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Design of Polymeric Hydrogels Biomaterials

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

Deadline for manuscript submissions: closed (31 January 2024) | Viewed by 41911

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Special Issue Editors

Dr. Diana C. Silva

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Centro de Química Estrutural, Institute of Molecular Sciences, Instituto Superior Técnico, Universidade de Lisboa, Av. Rovisco Pais, 1049-001 Lisboa, Portugal
Interests: hydrogels; drug delivery; biomaterial characterization; surface modification; wound dressings
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Dr. Ana Paula Serro

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Centro de Química Estrutural, Institute of Molecular Sciences, Instituto Superior Técnico, University of Lisbon, 1049-001 Lisboa, Portugal
Interests: hydrogels; controlled drug release; biomaterials characterization; biotribology; adsorption of biomolecules onto biomaterials; sterilization
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Dr. Maria Vivero-Lopez

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Guest Editor

Advanced Materials and Healthcare Technologies Division, School of Pharmacy, University of Nottingham, University Park, Nottingham NG7 2RD, UK
Interests: biomaterials characterization; hydrogels; polymeric micelles; drug delivery systems; controlled release; ocular delivery; drug-loaded contact lenses; antibiofilm medical devices
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

The term biomaterial refers to any material (natural or synthetic) designed to be in intimate contact with biological systems that can be used to treat or replace tissues, organs or functions of the body. Polymeric hydrogels are widely used in the modern biomedical field, as they can be manipulated to achieve a controlled structure, dynamic functionality, and biological complexity. They can be produced in different forms, such as films, 3D printable structures, fibers, and nanoparticles. In some cases, they can behave as smart stimuli-responsive materials since their network structure can suffer modifications in response to external environmental triggers and present, for example, self-healing or shape memory properties. Polymeric hydrogels also show the ability to load different compounds within their polymeric network, making it possible to tailor them to provide a sustained release. Although several advances in the design of polymeric hydrogel biomaterials have occurred recently, there are still many challenges to develop new materials that, in addition to being safe, ensure an improved performance.

This Special Issue aims to gather some of the most recent achievements and prospects related to the synthesis, processing, characterization, and applications of new polymeric hydrogel biomaterials. Both original research and comprehensive review papers are welcome.

Dr. Diana C. Silva
Dr. Ana Paula Serro
Dr. Maria Vivero-Lopez
Guest Editors

Manuscript Submission Information

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Keywords

biomaterials
biomedical applications
polymeric hydrogels
hydrogels design
multifunctional hydrogels
smart stimuli-responsive polymeric hydrogels
drug delivery
antimicrobial properties
advanced materials’ characterization

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Published Papers (12 papers)

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Editorial

Jump to: Research, Review

4 pages, 186 KiB

Open AccessEditorial

Editorial for the Special Issue Titled “Design of Polymeric Hydrogels Biomaterials”

by Ana Paula Serro, Maria Vivero-Lopez and Diana C. Silva

Gels 2024, 10(5), 344; https://doi.org/10.3390/gels10050344 - 18 May 2024

Viewed by 999

Abstract

Hydrogels have attracted great interest in the biomedical applications field in recent years [...] Full article

(This article belongs to the Special Issue Design of Polymeric Hydrogels Biomaterials)

Research

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15 pages, 3916 KiB

Open AccessArticle

A Covalently Cross-Linked Hyaluronic Acid/Carboxymethyl Cellulose Composite Hydrogel as a Potential Filler for Soft Tissue Augmentation

by Francesca Della Sala, Mario di Gennaro, Pooyan Makvandi and Assunta Borzacchiello

Gels 2024, 10(1), 67; https://doi.org/10.3390/gels10010067 - 16 Jan 2024

Cited by 3 | Viewed by 3352

Abstract

The use of fillers for soft tissue augmentation is an approach to restore the structure in surgically or traumatically created tissue voids. Hyaluronic acid (HA), is one of the main components of the extracellular matrix, and it is widely employed in the design of materials with features similar to human tissues. HA-based fillers already find extensive use in soft tissue applications, but are burdened with inherent drawbacks, such as poor thermal stability. A well-known strategy to improve the HA properties is to reticulate it with 1,4-Butanediol diglycidyl ether (BDDE). The aim of this work was to improve the design of HA hydrogels as fillers, by developing a crosslinking HA method with carboxymethyl cellulose (CMC) by means of BDDE. CMC is a water soluble cellulose ether, whose insertion into the hydrogel can lead to increased thermal stability. HA/CMC hydrogels at different ratios were prepared, and their rheological properties and thermal stability were investigated. The hydrogel with an HA/CMC ratio of 1/1 resulted in the highest values of viscoelastic moduli before and after thermal treatment. The morphology of the hydrogel was examined via SEM. Biocompatibility response, performed with the Alamar blue assay on fibroblast cells, showed a safety percentage of around 90% until 72 h. Full article

(This article belongs to the Special Issue Design of Polymeric Hydrogels Biomaterials)

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10 pages, 2317 KiB

Open AccessArticle

Regulated Self-Folding in Multi-Layered Hydrogels Considered with an Interfacial Layer

by Jun Woo Lim, Sang Jin Kim, Jimin Jeong, Sung Gyu Shin, Chaewon Woo, Woonggyu Jung and Jae Hyun Jeong

Gels 2024, 10(1), 48; https://doi.org/10.3390/gels10010048 - 10 Jan 2024

Cited by 1 | Viewed by 1359

Abstract

Multi-layered hydrogels consisting of bi- or tri-layers with different swelling ratios are designed to soft hydrogel actuators by self-folding. The successful use of multi-layered hydrogels in this application greatly relies on the precise design and fabrication of the curvature of self-folding. In general, however, the self-folding often results in an undesired mismatch with the expecting value. To address this issue, this study introduces an interfacial layer formed between each layered hydrogel, and this layer is evaluated to enhance the design and fabrication precision. By considering the interfacial layer, which forms through diffusion, as an additional layer in the multi-layered hydrogel, the degree of mismatch in the self-folding is significantly reduced. Experimental results show that as the thickness of the interfacial layer increases, the multi-layered hydrogel exhibits a 3.5-fold increase in its radius of curvature during the self-folding. In addition, the diffusion layer is crucial for creating robust systems by preventing the separation of layers in the muti-layered hydrogel during actuation, thereby ensuring the integrity of the system in operation. This new strategy for designing multi-layered hydrogels including an interfacial layer would greatly serve to fabricate precise and robust soft hydrogel actuators. Full article

(This article belongs to the Special Issue Design of Polymeric Hydrogels Biomaterials)

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18 pages, 6627 KiB

Open AccessArticle

Thermoresponsive Alginate-Graft-pNIPAM/Methyl Cellulose 3D-Printed Scaffolds Promote Osteogenesis In Vitro

by Aikaterini Gialouri, Sofia Falia Saravanou, Konstantinos Loukelis, Maria Chatzinikolaidou, George Pasparakis and Nikolaos Bouropoulos

Gels 2023, 9(12), 984; https://doi.org/10.3390/gels9120984 - 15 Dec 2023

Cited by 3 | Viewed by 2432

Abstract

In this work, a sodium alginate-based copolymer grafted by thermoresponsive poly(N-isopropylacrylamide) (PNIPAM) chains was used as gelator (Alg-g-PNIPAM) in combination with methylcellulose (MC). It was found that the mechanical properties of the resulting gel could be enhanced by the addition of MC and calcium ions (Ca²⁺). The proposed network is formed via a dual crosslinking mechanism including ionic interactions among Ca²⁺ and carboxyl groups and secondary hydrophobic associations of PNIPAM chains. MC was found to further reinforce the dynamic moduli of the resulting gels (i.e., a storage modulus of ca. 1500 Pa at physiological body and post-printing temperature), rendering them suitable for 3D printing in biomedical applications. The polymer networks were stable and retained their printed fidelity with minimum erosion as low as 6% for up to seven days. Furthermore, adhered pre-osteoblastic cells on Alg-g-PNIPAM/MC printed scaffolds presented 80% viability compared to tissue culture polystyrene control, and more importantly, they promoted the osteogenic potential, as indicated by the increased alkaline phosphatase activity, calcium, and collagen production relative to the Alg-g-PNIPAM control scaffolds. Specifically, ALP activity and collagen secreted by cells were significantly enhanced in Alg-g-PNIPAM/MC scaffolds compared to the Alg-g-PNIPAM counterparts, demonstrating their potential in bone tissue engineering. Full article

(This article belongs to the Special Issue Design of Polymeric Hydrogels Biomaterials)

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17 pages, 5511 KiB

Open AccessArticle

Carboxymethyl Chitosan Microgels for Sustained Delivery of Vancomycin and Long-Lasting Antibacterial Effects

by Mehtap Sahiner, Aynur S. Yilmaz, Ramesh S. Ayyala and Nurettin Sahiner

Gels 2023, 9(9), 708; https://doi.org/10.3390/gels9090708 - 1 Sep 2023

Cited by 5 | Viewed by 1718

Abstract

Carboxymethyl chitosan (CMCh) is a unique polysaccharide with functional groups that can develop positive and negative charges due to the abundant numbers of amine and carboxylic acid groups. CMCh is widely used in different areas due to its excellent biocompatibility, biodegradability, water solubility, and chelating ability. CMCh microgels were synthesized in a microemulsion environment using divinyl sulfone (DVS) as a crosslinking agent. CMCh microgel with tailored size and zeta potential values were obtained in a single stem by crosslinking CMCh in a water-in-oil environment. The spherical microgel structure is confirmed by SEM analysis. The sizes of CMCh microgels varied from one micrometer to tens of micrometers. The isoelectric point of CMCh microgels was determined as pH 4.4. Biocompatibility of CMCh microgels was verified on L929 fibroblasts with 96.5 ± 1.5% cell viability at 1 mg/mL concentration. The drug-carrying abilities of CMCh microgels were evaluated by loading Vancomycin (Van) antibiotic as a model drug. Furthermore, the antibacterial activity efficiency of Van-loaded CMCh microgels (Van@CMCh) was investigated. The MIC values of the released drug from Van@CMCh microgels were found to be 68.6 and 7.95 µg/mL against E. coli and S. aureus, respectively, at 24 h contact time. Disk diffusion tests confirmed that Van@CMCh microgels, especially for Gram-positive (S. aureus) bacteria, revealed long-lasting inhibitory effects on bacteria growth up to 72 h. Full article

(This article belongs to the Special Issue Design of Polymeric Hydrogels Biomaterials)

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14 pages, 5610 KiB

Open AccessArticle

Acceleration of Wound Healing in Rats by Modified Lignocellulose Based Sponge Containing Pentoxifylline Loaded Lecithin/Chitosan Nanoparticles

by Pouya Dehghani, Aliakbar Akbari, Milad Saadatkish, Jaleh Varshosaz, Monireh Kouhi and Mahdi Bodaghi

Gels 2022, 8(10), 658; https://doi.org/10.3390/gels8100658 - 15 Oct 2022

Cited by 3 | Viewed by 2355

Abstract

Dressing wounds accelerates the re-epithelialization process and changes the inflammatory environment towards healing. In the current study, a lignocellulose sponge containing pentoxifylline (PTX)-loaded lecithin/chitosan nanoparticles (LCNs) was developed to enhance the wound healing rate. Lecithin/chitosan nanoparticles were obtained by the solvent-injection method and characterized in terms of morphology, particle size distribution, and zeta potential. The lignocellulose hydrogels were functionalized through oxidation/amination and freeze-dried to obtain sponges. The prepared sponge was then loaded with LCNs/PTX to control drug release. The nanoparticle containing sponges were characterized using FTIR and SEM analysis. The drug release study from both nanoparticles and sponges was performed in PBS at 37 °C at different time points. The results demonstrated that PTX has sustained release from lignocellulose hydrogels. The wound healing was examined using a standard rat model. The results exhibited that PTX loaded hydrogels could achieve significantly accelerated and enhanced healing compared to the drug free hydrogels and the normal saline treatment. Histological examination of the healed skin confirmed the visual observations. Overall speaking, the in vivo assessment of the developed sponge asserts its suitability as wound dressing for treatment of chronic skin wounds. Full article

(This article belongs to the Special Issue Design of Polymeric Hydrogels Biomaterials)

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10 pages, 3222 KiB

Open AccessCommunication

Hydrotropic Hydrogels Prepared from Polyglycerol Dendrimers: Enhanced Solubilization and Release of Paclitaxel

by Tooru Ooya and Jaehwi Lee

Gels 2022, 8(10), 614; https://doi.org/10.3390/gels8100614 - 26 Sep 2022

Cited by 3 | Viewed by 2073

Abstract

Polyglycerol dendrimers (PGD) exhibit unique properties such as drug delivery, drug solubilization, bioimaging, and diagnostics. In this study, PGD hydrogels were prepared and evaluated as devices for controlled drug release with good solubilization properties. The PGD hydrogels were prepared by crosslinking using ethylene glycol diglycidylether (EGDGE). The concentrations of EGDGE and PGDs were varied. The hydrogels were swellable in ethanol for loading paclitaxel (PTX). The amount of PTX in the hydrogels increased with the swelling ratio, which is proportional to EGDGE/OH ratio, meaning that heterogeneous crosslinking of PGD made high dense region of PGD molecules in the matrix. The hydrogels remained transparent after loading PTX and standing in water for one day, indicating that PTX was dispersed in the hydrogels without any crystallization in water. The results of FTIR imaging of the PTX-loaded PGD hydrogels revealed good dispersion of PTX in the hydrogel matrix. Sixty percent of the loaded PTX was released in a sink condition within 90 min, suggesting that the solubilized PTX would be useful for controlled release without any precipitation. Polyglycerol dendrimer hydrogels are expected to be applicable for rapid release of poorly water-soluble drugs, e.g., for oral administration. Full article

(This article belongs to the Special Issue Design of Polymeric Hydrogels Biomaterials)

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Review

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54 pages, 15641 KiB

Open AccessReview

Novel Therapeutic Hybrid Systems Using Hydrogels and Nanotechnology: A Focus on Nanoemulgels for the Treatment of Skin Diseases

by Kamil Sghier, Maja Mur, Francisco Veiga, Ana Cláudia Paiva-Santos and Patrícia C. Pires

Gels 2024, 10(1), 45; https://doi.org/10.3390/gels10010045 - 6 Jan 2024

Cited by 6 | Viewed by 3624

Abstract

Topical and transdermal drug delivery are advantageous administration routes, especially when treating diseases and conditions with a skin etiology. Nevertheless, conventional dosage forms often lead to low therapeutic efficacy, safety issues, and patient noncompliance. To tackle these issues, novel topical and transdermal platforms involving nanotechnology have been developed. This review focuses on the latest advances regarding the development of nanoemulgels for skin application, encapsulating a wide variety of molecules, including already marketed drugs (miconazole, ketoconazole, fusidic acid, imiquimod, meloxicam), repurposed marketed drugs (atorvastatin, omeprazole, leflunomide), natural-derived compounds (eucalyptol, naringenin, thymoquinone, curcumin, chrysin, brucine, capsaicin), and other synthetic molecules (ebselen, tocotrienols, retinyl palmitate), for wound healing, skin and skin appendage infections, skin inflammatory diseases, skin cancer, neuropathy, or anti-aging purposes. Developed formulations revealed adequate droplet size, PDI, viscosity, spreadability, pH, stability, drug release, and drug permeation and/or retention capacity, having more advantageous characteristics than current marketed formulations. In vitro and/or in vivo studies established the safety and efficacy of the developed formulations, confirming their therapeutic potential, and making them promising platforms for the replacement of current therapies, or as possible adjuvant treatments, which might someday effectively reach the market to help fight highly incident skin or systemic diseases and conditions. Full article

(This article belongs to the Special Issue Design of Polymeric Hydrogels Biomaterials)

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22 pages, 3289 KiB

Open AccessEditor’s ChoiceReview

Exploring the Potential of Artificial Intelligence for Hydrogel Development—A Short Review

by Irina Negut and Bogdan Bita

Gels 2023, 9(11), 845; https://doi.org/10.3390/gels9110845 - 25 Oct 2023

Cited by 7 | Viewed by 3898

Abstract

AI and ML have emerged as transformative tools in various scientific domains, including hydrogel design. This work explores the integration of AI and ML techniques in the realm of hydrogel development, highlighting their significance in enhancing the design, characterisation, and optimisation of hydrogels for diverse applications. We introduced the concept of AI train hydrogel design, underscoring its potential to decode intricate relationships between hydrogel compositions, structures, and properties from complex data sets. In this work, we outlined classical physical and chemical techniques in hydrogel design, setting the stage for AI/ML advancements. These methods provide a foundational understanding for the subsequent AI-driven innovations. Numerical and analytical methods empowered by AI/ML were also included. These computational tools enable predictive simulations of hydrogel behaviour under varying conditions, aiding in property customisation. We also emphasised AI’s impact, elucidating its role in rapid material discovery, precise property predictions, and optimal design. ML techniques like neural networks and support vector machines that expedite pattern recognition and predictive modelling using vast datasets, advancing hydrogel formulation discovery are also presented. AI and ML’s have a transformative influence on hydrogel design. AI and ML have revolutionised hydrogel design by expediting material discovery, optimising properties, reducing costs, and enabling precise customisation. These technologies have the potential to address pressing healthcare and biomedical challenges, offering innovative solutions for drug delivery, tissue engineering, wound healing, and more. By harmonising computational insights with classical techniques, researchers can unlock unprecedented hydrogel potentials, tailoring solutions for diverse applications. Full article

(This article belongs to the Special Issue Design of Polymeric Hydrogels Biomaterials)

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35 pages, 5296 KiB

Open AccessReview

Dissolving and Swelling Hydrogel-Based Microneedles: An Overview of Their Materials, Fabrication, Characterization Methods, and Challenges

by Bana Shriky, Maksims Babenko and Ben R. Whiteside

Gels 2023, 9(10), 806; https://doi.org/10.3390/gels9100806 - 7 Oct 2023

Cited by 7 | Viewed by 4704

Abstract

Polymeric hydrogels are a complex class of materials with one common feature—the ability to form three-dimensional networks capable of imbibing large amounts of water or biological fluids without being dissolved, acting as self-sustained containers for various purposes, including pharmaceutical and biomedical applications. Transdermal pharmaceutical microneedles are a pain-free drug delivery system that continues on the path to widespread adoption—regulatory guidelines are on the horizon, and investments in the field continue to grow annually. Recently, hydrogels have generated interest in the field of transdermal microneedles due to their tunable properties, allowing them to be exploited as delivery systems and extraction tools. As hydrogel microneedles are a new emerging technology, their fabrication faces various challenges that must be resolved for them to redeem themselves as a viable pharmaceutical option. This article discusses hydrogel microneedles from a material perspective, regardless of their mechanism of action. It cites the recent advances in their formulation, presents relevant fabrication and characterization methods, and discusses manufacturing and regulatory challenges facing these emerging technologies before their approval. Full article

(This article belongs to the Special Issue Design of Polymeric Hydrogels Biomaterials)

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37 pages, 3146 KiB

Open AccessReview

Advancements and Applications of Injectable Hydrogel Composites in Biomedical Research and Therapy

by Hossein Omidian and Sumana Dey Chowdhury

Gels 2023, 9(7), 533; https://doi.org/10.3390/gels9070533 - 30 Jun 2023

Cited by 28 | Viewed by 6430

Abstract

Injectable hydrogels have gained popularity for their controlled release, targeted delivery, and enhanced mechanical properties. They hold promise in cardiac regeneration, joint diseases, postoperative analgesia, and ocular disorder treatment. Hydrogels enriched with nano-hydroxyapatite show potential in bone regeneration, addressing challenges of bone defects, osteoporosis, and tumor-associated regeneration. In wound management and cancer therapy, they enable controlled release, accelerated wound closure, and targeted drug delivery. Injectable hydrogels also find applications in ischemic brain injury, tissue regeneration, cardiovascular diseases, and personalized cancer immunotherapy. This manuscript highlights the versatility and potential of injectable hydrogel nanocomposites in biomedical research. Moreover, it includes a perspective section that explores future prospects, emphasizes interdisciplinary collaboration, and underscores the promising future potential of injectable hydrogel nanocomposites in biomedical research and applications. Full article

(This article belongs to the Special Issue Design of Polymeric Hydrogels Biomaterials)

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25 pages, 5312 KiB

Open AccessReview

Mucoadhesive Polymers and Their Applications in Drug Delivery Systems for the Treatment of Bladder Cancer

by Caroline S. A. de Lima, Justine P. R. O. Varca, Victória M. Alves, Kamila M. Nogueira, Cassia P. C. Cruz, M. Isabel Rial-Hermida, Sławomir S. Kadłubowski, Gustavo H. C. Varca and Ademar B. Lugão

Gels 2022, 8(9), 587; https://doi.org/10.3390/gels8090587 - 15 Sep 2022

Cited by 25 | Viewed by 7448

Abstract

Bladder cancer (BC) is the tenth most common type of cancer worldwide, affecting up to four times more men than women. Depending on the stage of the tumor, different therapy protocols are applied. Non-muscle-invasive cancer englobes around 70% of the cases and is usually treated using the transurethral resection of bladder tumor (TURBIT) followed by the instillation of chemotherapy or immunotherapy. However, due to bladder anatomy and physiology, current intravesical therapies present limitations concerning permeation and time of residence. Furthermore, they require several frequent catheter insertions with a reduced interval between doses, which is highly demotivating for the patient. This scenario has encouraged several pieces of research focusing on the development of drug delivery systems (DDS) to improve drug time residence, permeation capacity, and target release. In this review, the current situation of BC is described concerning the disease and available treatments, followed by a report on the main DDS developed in the past few years, focusing on those based on mucoadhesive polymers as a strategy. A brief review of methods to evaluate mucoadhesion properties is also presented; lastly, different polymers suitable for this application are discussed. Full article

(This article belongs to the Special Issue Design of Polymeric Hydrogels Biomaterials)

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