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Smart Hydrogels for (Bio)printing Applications
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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) | Viewed by 44166

Special Issue Editors

Prof. Dr. Peter Dubruel

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

E-Mail Website1 Website2
Co-Guest Editor
Polymer Chemistry & Biomaterials Research Group, Centre of Macromolecular Chemistry, Ghent University, Krijgslaan 281, S4 Bis, 9000 Ghent, Belgium
Interests: hydrogels; 3D printing; electrospinning; two-photon polymerization; proteins; polysaccharides; tissue engineering; hydrogel functionalization
Special Issues, Collections and Topics in MDPI journals

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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Keywords

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

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Published Papers (6 papers)

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Research

5457 KiB  
Article
Fabrication of Cell-Loaded Two-Phase 3D Constructs for Tissue Engineering
by Tobias Zehnder, Tim Freund, Merve Demir, Rainer Detsch and Aldo R. Boccaccini
Materials 2016, 9(11), 887; https://doi.org/10.3390/ma9110887 - 1 Nov 2016
Cited by 31 | Viewed by 8645
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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3665 KiB  
Communication
An Intriguing Method for Fabricating Arbitrarily Shaped “Matreshka” Hydrogels Using a Self-Healing Template
by Takeshi Sato, Koichiro Uto, Takao Aoyagi and Mitsuhiro Ebara
Materials 2016, 9(11), 864; https://doi.org/10.3390/ma9110864 - 25 Oct 2016
Viewed by 5818
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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1164 KiB  
Article
Charged Triazole Cross-Linkers for Hyaluronan-Based Hybrid Hydrogels
by Maike Martini, Patricia S. Hegger, Nicole Schädel, Burcu B. Minsky, Manuel Kirchhof, Sebastian Scholl, Alexander Southan, Günter E. M. Tovar, Heike Boehm and Sabine Laschat
Materials 2016, 9(10), 810; https://doi.org/10.3390/ma9100810 - 30 Sep 2016
Cited by 15 | Viewed by 5576
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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2952 KiB  
Communication
Electrochemical Hydrogel Lithography of Calcium-Alginate Hydrogels for Cell Culture
by Fumisato Ozawa, Kosuke Ino, Hitoshi Shiku and Tomokazu Matsue
Materials 2016, 9(9), 744; https://doi.org/10.3390/ma9090744 - 31 Aug 2016
Cited by 32 | Viewed by 8211
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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4651 KiB  
Article
Dedifferentiated Human Articular Chondrocytes Redifferentiate to a Cartilage-Like Tissue Phenotype in a Poly(ε-Caprolactone)/Self-Assembling Peptide Composite Scaffold
by Lourdes Recha-Sancho, Franklin T. Moutos, Jordi Abellà, Farshid Guilak and Carlos E. Semino
Materials 2016, 9(6), 472; https://doi.org/10.3390/ma9060472 - 17 Jun 2016
Cited by 29 | Viewed by 6928
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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4011 KiB  
Article
A Hydrogel Model Incorporating 3D-Plotted Hydroxyapatite for Osteochondral Tissue Engineering
by Michal Bartnikowski, Ashwini Rahul Akkineni, Michael Gelinsky, Maria A. Woodruff and Travis J. Klein
Materials 2016, 9(4), 285; https://doi.org/10.3390/ma9040285 - 14 Apr 2016
Cited by 31 | Viewed by 8385
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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