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3D Printing of Polymer Materials: Recent Advances and Future Perspectives

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

Deadline for manuscript submissions: 28 February 2025 | Viewed by 14281

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Dr. Michael A. Smirnov

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Institute of Macromolecular Compounds, Russian Academy of Sciences, V.O. Bolshoi Pr. 31, 199004 St. Petersburg, Russia
Interests: 3D printing; polymer chemistry; physical chemistry of polymer materials; electroactive polymers; polymer electrochemistry; carbohydrate polymers; deep eutectic solvents; polymer composites; ionic liquids; polymer ion gels

Dr. Maria P. Sokolova

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Institute of Macromolecular Compounds, Russian Academy of Sciences, V.O. Bolshoi Pr. 31, 199004 St. Petersburg, Russia
Interests: atomic force microscopy; scanning and transmission electron microscopy; X-ray diffraction analysis; structure of polymers; nano- and microstructures; carbohydrate polymeric materials; composite materials; deep eutectic solvents

Special Issue Information

Dear Colleagues,

The 3D printing of polymer materials is an intensively developed technology intended for the preparation of complex shaped materials with various mechanical properties. In spite of significant progress in 3D printing, obtaining advanced polymer materials such as composites, materials with ultimate mechanical or tailored functional properties, remains a challenge. Among others, polymer gels (“soft materials”) are subject to intensive study because they are often capable of mimicking the mechanical behavior of natural tissues and objects. Due to the opening of new opportunities for customization and personalization of products in the field of biomaterials, robotics, food science and technology, cell tissue engineering, and others, the development of production methods for polymer gels with arbitrary geometries has attracted significant attention in previous years. Inks applied for this process consist of artificial or natural polymers compatible with the used solvent, which is usually water. New types of solvents, namely ionic liquids and deep eutectic solvents, are also studied in the context of the elaboration of compositions with improved printability.

The main avenue of research on the way toward better printable compositions is the interplay between their rheological characteristics, which determine the printing performance and mechanical properties of the final material. In the case of gels, the problem of shape fidelity arises because of their slow structure recovery after extrusion and possible solvent evaporation. Additionally, the physico-chemical and often biological properties of printed materials should be taken into account, and this narrows the choice of possible components of printable composition. The chemical challenge is the elaboration of new shape fixation methods for gels via a suitable physical or chemical crosslinking process that meet the requirements of subsequent applications of the printed material, and the investigation of the influence of this process on the functional properties of the obtained gel product. New printing and curing strategies are also needed in order to achieve better interlayer adhesiveness and improve the mechanical characteristics of end products.

This Special Issue welcomes (but is not limited to) papers on 3D printing of polymer materials based on a wide range of synthetic or natural polymers, including theoretical and experimental studies of their rheological properties, crosslinking, and printing accuracy, as well as investigations of practical applications of 3D printed polymer materials.

Dr. Michael A. Smirnov
Dr. Maria P. Sokolova
Guest Editors

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Keywords

3D printing
additive manufacturing
printing accuracy
polymer materials
composites
polymer gels
rheology
crosslinking
properties of materials

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Research

17 pages, 6685 KiB

Open AccessArticle

Flexural Response Comparison of Nylon-Based 3D-Printed Glass Fiber Composites and Epoxy-Based Conventional Glass Fiber Composites in Cementitious and Polymer Concretes

by Abdirahman Ahmed Haibe and Shreya Vemuganti

Polymers 2025, 17(2), 218; https://doi.org/10.3390/polym17020218 - 16 Jan 2025

Viewed by 488

Abstract

With 3D printing technology, fiber-reinforced polymer composites can be printed with radical shapes and properties, resulting in varied mechanical performances. Their high strength, light weight, and corrosion resistance are already advantages that make them viable for physical civil infrastructure. It is important to understand these composites’ behavior when used in concrete, as their association can impact debonding failures and overall structural performance. In this study, the flexural behavior of two designs for 3D-printed glass fiber composites is investigated in both Portland cement concrete and polymer concrete and compared to conventional fiber-reinforced polymer composites manufactured using a wet layup method. Thermogravimetric analysis, volume fraction calculations, and tensile tests were performed to characterize the properties of the fiber-reinforced polymer composites. Flexural testing was conducted by a three-point bending setup, and post-failure analysis was performed using microscopic images. Compared to concretes with no FRP reinforcement, the incorporation of 3D-printed glass-fiber-reinforced polymer composites in cementitious concrete showed a 16.8% increase in load-carrying capacity, and incorporation in polymer concrete showed a 90% increase in flexural capacity. In addition, this study also provides key insights into the capabilities of polymer concrete to penetrate layers of at least 90 microns in 3D-printed composites, providing fiber bridging capabilities and better engagement resulting in improved bond strength that is reflected in mechanical performance. The polymer material has a much lower viscosity of 8 cps compared to the 40 cps viscosity of the cement slurry. This lower viscosity results in improved penetration, increasing contact surface area, with the reinforcement consequently improving bond strength. Overall, this work demonstrates that 3D-printed fiber-reinforced polymer composites are suitable for construction and may lead to the development of advanced concrete-based reinforced composites that can be 3D-printed with tailored mechanical properties and performance. Full article

(This article belongs to the Special Issue 3D Printing of Polymer Materials: Recent Advances and Future Perspectives)

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14 pages, 1875 KiB

Open AccessArticle

Selection of Network Parameters in Direct ANN Modeling of Roughness Obtained in FFF Processes

by Irene Buj-Corral, Maurici Sivatte-Adroer, Lourdes Rodero-de-Lamo and Lluís Marco-Almagro

Polymers 2025, 17(1), 120; https://doi.org/10.3390/polym17010120 - 6 Jan 2025

Viewed by 579

Abstract

Artificial neural network (ANN) models have been used in the past to model surface roughness in manufacturing processes. Specifically, different parameters influence surface roughness in fused filament fabrication (FFF) processes. In addition, the characteristics of the networks have a direct impact on the performance of the models. In this work, a study about the use of ANN to model surface roughness in FFF processes is presented. The main objective of the paper is discovering how key ANN parameters (specifically, the number of neurons, the training algorithm, and the percentage of training and validation datasets) affect the accuracy of surface roughness predictions. To address this question, 125 3D printing experiments were conducted changing orientation angle, layer height and printing temperature, and measuring average roughness Ra as response. A multilayer perceptron neural network model with backpropagation algorithm was used. The study evaluates the effect of three ANN parameters: (1) number of neurons in the hidden layer (4, 5, 6 or 7), (2) training algorithm (Levenberg–Marquardt, Resilient Backpropagation or Scaled Conjugate Gradient), and (3) data splitting ratios (70%–15%–15% vs. 55%–15%–30%). Mean Absolute Error (MAE) was used as the performance metric. The Resilient Backpropagation algorithm, 7 neurons, and using 55% of training data yielded the best predictive performance, minimizing the MAE. Additionally, the impact of the dataset size on prediction accuracy was analysed. It was observed that the performance of the ANN gets worse as the number of datasets is reduced, emphasizing the importance of having sufficient data. This study will help to select appropriate values for the printing parameters in FFF processes, as well as to define the characteristics of the ANN to be used to model surface roughness. Full article

(This article belongs to the Special Issue 3D Printing of Polymer Materials: Recent Advances and Future Perspectives)

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13 pages, 7300 KiB

Open AccessArticle

The Use of Terahertz Computed Tomography and Time Domain Spectroscopy to Evaluate Symmetry in 3D Printed Parts

by Dolores Termini, John Federici, Ian Gatley and Louis Rizzo

Polymers 2024, 16(23), 3296; https://doi.org/10.3390/polym16233296 - 26 Nov 2024

Viewed by 586

Abstract

3D printing has become essential to many fields for its low-cost production and rapid prototyping abilities. As 3D printing becomes an alternative manufacturing tool, developing methods to non-destructively evaluate defects for quality control is essential. This study integrates the non-destructive terahertz (THz) analysis methods of terahertz time-domain spectroscopy (THz-TDS) and terahertz computed tomography (THz CT) to image and assess 3D printed resin structures for defects. The terahertz images were reconstructed using MATLAB, and the rotational symmetry of various structures before and after the introduction of defects was evaluated by calculating the mean squared deviation (MSD), which served as a symmetry parameter to indicate the presence of defects. Structures A and B had MSD values that were at least three standard deviations larger after introducing defects to their structures, showing a significant change in symmetry and indicating the existence of defects. Similarly, in structure C, blockages in parts made with different post-cures were identified based on the increase in MSD values for those slices. For structure D, the presence of a defect increased the MSD value by 14%. The results of this study verify that the MSD calculated for the rotational symmetry of the structures was greater when defects were present, accurately reflecting the anticipated breaks in symmetry. This paper demonstrates that terahertz imaging, combined with MSD analysis, is a viable procedure to identify and quantify defects in rotationally symmetric 3D printed structures. Full article

(This article belongs to the Special Issue 3D Printing of Polymer Materials: Recent Advances and Future Perspectives)

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18 pages, 6447 KiB

Open AccessArticle

Mechanical Strength of Additive Manufactured and Standard Polymeric Components Joined Through Structural Adhesives

by Andrea Spaggiari and Simone Orlandini

Polymers 2024, 16(21), 3036; https://doi.org/10.3390/polym16213036 - 29 Oct 2024

Viewed by 789

Abstract

The main aim of this work is to evaluate the mechanical properties of additive manufactured polymeric parts joined with standard plastic parts through structural adhesives. The primary advantage of this technique is its ability to significantly increase the size of the final assembly by using additive manufacturing (AM) for complex joints and inexpensive, reliable extruded plastic parts for load-bearing components. This hybrid assembly combines the flexibility and shape adaptability of AM with the structural strength and cost-effectiveness of extruded polymer parts, resulting in a final design that performs comparably to the base material. The materials used in the paper are rigid acrylic adhesive and toughened acrylic, both applicable with almost no surface preparation and fast curing. The 3D-printed parts are produced in ABS, while the standard parts are in PVC. First, the work is devoted to estimating the performance of the adhesives using pin–collar joints and a combined numerical and experimental methodology. The second section presents and discusses the results of two more realistic applications of adhesive bonding to hybrid complex joints. For the pin–collar joints, the results show failure mostly in the adhesive, with an average shear stress of 11.5 MPa and 5.22 MPa and a stiffness of 4449 N/mm and 3649 N/mm for the rigid and toughened adhesives, respectively. The results of the adhesive bonding of structural joints show that the adhesive is always capable of providing the load-carrying capacity required to achieve the strength of traditionally manufactured polymeric parts. The paper shows that adhesives are a feasible way to expand the potential of 3D-printed equipment to obtain larger hybrid parts partially realized with traditional technology, especially with inexpensive off-the-shelf bars and sections. Full article

(This article belongs to the Special Issue 3D Printing of Polymer Materials: Recent Advances and Future Perspectives)

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18 pages, 8898 KiB

Open AccessArticle

The Influence of Printing Speed and Temperature on the Mechanical, Absorptive, and Morphological Properties of PLA-Based Hybrid Materials Produced with an FDM-Type 3D Printer

by Rumeysa İncesu and Tarkan Akderya

Polymers 2024, 16(19), 2771; https://doi.org/10.3390/polym16192771 - 30 Sep 2024

Viewed by 1453

Abstract

Composite materials are used in many engineering applications and industrial fields due to their superior properties, such as high strength, lightweight, and stiffness. These outstanding properties have made these materials an alternative to metallic materials. The vital need for new lightweight and inexpensive materials with superior strength properties has led to research on “hybridisation”. Hybrid composites with more than one type of polymer in the same structure are needed to achieve a better balance of properties and to combine many desired properties in a single material. Many researchers have studied the hybrid effect and contributed to the understanding and modelling of the subject. Studies to explain the primary mechanism of the hybrid effect are limited and insufficient to explain the complex interaction. In this study, a three-dimensional printer using fused deposition modelling technique was used to produce hybrid materials, and the influence of printing parameters on the mechanical, absorptive, and morphological properties of poly (lactic acid) (PLA), Tough PLA, and PLA/Tough PLA hybrid materials were investigated. The hybrid material form exhibited superior properties when selecting specific production parameters from individual raw elements. It can be said that the mechanical properties of the PLA/Tough PLA hybrid material increased with the increase in production temperature. Full article

(This article belongs to the Special Issue 3D Printing of Polymer Materials: Recent Advances and Future Perspectives)

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19 pages, 5627 KiB

Open AccessArticle

Precisely Printable Silk Fibroin/Carboxymethyl Cellulose/Alginate Bioink for 3D Printing

by Yuliya Nashchekina, Anastasia Militsina, Vladimir Elokhovskiy, Elena Ivan’kova, Alexey Nashchekin, Almaz Kamalov and Vladimir Yudin

Polymers 2024, 16(8), 1027; https://doi.org/10.3390/polym16081027 - 9 Apr 2024

Cited by 2 | Viewed by 2334

Abstract

Three-dimensional (3D) bioprinting opens up many possibilities for tissue engineering, thanks to its ability to create a three-dimensional environment for cells like an extracellular matrix. However, the use of natural polymers such as silk fibroin in 3D bioprinting faces obstacles such as having a limited printability due to the low viscosity of such solutions. This study addresses these gaps by developing highly viscous, stable, and biocompatible silk fibroin-based inks. The addition of 2% carboxymethyl cellulose sodium and 1% sodium alginate to an aqueous solution containing 2.5 to 5% silk fibroin significantly improves the printability, stability, and mechanical properties of the printed scaffolds. It has been demonstrated that the more silk fibroin there is in bioinks, the higher their printability. To stabilize silk fibroin scaffolds in an aqueous environment, the printed structures must be treated with methanol or ethanol, ensuring the transition from the silk fibroin’s amorphous phase to beta sheets. The developed bioinks that are based on silk fibroin, alginate, and carboxymethyl cellulose demonstrate an ease of printing and a high printing quality, and have a sufficiently good biocompatibility with respect to mesenchymal stromal cells. The printed scaffolds have satisfactory mechanical characteristics. The resulting 3D-printing bioink composition can be used to create tissue-like structures. Full article

(This article belongs to the Special Issue 3D Printing of Polymer Materials: Recent Advances and Future Perspectives)

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19 pages, 3949 KiB

Open AccessArticle

The Influence of Selected Fillers on the Functional Properties of Polycarbonate Dedicated to 3D Printing Applications

by Katarzyna Bulanda, Mariusz Oleksy and Rafał Oliwa

Polymers 2024, 16(5), 592; https://doi.org/10.3390/polym16050592 - 21 Feb 2024

Cited by 4 | Viewed by 1473

Abstract

Additive manufacturing is still the fastest-developing technology in the modern world. Three-dimensional printing has become popular due to the method’s numerous advantages, such as its short time and low cost, compared to conventional methods such as injection molding. Therefore, the demand for new materials and material systems that will be characterized by the desired functional properties is clearly growing. As part of this work, work was carried out on the development and preparation of new polymer composites dedicated to 3D printing applications, especially in FDM/FFF/MEM technologies. The influence of the content and amount of fillers, such as silica modified with alumina (S) and bentonite modified with a quaternary ammonium salt (B), on the functional properties of a commercially available fiber made of traditional plastic, such as polycarbonate, obtained in the form of a filament (PCF), was determined. It was found that the addition of B significantly increased the fluidity of the polymer, the introduction of a filler in the amount of 1.5% allowed to obtain a result that was 6% higher compared to PCF (16.8 g/10 min), while the amount of 3% was 20% higher. The obtained mass melt flow rate (MFR) results were confirmed by determining the viscosity of the produced polymer composites. Satisfactory results of mechanical properties were obtained, including the following: it was found that the introduced modified fillers increased the elasticity of the material. The introduction of modified silica resulted in a reduction in Young’s modulus by 10.02% at the content of 0.5% S and at 1% S by 8.64% compared to the polymer. The introduced modified filler S significantly increased the thermostability of polycarbonate (T_5% equal to 449 °C) by 23 °C for PCF/0.5% S and 14 °C for PCF/1% S, respectively. The SEM and WAXS results confirmed the appropriate dispersion of the fillers in the polymer matrix, which indicates well-selected conditions for the homogenization process of the components and the subsequent production of samples. Detailed characterization of the influence of selected fillers on the functional properties of the polymer matrix-polycarbonate allowed for an increase in the range of polymer composites and their use in rapid prototyping technologies, as well as supplementing the literature on databases regarding the characteristics of the obtained materials. Full article

(This article belongs to the Special Issue 3D Printing of Polymer Materials: Recent Advances and Future Perspectives)

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24 pages, 8460 KiB

Open AccessArticle

Drug Loaded 3D-Printed Poly(ε-Caprolactone) Scaffolds for Local Antibacterial or Anti-Inflammatory Treatment in Bone Regeneration

by Mariia Stepanova, Ilia Averianov, Iosif Gofman, Natalia Shevchenko, Artem Rubinstein, Tatiana Egorova, Andrey Trulioff, Yulia Nashchekina, Igor Kudryavtsev, Elena Demyanova, Evgenia Korzhikova-Vlakh and Viktor Korzhikov-Vlakh

Polymers 2023, 15(19), 3957; https://doi.org/10.3390/polym15193957 - 30 Sep 2023

Cited by 6 | Viewed by 2456

Abstract

Annual bone grafting surgeries due to bone fractures, resections of affected bones, skeletal anomalies, osteoporosis, etc. exceed two million worldwide. In this regard, the creation of new materials for bone tissue repair is one of the urgent tasks of modern medicine. Additive manufacturing, or 3D printing, offers great opportunities for the development of materials with diverse properties and designs. In this study, the one-pot technique for the production of 3D scaffolds based on poly(ε-caprolactone) (PCL) loaded with an antibiotic or anti-inflammatory drug was proposed. In contrast to previously described methods to prepare drug-containing scaffolds, drug-loaded PCL scaffolds were prepared by direct 3D printing from a polymer/drug blend. An investigation of the mechanical properties of 3D-printed scaffolds containing 0.5–5 wt% ciprofloxacin (CIP) or dexamethasone (DEX) showed almost no effect of the drug (compression modulus ~70–90 MPa) compared to unfilled PCL (74 MPa). At the same time, introducing the drug and increasing its content in the PCL matrix contributed to a 1.8–6.8-fold decrease in the specific surface area of the scaffold, depending on composition. The release of CIP and DEX in phosphate buffer solution and in the same buffer containing lipase revealed a faster release in enzyme-containing medium within 45 days. Furthermore, drug release was more intensive from scaffolds with a low drug load. Analysis of the release profiles using a number of mathematical dissolution models led to the conclusion that diffusion dominates over other probable factors. In vitro biological evaluation of the scaffolds containing DEX showed moderate toxicity against osteoblast-like and leukemia monocytic cells. Being 3D-printed together with PCL both drugs retain their biological activity. PCL/CIP and PCL/DEX scaffolds demonstrated antibacterial properties against Pseudomonas aeruginosa (a total inhibition after 48 h) and anti-inflammatory activity in experiments on TNFα-activated monocyte cells (a 4-time reduction in CD-54 expression relative to control), respectively. Full article

(This article belongs to the Special Issue 3D Printing of Polymer Materials: Recent Advances and Future Perspectives)

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21 pages, 7372 KiB

Open AccessArticle

Study on the Equation of State and Jet Forming of 3D-Printed PLA and PLA-Cu Materials

by Jianya Yi, Ruijie Hao, Qing Ji, Siman Guan, Zhijun Wang and Jianping Yin

Polymers 2023, 15(17), 3564; https://doi.org/10.3390/polym15173564 - 28 Aug 2023

Viewed by 1442

Abstract

In order to improve the research and development efficiency and quality of low-density liners in production and scientific research development, PLA and PLA-Cu composite liners were prepared based on 3D-printing technology. In this paper, the relationship between the shock wave velocity D and the particle velocity u of PLA and PLA-Cu materials was tested by a one-stage light gas gun experiment device, and then the Grüneisen equation of state parameters of the two materials was obtained by fitting. The forming process of the two jets was numerically simulated by using the equation of state. When combined with the pulsed X-ray shooting results of the jets, it was found that the jets of the two materials showed obvious characteristics of “expansion particle flow”, and the head of the PLA jet had a gasification phenomenon. The length of the PLA jet at 20 μs in the numerical simulation was 127.2 mm, and the average length of the PLA jet at 20 μs in the pulsed X-ray shooting experiment was 100.45 mm. The length of the PLA jet gasification part accounted for about 21% of the total length of the jet. The average velocity of the head of the PLA jet is 7798.35 m/s, and the average velocity of the head of the PLA-Cu jet is 8104.25 m/s. In this paper, 3D-printing technology is used to prepare the liner for the first time, aiming to open up a new preparation technology and provide a new material selection for low-density material liners. Full article

(This article belongs to the Special Issue 3D Printing of Polymer Materials: Recent Advances and Future Perspectives)

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16 pages, 2508 KiB

Open AccessArticle

Three-Dimensional Printed Shape Memory Gels Based on a Structured Disperse System with Hydrophobic Cellulose Nanofibers

by Angelina P. Prosvirnina, Alexander N. Bugrov, Natalya V. Bobrova, Eugene V. Sivtsov, Alexandra L. Nikolaeva, Almaz M. Kamalov, Maria P. Sokolova and Michael A. Smirnov

Polymers 2023, 15(17), 3547; https://doi.org/10.3390/polym15173547 - 26 Aug 2023

Cited by 3 | Viewed by 1420

Abstract

Inks for 3D printing were prepared by dispersing bacterial cellulose nanofibers (CNF) functionalized with methacrylate groups in a polymerizable deep eutectic solvent (DES) based on choline chloride and acrylic acid with water as a cosolvent. After 3D printing and UV-curing, the double-network composite gel consisting of chemically and physically crosslinked structures composed from sub-networks of modified CNF and polymerized DES, respectively, was formed. The rheological properties of inks, as well as mechanical and shape memory properties of the 3D-printed gels, were investigated in dynamic and static modes. It was shown that the optimal amount of water allows improvement of the mechanical properties of the composite gel due to the formation of closer contacts between the modified CNF. The addition of 12 wt% water results in an increase in strength and ultimate elongation to 11.9 MPa and 300%, respectively, in comparison with 5.5 MPa and 100% for an anhydrous system. At the same time, the best shape memory properties were found for an anhydrous system: shape fixation and recovery coefficients were 80.0 and 95.8%, respectively. Full article

(This article belongs to the Special Issue 3D Printing of Polymer Materials: Recent Advances and Future Perspectives)

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