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Polymers
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Polymeric Materials in 3D and 4D Printing
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Polymeric Materials in 3D and 4D Printing

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

Deadline for manuscript submissions: closed (30 November 2020) | Viewed by 36609

Special Issue Editor

Prof. Dr. Yi-Wen Chen

E-Mail Website
Guest Editor
Graduate Institute of Biomedical Sciences, China Medical University, Taichung City 40402, Taiwan
Interests: 3D printing technologies; biomedical materials and nanomaterials; additive manufacturing in medicine; bioprinting and regeneration medicine

Special Issue Information

Dear Colleagues,

Engineering by multilayered methodologies, such as 3D or 4D printing, is redefining the manufacturing process at multiscale levels with extraordinary design freedom in the era of digital fabrication technology. The stepwise layer-by-layer process which is typical in 3D printing to a continuous process may significantly accelerate the practical potential of printing technology. Being based on traditional 3D printing, it and 4D printing can encompass a wide range of disciplines, such as materials science, bioengineering, and chemistry/chemical engineering, and have the true potential to emerge as the next-generation manufacturing technique. The art of 3D or 4D Printing technologies has regenerated tremendous attention but also created massive challenges at the same time. Among these, the most serious issue in the progress of 3D or 4D Printing applications is material science advancement. With our broad understanding of polymeric material science, we can build the precise perception of multidimensional processes for unconventional materials (e.g., smart stimuli-responsive materials) that pose limitations on closing the gap between manufacturing processes and developing novel applications.

The innovation of polymeric materials, the material properties discussion, the correlation between material and fabrication process, the novel applications of 3D or 4D printing with polymeric materials, and the state-of-the-art and limitations that exist in the current material modalities will be explored in this proposed Special Issue of Polymers.

Prof. Dr. Yi-Wen Chen
Guest Editor

Keywords

  • 3D and 4D printing
  • Shape memory
  • Smart materials
  • Biomimetic
  • Stimuli-responsive polymers
  • Soft robotics
  • Biofabrication

Published Papers (7 papers)

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Research

26 pages, 9596 KiB  
Article
Biomimetic Mineralization on 3D Printed PLA Scaffolds: On the Response of Human Primary Osteoblasts Spheroids and In Vivo Implantation
by Marianna O. C. Maia-Pinto, Ana Carolina B. Brochado, Bruna Nunes Teixeira, Suelen C. Sartoretto, Marcelo J. Uzeda, Adriana T. N. N. Alves, Gutemberg G. Alves, Mônica D. Calasans-Maia and Rossana M. S. M. Thiré
Polymers 2021, 13(1), 74; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13010074 - 27 Dec 2020
Cited by 30 | Viewed by 4883
Abstract
This study aimed to assess the response of 3D printed polylactic acid (PLA) scaffolds biomimetically coated with apatite on human primary osteoblast (HOb) spheroids and evaluate the biological response to its association with Bone Morphogenetic Protein 2 (rhBMP-2) in rat calvaria. PLA scaffolds [...] Read more.
This study aimed to assess the response of 3D printed polylactic acid (PLA) scaffolds biomimetically coated with apatite on human primary osteoblast (HOb) spheroids and evaluate the biological response to its association with Bone Morphogenetic Protein 2 (rhBMP-2) in rat calvaria. PLA scaffolds were produced via 3D printing, soaked in simulated body fluid (SBF) solution to promote apatite deposition, and characterized by physical-chemical, morphological, and mechanical properties. PLA-CaP scaffolds with interconnected porous and mechanical properties suitable for bone repairing were produced with reproducibility. The in vitro biological response was assessed with human primary osteoblast spheroids. Increased cell adhesion and the rise of in vitro release of growth factors (Platelet-Derived Growth Factor (PDGF), Basic Fibroblast Growth Factor (bFGF), Vascular Endothelial Growth Factor (VEGF) was observed for PLA-CaP scaffolds, when pre-treated with fetal bovine serum (FBS). This pre-treatment with FBS was done in a way to enhance the adsorption of serum proteins, increasing the number of bioactive sites on the surface of scaffolds, and to partially mimic in vivo interactions. The in vivo analysis was conducted through the implantation of 3D printed PLA scaffolds either alone, coated with apatite (PLA-CaP) or PLA-CaP loaded with rhBMP-2 on critical-sized defects (8 mm) of rat calvaria. PLA-CaP+rhBMP2 presented higher values of newly formed bone (NFB) than other groups at all in vivo experimental periods (p < 0.05), attaining 44.85% of NFB after six months. These findings indicated two new potential candidates as alternatives to autogenous bone grafts for long-term treatment: (i) 3D-printed PLA-CaP scaffold associated with spheroids, since it can reduce the time of repair in situ by expression of biomolecules and growth factors; and (ii) 3D-printed PLA-CaP functionalized rhBMP2 scaffold, a biocompatible, bioactive biomaterial, with osteoconductivity and osteoinductivity. Full article
(This article belongs to the Special Issue Polymeric Materials in 3D and 4D Printing)
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12 pages, 4797 KiB  
Article
Quantitative Investigation of the Process Parameters of Electrohydrodynamic Direct-Writing and Their Effects on Fiber Surface Roughness and Cell Adhesion
by Chen Jiang, Kan Wang, Xuzhou Jiang, Chuck Zhang and Ben Wang
Polymers 2020, 12(11), 2475; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12112475 - 25 Oct 2020
Cited by 15 | Viewed by 2441
Abstract
Electrohydrodynamic (EHD) direct-writing has been widely used to fabricate micro/nanofibers that can serve as a building block in tissue engineering scaffolds. However, the application of EHD direct-writing in tissue engineering is limited by the lack of fundamental knowledge in the correlations among the [...] Read more.
Electrohydrodynamic (EHD) direct-writing has been widely used to fabricate micro/nanofibers that can serve as a building block in tissue engineering scaffolds. However, the application of EHD direct-writing in tissue engineering is limited by the lack of fundamental knowledge in the correlations among the process parameters, the fiber surface roughness, and the cell adhesion performance. Without a standardized experimental setting and the quantitative database, inconsistent results have been reported. Here, we quantitatively investigate the process–structure–property relationships as the first step towards a better understanding of the EHD direct-writing technology for tissue engineering. Polycaprolactone (PCL) solution is used as a model ink material, and human mesenchymal stem cells (hMSCs) are used to study cell adhesion on PCL fibers. We investigate the different jetting modes defined by the applied voltage, the feed rate, and the nozzle–collector distance. The quantitative effects of process parameters on the fiber surface roughness and the cell adhesion performance are experimentally determined. The quantitative process–structure–property relationships revealed in this study provide guidelines for controlling the surface roughness and the cell adhesion performance of EHD direct-written fibers. This study will facilitate the application of EHD direct-writing in tissue engineering. Full article
(This article belongs to the Special Issue Polymeric Materials in 3D and 4D Printing)
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18 pages, 6707 KiB  
Article
Effects of Gelatin Methacrylate Bio-ink Concentration on Mechano-Physical Properties and Human Dermal Fibroblast Behavior
by Ming-You Shie, Jian-Jr Lee, Chia-Che Ho, Ssu-Yin Yen, Hooi Yee Ng and Yi-Wen Chen
Polymers 2020, 12(9), 1930; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12091930 - 26 Aug 2020
Cited by 70 | Viewed by 9297
Abstract
Gelatin-methacryloyl (GelMa) is a very versatile biomaterial widely used in various biomedical applications. The addition of methacryloyl makes it possible to have hydrogels with varying mechanical properties due to its photocuring characteristics. In addition, gelatin is obtained and derived from natural material; thus, [...] Read more.
Gelatin-methacryloyl (GelMa) is a very versatile biomaterial widely used in various biomedical applications. The addition of methacryloyl makes it possible to have hydrogels with varying mechanical properties due to its photocuring characteristics. In addition, gelatin is obtained and derived from natural material; thus, it retains various cell-friendly motifs, such as arginine-glycine-aspartic acid, which then provides implanted cells with a friendly environment for proliferation and differentiation. In this study, we fabricated human dermal fibroblast cell (hDF)-laden photocurable GelMa hydrogels with varying physical properties (5%, 10%, and 15%) and assessed them for cellular responses and behavior, including cell spreading, proliferation, and the degree of extracellular matrix remodeling. Under similar photocuring conditions, lower concentrations of GelMa hydrogels had lower mechanical properties than higher concentrations. Furthermore, other properties, such as swelling and degradation, were compared in this study. In addition, our findings revealed that there were increased remodeling and proliferation markers in the 5% GelMa group, which had lower mechanical properties. However, it was important to note that cellular viabilities were not affected by the stiffness of the hydrogels. With this result in mind, we attempted to fabricate 5–15% GelMa scaffolds (20 × 20 × 3 mm3) to assess their feasibility for use in skin regeneration applications. The results showed that both 10% and 15% GelMa scaffolds could be fabricated easily at room temperature by adjusting several parameters, such as printing speed and extrusion pressure. However, since the sol-gel temperature of 5% GelMa was noted to be lower than its counterparts, 5% GelMa scaffolds had to be printed at low temperatures. In conclusion, GelMa once again was shown to be an ideal biomaterial for various tissue engineering applications due to its versatile mechanical and biological properties. This study showed the feasibility of GelMa in skin tissue engineering and its potential as an alternative for skin transplants. Full article
(This article belongs to the Special Issue Polymeric Materials in 3D and 4D Printing)
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18 pages, 2066 KiB  
Article
Synthesis and Characterisation of Acrylic Resin-Al Powder Composites Suitable for Additive Manufacturing
by J. J. Relinque, Ismael Romero-Ocaña, Francisco J. Navas-Martos, F. J. Delgado, M. Domínguez and S. I. Molina
Polymers 2020, 12(8), 1642; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12081642 - 23 Jul 2020
Cited by 4 | Viewed by 3445
Abstract
Stereolithography is an additive manufacturing technology commonly used to build either prototypes or final parts. Nevertheless, the manufacture of structural parts has been ruled out owing to the poor mechanical properties of conventional UV-curable resins. Moreover, the inventory of available commercial resins is [...] Read more.
Stereolithography is an additive manufacturing technology commonly used to build either prototypes or final parts. Nevertheless, the manufacture of structural parts has been ruled out owing to the poor mechanical properties of conventional UV-curable resins. Moreover, the inventory of available commercial resins is still limited and they exhibit low thermal and electrical conductivity values. In this work, some composite materials were designed using Al microparticles dispersed within an SLA commercial resin matrix. These composites overcame the difficulties caused by the light scattering effect during the photopolymerisation process in the SLA technology. Dispersion of the filler was characterised by means of SEM/EDX and AFM. The composites exhibited improved thermal and mechanical behaviour in comparison with the pristine resin. The simplicity of the synthesis method used to prepare the composites provides a convenient starting point to explore new ways of designing composites for SLA with improved mechanical and functional properties. Full article
(This article belongs to the Special Issue Polymeric Materials in 3D and 4D Printing)
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18 pages, 10016 KiB  
Article
Tribological Behaviour of Additively Manufactured Fiber-Reinforced Thermoplastic Composites in Various Environments
by Artur Prusinowski and Roman Kaczyński
Polymers 2020, 12(7), 1551; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12071551 - 13 Jul 2020
Cited by 8 | Viewed by 2960
Abstract
Polymer composites with increased utility properties are becoming competition for conventional materials, in conjunction with additive manufacturing techniques. The aim of this study was to evaluate tribological characteristics of fibrous composites produced in fused deposition modeling (FDM) with the use of an innovative [...] Read more.
Polymer composites with increased utility properties are becoming competition for conventional materials, in conjunction with additive manufacturing techniques. The aim of this study was to evaluate tribological characteristics of fibrous composites produced in fused deposition modeling (FDM) with the use of an innovative head with symmetrical feeding of the matrix material. Analysis of the influence of composite-forming temperature on their tribological properties allowed the determining of the optimal printing process parameters for this group of composites. Significant differences in the friction process of the same reinforced materials were observed in dry and wet environments. Fibrous composites showed 10 times lower wear intensity as well as two times lower friction value in water than in air. Research shows friction in the water environment ensures more even wear of the surface of the composites involved in the work. The article contains 3D microscopic imaging of the friction plane of the tested composites and a description of a typical course of material wear is described. Full article
(This article belongs to the Special Issue Polymeric Materials in 3D and 4D Printing)
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17 pages, 6785 KiB  
Article
Synthesis and Formulation of PCL-Based Urethane Acrylates for DLP 3D Printers
by Hsuan Chen, Shyh-Yuan Lee and Yuan-Min Lin
Polymers 2020, 12(7), 1500; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12071500 - 5 Jul 2020
Cited by 39 | Viewed by 9948
Abstract
In this study, three PCL-based polyurethane acrylates were synthesized and further formulated into twelve resins for digital light processing (DLP) 3D printing. Three PCL diols with different molecular weights were synthesized via ring-opening reaction of ε-caprolactone on diethylene glycol, with the catalyst stannous [...] Read more.
In this study, three PCL-based polyurethane acrylates were synthesized and further formulated into twelve resins for digital light processing (DLP) 3D printing. Three PCL diols with different molecular weights were synthesized via ring-opening reaction of ε-caprolactone on diethylene glycol, with the catalyst stannous octoate. Isophorone diisocyanate (IPDI) was reacted with 2-hydroxyethyl acrylate (2-HEA) and the PCL diols form PCL-based polyurethane acrylates. Twelve resins composed of different percentages of PCL-based polyurethane acrylates, poly (ethylene glycol) diacrylate (PEGDA), propylene glycol (PPG) and photo-initiator were further printed from a DLP 3D printer. The viscosities of twelve resins decreased by 10 times and became printable after adding 30% of PEGDA. The degree of conversion for the twelve resins can reach more than 80% after the post-curing process. By changing the amount of PEGDA and PPG, the mechanical properties of the twelve resins could be adjusted. PUA530-PEG-PPG (70:30:0), PUA800-PEG-PPG (70:30:0), and PUA1000-PEG-PPG (70:30:0) were successfully printed into customized tissue scaffolds. Twelve PCL-based polyurethane photo-curable resins with tunable mechanical properties, cytotoxicity, and degradability were successfully prepared. With the DLP 3D printing technique, a complex structure could be achieved. These resins have great potential for customized tissue engineering and other biomedical application. Full article
(This article belongs to the Special Issue Polymeric Materials in 3D and 4D Printing)
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17 pages, 9856 KiB  
Article
Assessment of the Release of Vascular Endothelial Growth Factor from 3D-Printed Poly-ε-Caprolactone/Hydroxyapatite/Calcium Sulfate Scaffold with Enhanced Osteogenic Capacity
by Cheng-Yu Chen, Chien-Chang Chen, Chen-Ying Wang, Alvin Kai-Xing Lee, Chun-Liang Yeh and Chun-Pin Lin
Polymers 2020, 12(7), 1455; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12071455 - 29 Jun 2020
Cited by 35 | Viewed by 3247
Abstract
Vascular endothelial growth factor (VEGF) is one of the most crucial growth factors and an assistant for the adjustment of bone regeneration. In this study, a 3D scaffold is fabricated using the method of fused deposition modeling. Such a fabricated method allows us [...] Read more.
Vascular endothelial growth factor (VEGF) is one of the most crucial growth factors and an assistant for the adjustment of bone regeneration. In this study, a 3D scaffold is fabricated using the method of fused deposition modeling. Such a fabricated method allows us to fabricate scaffolds with consistent pore sizes, which could promote cellular ingrowth into scaffolds. Therefore, we drafted a plan to accelerate bone regeneration via VEGF released from the hydroxyapatite/calcium sulfate (HACS) scaffold. Herein, HACS will gradually degrade and provide a suitable environment for cell growth and differentiation. In addition, HACS scaffolds have higher mechanical properties and drug release compared with HA scaffolds. The drug release profile of the VEGF-loaded scaffolds showed that VEGF could be loaded and released in a stable manner. Furthermore, initial results showed that VEGF-loaded scaffolds could significantly enhance the proliferation of human mesenchymal stem cells (hMSCs) and human umbilical vein endothelial cells (HUVEC). In addition, angiogenic- and osteogenic-related proteins were substantially increased in the HACS/VEGF group. Moreover, in vivo results revealed that HACS/VEGF improved the regeneration of the rabbit’s femur bone defect, and VEGF loading improved bone tissue regeneration and remineralization after implantation for 8 weeks. All these results strongly imply that the strategy of VEGF loading onto scaffolds could be a potential candidate for future bone tissue engineering. Full article
(This article belongs to the Special Issue Polymeric Materials in 3D and 4D Printing)
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