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Special Issue "Smart Hydrogels for (Bio)printing Applications"

A special issue of Materials (ISSN 1996-1944). This special issue belongs to the section "Biomaterials".

Deadline for manuscript submissions: closed (31 July 2016)

Special Issue Editors

Guest Editor
Prof. Dr. Peter Dubruel

Polymer Chemistry & Biomaterials Research Group, Ghent University, Krijgslaan 281 S4 Bis, Ghent 9000, Belgium
Website | E-Mail
Interests: hydrogels, polyesters, 3D printing, surface modification, biomedical applications of polymers
Co-Guest Editor
Prof. Dr. Sandra Van Vlierberghe

1. Brussels Photonics Team (B-PHOT), Vrije Universiteit Brussel, Pleinlaan 2, B-1050 Brussel, Belgium 2. Polymer Chemistry & Biomaterials Research Group, Ghent University, Krijgslaan 281 S4 Bis, Ghent 9000, Belgium
Website1 | Website2 | E-Mail

Special Issue Information

Dear Colleagues,

Hydrogels represent a paramount biomaterial class. As they retain large amounts of water, they are potential key candidates as extra-cellular matrix mimics, with the final aim to enhance the quality of human life.

Hydrogels have been investigated for a long time and encompass synthetic polymers, biopolymers or combinations of both as building blocks. In recent years, hydrogels have successfully been taken to the next level, as various 3D (bio)printing technologies have emerged with or without embedded cells.

In the current Special Issue of Materials, we offer a platform for the above-described ground breaking science. We hope that the issue will bring new insights to the scientific community in an ever-expanding research field.

Peter Dubruel
Sandra Van Vlierberghe
Guest Editors

Manuscript Submission Information

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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. Materials 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 1500 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

  • hydrogel;
  • biopolymer;
  • (bio)printing;
  • cell encapsulation;
  • soft tissue regeneration.

Published Papers (6 papers)

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Research

Open AccessArticle Fabrication of Cell-Loaded Two-Phase 3D Constructs for Tissue Engineering
Materials 2016, 9(11), 887; doi:10.3390/ma9110887
Received: 22 August 2016 / Revised: 14 October 2016 / Accepted: 17 October 2016 / Published: 1 November 2016
Cited by 1 | PDF Full-text (5457 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
Hydrogel optimisation for biofabrication considering shape stability/mechanical properties and cell response is challenging. One approach to tackle this issue is to combine different additive manufacturing techniques, e.g., hot-melt extruded thermoplastics together with bioplotted cell loaded hydrogels in a sequential plotting process. This method
[...] Read more.
Hydrogel optimisation for biofabrication considering shape stability/mechanical properties and cell response is challenging. One approach to tackle this issue is to combine different additive manufacturing techniques, e.g., hot-melt extruded thermoplastics together with bioplotted cell loaded hydrogels in a sequential plotting process. This method enables the fabrication of 3D constructs mechanically supported by the thermoplastic structure and biologically functionalised by the hydrogel phase. In this study, polycaprolactone (PCL) and polyethylene glycol (PEG) blend (PCL-PEG) together with alginate dialdehyde gelatine hydrogel (ADA-GEL) loaded with stromal cell line (ST2) were investigated. PCL-PEG blends were evaluated concerning plotting properties to fabricate 3D scaffolds, namely miscibility, wetting behaviour and in terms of cell response. Scaffolds were characterised considering pore size, porosity, strut width, degradation behaviour and mechanical stability. Blends showed improved hydrophilicity and cell response with PEG blending increasing the degradation and decreasing the mechanical properties of the scaffolds. Hybrid constructs with PCL-PEG blend and ADA-GEL were fabricated. Cell viability, distribution, morphology and interaction of cells with the support structure were analysed. Increased degradation of the thermoplastic support structure and proliferation of the cells not only in the hydrogel, but also on the thermoplastic phase, indicates the potential of this novel material combination for biofabricating 3D tissue engineering scaffolds. Full article
(This article belongs to the Special Issue Smart Hydrogels for (Bio)printing Applications)
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Open AccessCommunication An Intriguing Method for Fabricating Arbitrarily Shaped “Matreshka” Hydrogels Using a Self-Healing Template
Materials 2016, 9(11), 864; doi:10.3390/ma9110864
Received: 30 September 2016 / Revised: 14 October 2016 / Accepted: 18 October 2016 / Published: 25 October 2016
PDF Full-text (3665 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
This work describes an intriguing strategy for the creation of arbitrarily shaped hydrogels utilizing a self-healing template (SHT). A SHT was loaded with a photo-crosslinkable monomer, PEG diacrylate (PEGDA), and then ultraviolet light (UV) crosslinked after first shaping. The SHT template was removed
[...] Read more.
This work describes an intriguing strategy for the creation of arbitrarily shaped hydrogels utilizing a self-healing template (SHT). A SHT was loaded with a photo-crosslinkable monomer, PEG diacrylate (PEGDA), and then ultraviolet light (UV) crosslinked after first shaping. The SHT template was removed by simple washing with water, leaving behind the hydrogel in the desired physical shape. A hierarchical 3D structure such as “Matreshka” boxes were successfully prepared by simply repeating the “self-healing” and “photo-irradiation” processes. We have also explored the potential of the SHT system for the manipulation of cells. Full article
(This article belongs to the Special Issue Smart Hydrogels for (Bio)printing Applications)
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Figure 1

Open AccessArticle Charged Triazole Cross-Linkers for Hyaluronan-Based Hybrid Hydrogels
Materials 2016, 9(10), 810; doi:10.3390/ma9100810
Received: 28 July 2016 / Revised: 13 September 2016 / Accepted: 23 September 2016 / Published: 30 September 2016
Cited by 2 | PDF Full-text (1164 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
Polyelectrolyte hydrogels play an important role in tissue engineering and can be produced from natural polymers, such as the glycosaminoglycan hyaluronan. In order to control charge density and mechanical properties of hyaluronan-based hydrogels, we developed cross-linkers with a neutral or positively charged triazole
[...] Read more.
Polyelectrolyte hydrogels play an important role in tissue engineering and can be produced from natural polymers, such as the glycosaminoglycan hyaluronan. In order to control charge density and mechanical properties of hyaluronan-based hydrogels, we developed cross-linkers with a neutral or positively charged triazole core with different lengths of spacer arms and two terminal maleimide groups. These cross-linkers react with thiolated hyaluronan in a fast, stoichiometric thio-Michael addition. Introducing a positive charge on the core of the cross-linker enabled us to compare hydrogels with the same interconnectivity, but a different charge density. Positively charged cross-linkers form stiffer hydrogels relatively independent of the size of the cross-linker, whereas neutral cross-linkers only form stable hydrogels at small spacer lengths. These novel cross-linkers provide a platform to tune the hydrogel network charge and thus the mechanical properties of the network. In addition, they might offer a wide range of applications especially in bioprinting for precise design of hydrogels. Full article
(This article belongs to the Special Issue Smart Hydrogels for (Bio)printing Applications)
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Figure 1

Open AccessCommunication Electrochemical Hydrogel Lithography of Calcium-Alginate Hydrogels for Cell Culture
Materials 2016, 9(9), 744; doi:10.3390/ma9090744
Received: 31 July 2016 / Revised: 12 August 2016 / Accepted: 22 August 2016 / Published: 31 August 2016
Cited by 2 | PDF Full-text (2952 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
Here we propose a novel electrochemical lithography methodology for fabricating calcium-alginate hydrogels having controlled shapes. We separated the chambers for Ca2+ production and gel formation with alginate with a semipermeable membrane. Ca2+ formed in the production chamber permeated through the membrane
[...] Read more.
Here we propose a novel electrochemical lithography methodology for fabricating calcium-alginate hydrogels having controlled shapes. We separated the chambers for Ca2+ production and gel formation with alginate with a semipermeable membrane. Ca2+ formed in the production chamber permeated through the membrane to fabricate a gel structure on the membrane in the gel formation chamber. When the calcium-alginate hydrogels were modified with collagen, HepG2 cells proliferated on the hydrogels. These results show that electrochemical hydrogel lithography is useful for cell culture. Full article
(This article belongs to the Special Issue Smart Hydrogels for (Bio)printing Applications)
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Figure 1

Open AccessArticle Dedifferentiated Human Articular Chondrocytes Redifferentiate to a Cartilage-Like Tissue Phenotype in a Poly(ε-Caprolactone)/Self-Assembling Peptide Composite Scaffold
Materials 2016, 9(6), 472; doi:10.3390/ma9060472
Received: 27 April 2016 / Revised: 29 May 2016 / Accepted: 3 June 2016 / Published: 17 June 2016
Cited by 2 | PDF Full-text (4651 KB) | HTML Full-text | XML Full-text
Abstract
Adult articular cartilage has a limited capacity for growth and regeneration and, with injury, new cellular or biomaterial-based therapeutic platforms are required to promote repair. Tissue engineering aims to produce cartilage-like tissues that recreate the complex mechanical and biological properties found in vivo
[...] Read more.
Adult articular cartilage has a limited capacity for growth and regeneration and, with injury, new cellular or biomaterial-based therapeutic platforms are required to promote repair. Tissue engineering aims to produce cartilage-like tissues that recreate the complex mechanical and biological properties found in vivo. In this study, a unique composite scaffold was developed by infiltrating a three-dimensional (3D) woven microfiber poly (ε-caprolactone) (PCL) scaffold with the RAD16-I self-assembling nanofibers to obtain multi-scale functional and biomimetic tissue-engineered constructs. The scaffold was seeded with expanded dedifferentiated human articular chondrocytes and cultured for four weeks in control and chondrogenic growth conditions. The composite constructs were compared to control constructs obtained by culturing cells with 3D woven PCL scaffolds or RAD16-I independently. High viability and homogeneous cell distribution were observed in all three scaffolds used during the term of the culture. Moreover, gene and protein expression profiles revealed that chondrogenic markers were favored in the presence of RAD16-I peptide (PCL/RAD composite or alone) under chondrogenic induction conditions. Further, constructs displayed positive staining for toluidine blue, indicating the presence of synthesized proteoglycans. Finally, mechanical testing showed that constructs containing the PCL scaffold maintained the initial shape and viscoelastic behavior throughout the culture period, while constructs with RAD16-I scaffold alone contracted during culture time into a stiffer and compacted structure. Altogether, these results suggest that this new composite scaffold provides important mechanical requirements for a cartilage replacement, while providing a biomimetic microenvironment to re-establish the chondrogenic phenotype of human expanded articular chondrocytes. Full article
(This article belongs to the Special Issue Smart Hydrogels for (Bio)printing Applications)
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Open AccessArticle A Hydrogel Model Incorporating 3D-Plotted Hydroxyapatite for Osteochondral Tissue Engineering
Materials 2016, 9(4), 285; doi:10.3390/ma9040285
Received: 26 January 2016 / Revised: 24 March 2016 / Accepted: 6 April 2016 / Published: 14 April 2016
Cited by 3 | PDF Full-text (4011 KB) | HTML Full-text | XML Full-text
Abstract
The concept of biphasic or multi-layered compound scaffolds has been explored within numerous studies in the context of cartilage and osteochondral regeneration. To date, no system has been identified that stands out in terms of superior chondrogenesis, osteogenesis or the formation of a
[...] Read more.
The concept of biphasic or multi-layered compound scaffolds has been explored within numerous studies in the context of cartilage and osteochondral regeneration. To date, no system has been identified that stands out in terms of superior chondrogenesis, osteogenesis or the formation of a zone of calcified cartilage (ZCC). Herein we present a 3D plotted scaffold, comprising an alginate and hydroxyapatite paste, cast within a photocrosslinkable hydrogel made of gelatin methacrylamide (GelMA), or GelMA with hyaluronic acid methacrylate (HAMA). We hypothesized that this combination of 3D plotting and hydrogel crosslinking would form a high fidelity, cell supporting structure that would allow localization of hydroxyapatite to the deepest regions of the structure whilst taking advantage of hydrogel photocrosslinking. We assessed this preliminary design in terms of chondrogenesis in culture with human articular chondrocytes, and verified whether the inclusion of hydroxyapatite in the form presented had any influence on the formation of the ZCC. Whilst the inclusion of HAMA resulted in a better chondrogenic outcome, the effect of HAP was limited. We overall demonstrated that formation of such compound structures is possible, providing a foundation for future work. The development of cohesive biphasic systems is highly relevant for current and future cartilage tissue engineering. Full article
(This article belongs to the Special Issue Smart Hydrogels for (Bio)printing Applications)
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