization process. In this work, owing to the combination of hydrophilic PAMPS hydrogel coating and β-FeOOH nanorods anchored onto PVDF membrane, the resultant PVDF/PAMPS/β-FeOOH membrane achieved outstanding superhydrophilicity/underwater superoleophobicity. Moreover, the membrane not only effectively separated surfactant-stabilized oil/water emulsions, but also possessed a long-term use capacity. In addition, excellent photocatalytic activity against organic pollutants was demonstrated so that the PVDF/PAMPS/β-FeOOH membrane could be utilized to deal with wastewater. It is envisioned that these hydrogel/β-FeOOH-coated PVDF membranes have versatile applications in the fields of oil/water separation and wastewater purification. Full article
(This article belongs to the Special Issue Composite Hydrogels towards Next-Generation Functional Materials and Devices)
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17 pages, 6144 KiB  
Article
Cell-Laden Composite Hydrogel Bioinks with Human Bone Allograft Particles to Enhance Stem Cell Osteogenesis
by Hadis Gharacheh and Murat Guvendiren
Polymers 2022, 14(18), 3788; https://doi.org/10.3390/polym14183788 - 10 Sep 2022
Cited by 8 | Viewed by 2812
Abstract
There is a growing demand for bone graft substitutes that mimic the extracellular matrix properties of the native bone tissue to enhance stem cell osteogenesis. Composite hydrogels containing human bone allograft particles are particularly interesting due to inherent bioactivity of the allograft tissue. [...] Read more.
There is a growing demand for bone graft substitutes that mimic the extracellular matrix properties of the native bone tissue to enhance stem cell osteogenesis. Composite hydrogels containing human bone allograft particles are particularly interesting due to inherent bioactivity of the allograft tissue. Here, we report a novel photocurable composite hydrogel bioink for bone tissue engineering. Our composite bioink is formulated by incorporating human allograft bone particles in a methacrylated alginate formulation to enhance adult human mesenchymal stem cell (hMSC) osteogenesis. Detailed rheology and printability studies confirm suitability of our composite bioinks for extrusion-based 3D bioprinting technology. In vitro studies reveal high cell viability (~90%) for hMSCs up to 28 days of culture within 3D bioprinted composite scaffolds. When cultured within bioprinted composite scaffolds, hMSCs show significantly enhanced osteogenic differentiation as compared to neat scaffolds based on alkaline phosphatase activity, calcium deposition, and osteocalcin expression. Full article
(This article belongs to the Special Issue Composite Hydrogels towards Next-Generation Functional Materials and Devices)
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14 pages, 6545 KiB  
Article
An Ultra-Stretchable Polyvinyl Alcohol Hydrogel Based on Tannic Acid Modified Aramid Nanofibers for Use as a Strain Sensor
by Lei Miao, Xiao Wang, Shi Li, Yuanyuan Tu, Jiwen Hu, Zhenzhu Huang, Shudong Lin and Xuefeng Gui
Polymers 2022, 14(17), 3532; https://doi.org/10.3390/polym14173532 - 28 Aug 2022
Cited by 6 | Viewed by 2230
Abstract
The mechanical performance is critical for hydrogels that are used as strain sensors. p-Aramid nanofiber (ANF) is preferable as an additive to the reinforce the mechanical performance of a poly(vinyl alcohol) (PVA). However, due to the limited hydrogen bond sites, the preparation [...] Read more.
The mechanical performance is critical for hydrogels that are used as strain sensors. p-Aramid nanofiber (ANF) is preferable as an additive to the reinforce the mechanical performance of a poly(vinyl alcohol) (PVA). However, due to the limited hydrogen bond sites, the preparation of ultra-stretchable, ANF-based hydrogel strain sensor is still a challenge. Herein, we reported an ultra-stretchable PVA hydrogel sensor based on tea stain-inspired ANFs. Due to the presence of numerous phenol groups in the tannic acid (TA) layer, the interaction between PVA and the ANFs was significantly enhanced even though the mass ratio of TA@ANF in the hydrogel was 2.8 wt‰. The tensile breaking modulus of the PVA/TA@ANF/Ag hydrogel sensor was increased from 86 kPa to 326 kPa, and the tensile breaking elongation was increased from 356% to 602%. Meanwhile, the hydrogel became much softer, and no obvious deterioration of the flexibility was observed after repeated use. Moreover, Ag NPs were formed in situ on the surfaces of the ANFs, which imparted the sensor with electrical conductivity. The hydrogel-based strain sensor could be used to detect the joint movements of a finger, an elbow, a wrist, and a knee, respectively. This ultra-stretchable hydrogel described herein was a promising candidate for detecting large-scale motions. Full article
(This article belongs to the Special Issue Composite Hydrogels towards Next-Generation Functional Materials and Devices)
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Review

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23 pages, 5131 KiB  
Review
Bacterial Nanocellulose Hydrogel: A Promising Alternative Material for the Fabrication of Engineered Vascular Grafts
by Daichen Liu, Qingshan Meng and Jinguang Hu
Polymers 2023, 15(18), 3812; https://doi.org/10.3390/polym15183812 - 18 Sep 2023
Cited by 1 | Viewed by 1302
Abstract
Blood vessels are crucial in the human body, providing essential nutrients to all tissues while facilitating waste removal. As the incidence of cardiovascular disease rises, the demand for efficient treatments increases concurrently. Currently, the predominant interventions for cardiovascular disease are autografts and allografts. [...] Read more.
Blood vessels are crucial in the human body, providing essential nutrients to all tissues while facilitating waste removal. As the incidence of cardiovascular disease rises, the demand for efficient treatments increases concurrently. Currently, the predominant interventions for cardiovascular disease are autografts and allografts. Although effective, they present limitations including high costs and inconsistent success rates. Recently, synthetic vascular grafts, made from artificial materials, have emerged as promising alternatives to traditional methods. Among these materials, bacterial cellulose hydrogel exhibits significant potential for tissue engineering applications, particularly in developing nanoscale platforms that regulate cell behavior and promote tissue regeneration, attributed to its notable physicochemical and biocompatible properties. This study reviews recent progress in fabricating engineered vascular grafts using bacterial nanocellulose, demonstrating the efficacy of bacterial cellulose hydrogel as a biomaterial for synthetic vascular grafts, specifically for stimulating angiogenesis and neovascularization. Full article
(This article belongs to the Special Issue Composite Hydrogels towards Next-Generation Functional Materials and Devices)
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24 pages, 5471 KiB  
Review
Modification Strategies for Ionic Complementary Self-Assembling Peptides: Taking RADA16-I as an Example
by Weiwei Guo, Yinping Ma, Lei Hu, Yujie Feng, Yanmiao Liu, Xuedong Yi, Wenzhi Zhang and Fushan Tang
Polymers 2022, 14(23), 5221; https://doi.org/10.3390/polym14235221 - 30 Nov 2022
Cited by 2 | Viewed by 1303
Abstract
Ion-complementary self-assembling peptides have been studied in many fields for their distinct advantages, mainly due to their self-assembly properties. However, their shortcomings, such as insufficient specific activity and poor mechanical properties, also limited their application. For the better and wider application of these [...] Read more.
Ion-complementary self-assembling peptides have been studied in many fields for their distinct advantages, mainly due to their self-assembly properties. However, their shortcomings, such as insufficient specific activity and poor mechanical properties, also limited their application. For the better and wider application of these promising biomaterials, ion-complementary self-assembling peptides can be modified with their self-assembly properties not being destroyed to the greatest extent. The modification strategies were reviewed by taking RADA16-I as an example. For insufficient specific activity, RADA16-I can be structurally modified with active motifs derived from the active domain of the extracellular matrix or other related active factors. For weak mechanical properties, materials with strong mechanical properties or that can undergo chemical crosslinking were used to mix with RADA16-I to enhance the mechanical properties of RADA16-I. To improve the performance of RADA16-I as drug carriers, appropriate adjustment of the RADA16-I sequence and/or modification of the RADA16-I-related delivery system with polymer materials or specific molecules can be considered to achieve sustained and controlled release of specific drugs or active factors. The modification strategies reviewed in this paper may provide some references for further basic research and clinical application of ion-complementary self-assembling peptides and their derivatives. Full article
(This article belongs to the Special Issue Composite Hydrogels towards Next-Generation Functional Materials and Devices)
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