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Search Results (1,969)

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15 pages, 31617 KiB  
Article
The Effect of the Conformation Process on the Physicochemical Properties of Carboxymethylcellulose–Starch Hydrogels
by Priscila Vedovello, Robert Silva Paiva, Ricardo Bortoletto-Santos, Caue Ribeiro and Fernando Ferrari Putti
Gels 2025, 11(3), 183; https://doi.org/10.3390/gels11030183 - 6 Mar 2025
Abstract
This study discusses the preparation of biopolymeric hydrogels (a biomaterial) via different techniques, such as casting and extrusion, to compare the effects of the process and the use of citric acid as a crosslinker on the morphology, physicochemical properties, and degree of swelling [...] Read more.
This study discusses the preparation of biopolymeric hydrogels (a biomaterial) via different techniques, such as casting and extrusion, to compare the effects of the process and the use of citric acid as a crosslinker on the morphology, physicochemical properties, and degree of swelling of the hydrogel. Casting is widely used for its low cost and space-saving nature, but upscaling is problematic. Extrusion offers a way to produce materials in large quantities; these materials can undergo mechanical and thermal energy, which can significantly alter their properties. The samples obtained by extrusion had porous surfaces, which are critical for the water penetration and swelling of superabsorbent hydrogels. In contrast, the hydrogels produced by casting did not form pores, resulting in a lower degree of swelling. Extrusion increased the degree of swelling threefold due to the formation of pores, influencing water absorption and diffusion dynamics, especially in samples with higher starch content, where crosslinking occurred more effectively. Full article
(This article belongs to the Special Issue Recent Advances in Multi-Functional Hydrogels)
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Figure 1
<p>FTIR spectra of samples: (<b>a</b>) casting, (<b>b</b>) extrusion, and (<b>c</b>) pure components.</p>
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<p>TGA (black color) and derived thermogravimetric analysis (DTG) (blue color) of CMC: (<b>a</b>) casting and (<b>b</b>) extrusion.</p>
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<p>TGA and DTG analysis of CMC/S: (<b>a</b>) casting and (<b>b</b>) extrusion.</p>
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<p>X-ray diffraction (XRD) patterns of CMC, starch, and their respective formulations: (<b>a</b>) casting and (<b>b</b>) extrusion.</p>
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<p>Complex viscosity versus angular frequency for samples with varying CMC/S ratios was prepared using (<b>a</b>) casting and (<b>b</b>) mechanical extrusion.</p>
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<p>The SEMs of the cryogenic fracture surface of the composites obtained by (<b>a</b>) casting and (<b>b</b>) extrusion: 1. CMC pure; 2. 90/10 wt. CMC/S; 3. 75/25 wt. CMC/S, and 4. 50/50 wt. CMC/S.</p>
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<p>The SEMs of the cryogenic fracture surface of the composites obtained by (<b>a</b>) casting and (<b>b</b>) extrusion: 1. CMC pure; 2. 90/10 wt. CMC/S; 3. 75/25 wt. CMC/S, and 4. 50/50 wt. CMC/S.</p>
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<p>The swelling ratio of CMC/S: (<b>a</b>) casting and (<b>b</b>) extrusion.</p>
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<p>The percentage of the porosity of the samples obtained by extrusion.</p>
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<p>Schematic diagram of the different manufacturing processes of hydrogels. Created by Canvas<sup>®</sup>.</p>
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17 pages, 3924 KiB  
Article
Photo- and Schiff Base-Crosslinkable Chitosan/Oxidized Glucomannan Composite Hydrogel for 3D Bioprinting
by Mitsuyuki Hidaka and Shinji Sakai
Polysaccharides 2025, 6(1), 19; https://doi.org/10.3390/polysaccharides6010019 - 4 Mar 2025
Viewed by 113
Abstract
Chitosan is an attractive material for developing inks for extrusion-based bioprinting of 3D structures owing to its excellent properties, including its mechanical properties and antimicrobial activity when used in wound dressings. A key challenge in formulating chitosan-based inks is to improve its gelation [...] Read more.
Chitosan is an attractive material for developing inks for extrusion-based bioprinting of 3D structures owing to its excellent properties, including its mechanical properties and antimicrobial activity when used in wound dressings. A key challenge in formulating chitosan-based inks is to improve its gelation property to ensure reliable printing and the mechanical stability of the printed structures. To address these challenges, this article presents a novel chitosan/oxidized glucomannan composite hydrogel obtained through the combination of Schiff base and phenol crosslinking reactions. The proposed biomaterial forms soft hydrogels through Schiff base crosslinking, which can be further stabilized via visible light-induced phenol crosslinking. This dual-crosslinking approach enhances the printability and robustness of chitosan-based ink materials. The proposed chitosan/oxidized glucomannan hydrogel exhibits excellent extrudability and improved shape retention after extrusion, along with antimicrobial properties against Escherichia coli. Moreover, good cytocompatibility was confirmed in animal cell studies using mouse fibroblast 10T1/2 cells. These favorable features make this hydrogel highly promising for the extrusion-based bioprinting of complex 3D structures, such as tubes and nose-like structures, at a low crosslinker concentration and can expand the prospects of chitosan in bioprinting, providing a safer and more efficient alternative for tissue engineering and other biomedical applications. Full article
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Graphical abstract

Graphical abstract
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<p>(<b>a</b>) Derivatization of chitosan with phenol moieties; (<b>b</b>) phenol crosslinking of ChPh; (<b>c</b>) oxidation of glucomannan; (<b>d</b>) Schiff base (imine) crosslinking of ChPh and Ox-glucomannan; (<b>e</b>) Concept of this study.</p>
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<p>FTIR spectra of glucomannan and Ox-glucomannan.</p>
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<p>Extrudabilities of ChPh (<b>upper left</b>), ChPh-Ox25 (<b>upper middle</b>), ChPh-Ox50 (<b>upper right</b>), ChPh-Ox100 (<b>lower left</b>), ChPh-Ox200 (<b>lower middle</b>), and ChPh-Ox300 (<b>lower right</b>) hydrogels containing 2.0 mM SPS and 1.0 mM Ru(bpy)<sub>3</sub>. The samples were extruded from a syringe.</p>
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<p>Rheological behaviors of (<b>a</b>) ChPh, (<b>b</b>) ChPh-Ox25, (<b>c</b>) ChPh-Ox50, (<b>d</b>) ChPh-Ox100, (<b>e</b>) glucomannan, (<b>f</b>) ChPh and glucomannan, and (<b>g</b>) Ox-glucomannan under varied strain (5–1000%) at 1.6 kHz frequency. Solid circles (G′) and open circles (G″).</p>
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<p>Changes in G′ and G″ over time under visible-light exposure (0.2 W/m<sup>2</sup> @ 452 nm) for (<b>a</b>) ChPh, (<b>b</b>) ChPh-Ox25, (<b>c</b>) ChPh-Ox50, and (<b>d</b>) ChPh-Ox100 containing 2.0 mM SPS and 1.0 mM Ru(bpy)<sub>3</sub> under 5% strain at 0.3 kHz frequency.</p>
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<p>(<b>a</b>) Swelling behaviors of the ChPh, ChPh-Ox25, ChPh-Ox50, and ChPh-Ox100 hydrogels over 72 h. Data: mean ± standard deviation (<span class="html-italic">n</span> = 3–4, <span class="html-italic">n.s.</span>: <span class="html-italic">p</span> &gt; 0.05). Each hydrogel contained 2.0 mM SPS and 1.0 mM Ru(bpy)<sub>3</sub> and was exposed to visible light (0.2 W/m<sup>2</sup> @ 452 nm) for 10 min. (<b>b</b>) Photographs of the ChPh, ChPh-Ox25, ChPh-Ox50, and ChPh-Ox100 hydrogels before and after immersion in PBS. Scale bars: 5 mm.</p>
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<p>Swelling behaviors of ChPh-Ox50 with and without phenol crosslinking in (<b>a</b>) acidic and (<b>b</b>) neutral conditions (scale bars: 5 mm). (<b>c</b>) Effect of pH on the swelling of ChPh-Ox50 hydrogels obtained through Schiff base and phenol crosslinking. For phenol crosslinking, the hydrogel samples containing 2.0 mM SPS and 1.0 mM Ru(bpy)<sub>3</sub> were exposed to the visible light (0.2 W/m<sup>2</sup> @ 452 nm) for 10 min. Data: mean ± standard deviation (<span class="html-italic">n</span> = 4).</p>
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<p>Cell behaviors on a cell culture dish and ChPh, ChPh-Ox25, ChPh-Ox50, and ChPh-Ox100 hydrogel specimens during 3 days of incubation (Scale bars: 250 µm). For phenol crosslinking, the hydrogel samples containing 2.0 mM SPS and 1.0 mM Ru(bpy)<sub>3</sub> were exposed to the visible light (0.2 W/m<sup>2</sup> @ 452 nm) for 10 min.</p>
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<p>Antimicrobial activities of ChPh, ChPh-Ox25, ChPh-Ox50, and ChPh-Ox100 hydrogels containing 2.0 mM SPS and 1.0 mM Ru(bpy)<sub>3</sub>. (<b>a</b>) Photographs of the bacterial suspensions incubated with hydrogel samples for 24 h. (<b>b</b>) CFU values of the suspensions after 24 h of incubation. Data: mean ± standard deviation (<span class="html-italic">n</span> = 3).</p>
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<p>(<b>a</b>) Image of extrusion-based 3D printing using ChPh-Ox glucomannan ink. (<b>b</b>) Comparison of the printability of the ChPh, ChPh-Ox25, ChPh-Ox50, and ChPh-Ox100 hydrogels in printing 3D structures using an extrusion-based 3D printer: (upper) tubular structure, (middle and bottom) top and side views of a nose structure, respectively (scale bars: 5 mm). Each ink contained 2.0 mM SPS and 1.0 mM Ru(bpy)<sub>3</sub>.</p>
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15 pages, 10753 KiB  
Article
The Influence of Li on the Fracture Characteristics and Mechanical Properties of Extruded Beryllium–Aluminum Composites
by Wentong Li, Yixiao Xia, Yutong Sun, Juanrui Hu, Leilei Hao, Yun Liu, Boyu Ju, Guoqin Chen and Wenshu Yang
Materials 2025, 18(5), 1055; https://doi.org/10.3390/ma18051055 - 27 Feb 2025
Viewed by 161
Abstract
Alloying is an important method to improve the mechanical properties of beryllium–aluminum composites. In this study, two kinds of beryllium–aluminum composites with and without Li were prepared by pressure impregnation method and extrusion, and the effects of Li on the microstructure and mechanical [...] Read more.
Alloying is an important method to improve the mechanical properties of beryllium–aluminum composites. In this study, two kinds of beryllium–aluminum composites with and without Li were prepared by pressure impregnation method and extrusion, and the effects of Li on the microstructure and mechanical properties of beryllium–aluminum alloy were investigated by XRD, SEM and tensile test. The results show the addition of Li enhances the absorption of oxygen and nitrogen in the alloy; however, there is no significant change in the material’s density, which remains at 2.07 g/cm3. Despite an exacerbation of debonding phenomena at the fracture surface of Li-containing beryllium–aluminum alloys and a decrease in ductile dimples density, the yield strength increased from 266.2 MPa to 317.1 MPa, the tensile strength increased from 348.6 MPa to 411.4 MPa, and the elongation only decreased slightly from 2.9% to 2.5%. These experimental results support the design and preparation of high-performance beryllium–aluminum composites. Full article
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<p>Schematic diagram of the pressure infiltration technology.</p>
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<p>The microstructure of Be/Al (<b>a</b>) and Be/AlLi (<b>b</b>).</p>
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<p>Schematic diagram of the tensile sample sizes.</p>
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<p>XRD patterns of beryllium–aluminum composites. (<b>a</b>) full spectrum; (<b>b</b>) the date in the blue box.</p>
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<p>SEM and EDS analysis of Be/AlLi. (<b>a</b>) SEM; (<b>b</b>–<b>d</b>) distribution maps of elements.</p>
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<p>Tensile stress-strain curves of composites.</p>
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<p>Microstructure of composites in the transverse direction after fracture. (<b>a</b>–<b>b</b>) Be/Al; (<b>c</b>–<b>d</b>) Be/AlLi.</p>
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<p>Microstructure of composites in the transverse direction after fracture. (<b>a</b>–<b>b</b>) Be/Al; (<b>c</b>–<b>d</b>) Be/AlLi.</p>
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<p>Fracture morphology of composites. (<b>a</b>–<b>c</b>) Be/Al; (<b>d</b>–<b>f</b>) Be/AlLi.</p>
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<p>The calculation and experimental yield strength of the composites.</p>
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<p>XPS result of Be/AlLi and Al-Li binary. (<b>a</b>) Full spectrum; (<b>b</b>) high-resolution envelop of the Li 1 s peak.</p>
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<p>Typical Fracture Morphologies of (<b>a</b>) Be/Al, (<b>b</b>) Be/AlLi and (<b>c</b>) the schematic diagram.</p>
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<p>Comparison of the properties of various beryllium–aluminum composites.</p>
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15 pages, 18343 KiB  
Review
Sustainable Cooling, Layer by Layer, Shaping Magnetic Regenerators via Additive Manufacturing
by Vaibhav Sharma, Krishbold Bhandari and Radhika Barua
J. Compos. Sci. 2025, 9(3), 114; https://doi.org/10.3390/jcs9030114 - 27 Feb 2025
Viewed by 199
Abstract
Additive manufacturing (AM) is revolutionizing magnetic heat pumping technology by enabling the design and production of highly optimized, customizable components that enhance efficiency, reduce costs, and accelerate innovation in thermal management systems. This review highlights recent advances in AM for magnetocaloric materials, emphasizing [...] Read more.
Additive manufacturing (AM) is revolutionizing magnetic heat pumping technology by enabling the design and production of highly optimized, customizable components that enhance efficiency, reduce costs, and accelerate innovation in thermal management systems. This review highlights recent advances in AM for magnetocaloric materials, emphasizing its role in fabricating heat exchange structures with complex geometries and unique microstructures to enhance thermal and magnetic performance. Key AM techniques, including material extrusion, binder jetting, laser powder bed fusion, and directed energy deposition, are compared, with an in-depth discussion of critical challenges such as achieving precise material composition, controlling porosity, and maintaining phase stability. Finally, the review offers guidelines for future research to overcome these challenges. These innovations are essential for transitioning from laboratory demonstrations to real-world applications, paving the way for sustainable cooling solutions that could replace traditional gas compression systems on an industrial scale. Full article
(This article belongs to the Special Issue 3D Printing and Additive Manufacturing of Composites)
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<p>Schematic of a magnetic heat pump showing its key components. The AMR consists of a porous magnetocaloric heat exchange structure that facilitates fluid flow. The permanent magnet assembly moves in relation to the AMR bed, alternately magnetizing and demagnetizing it. As a result, the MCM experiences a temperature change. The control valves regulate the fluid flow in coordination with the magnetic fields to transfer heat from the cold to the hot heat exchanger.</p>
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<p>Schematic of material extrusion AM techniques with different precursor feeds: (<b>a</b>) fused filament fabrication (FFF) extrudes filaments made from binder and MCM powder; (<b>b</b>) fused granular fabrication (FGF) uses composite pellets of binder and MCM powder; (<b>c</b>) direct ink writing (DIW) extrudes viscous ink with a sacrificial binder and MCM powder.</p>
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<p>(<b>a</b>) A 3D-printed cylindrical sample (5 mm height, 10 mm diameter) with hexagonal channels of spatial dimension 900 µm; (<b>b</b>) 3D-printed cylindrical sample (2 mm height, 10 mm diameter) with 150 µm rectangular channels.</p>
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<p>(<b>a</b>) Magnetothermal curves of precursor LCMO powder and 3D-printed test coupon before and after sintering. (<b>b</b>) Temperature-dependent magnetic entropy change of the same test specimens. (<b>c</b>) Cross-sectional views of sintered 3D-printed LCMO scaffolds showing ~17% porosity. (<b>d</b>) The XRD pattern confirms the absence of secondary impurity phases in the sintered test coupon. Figure adapted from Ref. [<a href="#B16-jcs-09-00114" class="html-bibr">16</a>].</p>
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<p>(<b>a</b>,<b>b</b>) Magnetothermal characteristics of the precursor AlFe<sub>2</sub>B<sub>2</sub> and LaFeSiCo powders and 3D-printed test coupon before and after sintering. (<b>c</b>,<b>d</b>) Temperature-dependent magnetic entropy change of the identical test specimens. (<b>e</b>,<b>f</b>) The XRD pattern of the sintered AlFe<sub>2</sub>B<sub>2</sub> and LaFeSiCo test coupons indicates the significant presence of secondary impurity phases in the sintered test coupons, likely due to phase decomposition at high temperatures or carbon contamination during debinding.</p>
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<p>Temperature dependence of magnetic entropy change (<b>a</b>) and adiabatic temperature change curves (<b>b</b>) of compacted (La,Ce)(Fe,Mn,Si)<sub>13</sub>–H powders and 3D-printed composites (55 wt% filler loading) fabricated using FFF. Figure taken from Ref. [<a href="#B19-jcs-09-00114" class="html-bibr">19</a>]. (<b>c</b>) Evolutions of the initial Young’s modulus <span class="html-italic">E</span><sub>0</sub> and yield strength as a function of the temperature of the printed composite. Figure taken from Ref. [<a href="#B17-jcs-09-00114" class="html-bibr">17</a>].</p>
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<p>(<b>a</b>) Backscattered electron micrographs of a polished cross-section of the BJ showing significant porosity along the grain boundaries. (<b>b</b>) Magnetic field-induced ΔT<sub>ad</sub> in Ni-Mn-Cu-Ga 3D-printed test coupons, measured at magnetic field strengths of 1 T and 2 T near room temperature. (<b>c</b>) Stability of ΔT<sub>ad</sub> during thermal cycling. Figure taken from Ref. [<a href="#B25-jcs-09-00114" class="html-bibr">25</a>].</p>
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<p>(<b>a</b>) Temperature-dependent magnetization of DED-processed Ni-Mn-Sn in the as-built and heat-treated conditions. EBSD analysis of the DED-processed Ni-Mn-Sn alloys showing elongated grains along build direction. Figure taken from Ref. [<a href="#B33-jcs-09-00114" class="html-bibr">33</a>]. (<b>b</b>) Temperature-dependent magnetic entropy changes, Δ<span class="html-italic">S<sub>mag</sub></span>, measured in a 2 T applied magnetic field for suction-cast and DED-processed AlFe<sub>2</sub>B<sub>2</sub> samples (cylinders and porous blocks with honeycomb-shaped channels). Figure taken from Ref. [<a href="#B35-jcs-09-00114" class="html-bibr">35</a>].</p>
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<p>(<b>a</b>) Temperature-dependent magnetic entropy changes, Δ<span class="html-italic">S<sub>mag</sub></span>, measured in a 1 T applied magnetic field for PBF-processed LaCe(Fe,Mn,Si)<sub>13</sub> test coupons at different laser volumetric energy densities, E; (<b>b</b>) SEM micrographs showing the influence of a 3D-printed micro channeled structure and indicating presence of unmelted particles around a microchannel. Image taken from Ref. [<a href="#B42-jcs-09-00114" class="html-bibr">42</a>].</p>
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25 pages, 4688 KiB  
Article
Enhancing Mechanical and Thermal Performance of Recycled PA6/PP Blends: Chain Extension and Carbon Fiber Reinforcement Synergy
by Neslihan Ergun, Mustafa Oksuz and Aysun Ekinci
Materials 2025, 18(5), 1027; https://doi.org/10.3390/ma18051027 - 26 Feb 2025
Viewed by 187
Abstract
To develop novel materials through the recycling of waste polymers and to enhance their mechanical and thermal properties, composites were synthesized using chain extenders (CEs), compatibilizers (PP-g-MA), and short carbon fiber (CF) reinforcements within recycled polyamide 6 (rPA6) and polypropylene (rPP) blends. The [...] Read more.
To develop novel materials through the recycling of waste polymers and to enhance their mechanical and thermal properties, composites were synthesized using chain extenders (CEs), compatibilizers (PP-g-MA), and short carbon fiber (CF) reinforcements within recycled polyamide 6 (rPA6) and polypropylene (rPP) blends. The recycling of waste polymers holds paramount importance in the context of environmental sustainability. This study investigates the role of additives in effectively improving the properties of recycled polymers. The composites were fabricated using the twin-screw extrusion method and subjected to a comprehensive range of characterizations, including Fourier Transform Infrared Spectroscopy (FTIR), differential scanning calorimetry (DSC), molecular weight analysis, melt flow index (MFI), heat deflection temperature (HDT), tensile testing, impact testing, and Scanning Electron Microscopy (SEM). Additionally, ANOVA statistical methods were applied to analyze HDT, tensile, and impact test results. The findings of this research demonstrate that chain extenders and compatibilizers significantly enhance the mechanical properties of rPA6/rPP blends, while carbon fiber reinforcements markedly improve both tensile strength and impact resistance. Furthermore, the incorporation of rPP led to an approximately 4% reduction in hardness values; however, this loss was effectively compensated by the addition of chain extenders and CF reinforcements, resulting in an overall increase in hardness. It was observed that chain extenders enhanced the elastic modulus and tensile strength by reinforcing interphase bonding, whereas CF reinforcements strengthened the polymer matrix, leading to improved impact resistance. These findings emphasize the synergistic role of chain extenders, compatibilizers, and CF reinforcements in enhancing the mechanical properties of rPA6/rPP blends. The study underscores recycling as both an environmentally beneficial and effective strategy for developing durable, high-performance composites for industrial use. Consequently, the utilization of recycled polymers contributes substantially to the circular and sustainable materials economy, demonstrating the potential for the widespread industrial adoption of such composites. Full article
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<p>Chemical structures of chain extenders; (<b>a</b>) 1,4 phenylene diisocynate, (<b>b</b>) Joncryl<sup>®</sup> ADR 4368 [<a href="#B33-materials-18-01027" class="html-bibr">33</a>].</p>
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<p>Chemical structure of PP-g-MA [<a href="#B47-materials-18-01027" class="html-bibr">47</a>].</p>
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<p>The production scheme for the polymer composites.</p>
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<p>FTIR spectrum of Joncryl, rPP, PP-g-MA, and rPA6+PP-g-MA 2.5 samples.</p>
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<p>DSC analysis result thermograms of samples (<b>a</b>) rPA6, (<b>b</b>) rPA6 + PP-g-MA 2.5, (<b>c</b>) 0.2CE+rPA6 +PP-g-MA 2.5, (<b>d</b>) 0.2CE+rPA6, (<b>e</b>) 0.5CE+rPA, and (<b>f</b>) 0.75CE+rPA6.</p>
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<p>DSC analysis result thermograms of samples (<b>a</b>) rPA6, (<b>b</b>) rPA6 + PP-g-MA 2.5, (<b>c</b>) 0.2CE+rPA6 +PP-g-MA 2.5, (<b>d</b>) 0.2CE+rPA6, (<b>e</b>) 0.5CE+rPA, and (<b>f</b>) 0.75CE+rPA6.</p>
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<p>HDT values of rPA6/rPP blend-based composites.</p>
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<p>Tensile properties of rPA6/rPP blend-based composites; (<b>a</b>) Elasticity Modulus (MPa), (<b>b</b>) Tensile Strength (MPa), (<b>c</b>) Elongation at Break (%).</p>
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<p>Izod impact strength values of rPA6/rPP blend-based composites.</p>
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<p>Hardness values of rPA6/rPP blend-based composites.</p>
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<p>SEM images of Group 1, Group 2, Group 3, Group 4, Group 5, and Group 6 samples (10 kV voltage rate, ×1.00 kx magnification ratio, SE (Secondary Electron) detector, 10 mm working distance). There are differences in material morphology with different color squares.</p>
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<p>SEM images of Group 1, Group 2, Group 3, Group 4, Group 5, and Group 6 samples (10 kV voltage rate, ×1.00 kx magnification ratio, SE (Secondary Electron) detector, 10 mm working distance). There are differences in material morphology with different color squares.</p>
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15 pages, 2289 KiB  
Article
From Marble Waste to Eco-Friendly Filament for 3D Printing to Help Renaturalization of Quarries
by Daniela Fico, Daniela Rizzo, Valentina De Carolis, Francesca Lerario, Annalisa Di Roma and Carola Esposito Corcione
Sustainability 2025, 17(5), 1977; https://doi.org/10.3390/su17051977 - 25 Feb 2025
Viewed by 262
Abstract
The excessive use of materials that are generally difficult to discard, such as stone materials, has caused growing ecological concern. Among these, marble is extracted from quarries, but when the raw material is exhausted, these places are deserted. For this reason, several measures [...] Read more.
The excessive use of materials that are generally difficult to discard, such as stone materials, has caused growing ecological concern. Among these, marble is extracted from quarries, but when the raw material is exhausted, these places are deserted. For this reason, several measures have been adopted in recent years to requalify these areas. In addition, recent technological developments involve the creation of innovative green materials that privilege the circular economy and waste recycling. This research presents the development of innovative, sustainable filaments for the fused filament fabrication (FFF) printing technique from recycled marble waste (MW) and biocompostable and biodegradable polylactic acid (PLA) matrix. MW was added to the polymer in concentrations of 10 wt.%, 20 wt.%, and 30 wt.%, and the blends were extruded to develop innovative green filaments. The chemical/structural properties of the raw materials and the thermal and mechanical features of the new composites were investigated. Composites containing 10 and 20 wt.% of MW showed good printability. In contrast, extrusion and printing difficulties were observed with 30 wt.% of MW. Finally, this paper proposes a project to renaturalize and requalify a disused marble quarry located in Trani (Apulia, Italy) with 3D printing devices using the newly produced eco-filaments, which have better features. The main purpose of this article is to propose a concrete, economic, and sustainable application of 3D printing involving processes such as waste and by-product recycling and renaturalization of disused quarries, with both economic and environmental benefits. Full article
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<p>Sample measurements designed for FFF printing of prototypes for aesthetic tests.</p>
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<p>Diagram of the research phases from left to right: from the selection of raw materials (PLA and MW) to the production of green composite filaments and 3D printing of aesthetic and functional prototypes to the renaturalization of the quarry.</p>
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<p>XRD diffractogram of PLA (<b>A</b>) and MW (<b>B</b>); ATR-FTIR spectra of PLA (<b>C</b>) and MW (<b>D</b>) with indication of main peaks identified.</p>
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<p>New developed filaments for FFF and DSC thermograms of 100PLA_f, 90PLA/10MW_f, 80PLA/20MW_f, and 70PLA/30MW_f, and of the PLA pellet.</p>
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<p>CAD model of the aesthetic prototype designed with Rhinoceros software (<b>A</b>) and modified with Cura software (<b>B</b>); printing of the aesthetic prototype using the Creality CP-01 printer (<b>C</b>) and final printed aesthetic tests (<b>D</b>).</p>
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<p>Top: adaptability of the device to the side of the quarry, scale 1:50, angle 90°–30°–45° and example of arrangement in quarry with simulated route, scale 1:100; bottom: study on the adaptability of plants and prototype in the quarry.</p>
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21 pages, 3175 KiB  
Article
Bio-Hybrid Films from Chirich Tuber Starch: A Sustainable Approach with Machine Learning-Driven Optimization
by Eyyup Karaogul, Gencay Sarıışık and Ahmet Sabri Öğütlü
Sustainability 2025, 17(5), 1935; https://doi.org/10.3390/su17051935 - 24 Feb 2025
Viewed by 467
Abstract
This study investigates the potential of Chirich (Asphodelus aestivus) tuber, one of Turkey’s natural resources, for sustainable bio-hybrid film production. Bio-hybrid films developed from Chirich tuber starch in composite form with polyvinyl alcohol (PVOH) were thoroughly examined for their physical, mechanical, [...] Read more.
This study investigates the potential of Chirich (Asphodelus aestivus) tuber, one of Turkey’s natural resources, for sustainable bio-hybrid film production. Bio-hybrid films developed from Chirich tuber starch in composite form with polyvinyl alcohol (PVOH) were thoroughly examined for their physical, mechanical, and barrier properties. During the production process, twin-screw extrusion and hydraulic hot pressing methods were employed; the films’ optical, chemical, and barrier performances were analyzed through FT-IR spectroscopy, water vapor permeability, solubility, and mechanical tests. To evaluate the films’ durability against environmental factors and model their properties, advanced computational model algorithms such as Gradient Boosting Regression (GBR), Random Forest Regression (RFR), and AdaBoost Regression (ABR) were utilized. The results showed that the GBR algorithm achieved the highest accuracy with 99.92% R2 and presented the most robust model in terms of sensitivity to environmental factors. The results indicate that Chirich tuber-based bio-hybrid films exhibit significantly enhanced mechanical strength and barrier performance compared to conventional corn starch-based biodegradable polymers. These superior properties make them particularly suitable for industrial applications such as food packaging and medical materials, where durability, moisture resistance, and gas barrier characteristics are critical. Moreover, their biodegradability and potential for integration into circular economy frameworks underscore their environmental sustainability, offering a viable alternative to petroleum-derived plastics. The incorporation of ML-driven optimization not only facilitates precise property prediction but also enhances the scalability of bio-hybrid film production. By introducing an innovative, data-driven approach to sustainable material design, this study contributes to the advancement of bio-based polymers in industrial applications, supporting global efforts to mitigate plastic waste and promote environmentally responsible manufacturing practices. Full article
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<p>Flowchart of the multi-step methodology applied for the development and characterization of bio-hybrid films.</p>
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<p>Heatmap of the correlation matrix showing the relationships between the mechanical, physical, barrier, optical, and chemical properties of bio-hybrid films.</p>
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<p>Frequency distributions for the tensile strength (TS), tensile modulus (TM), density (D), water absorption (WA), water vapor permeability (WVP), and carbonyl index (CI) parameters of bio-hybrid films.</p>
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<p>Importance ranking of parameters for bio-hybrid films not exposed to environmental conditions (% Importance Distribution).</p>
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<p>Importance ranking of parameters for bio-hybrid films exposed to environmental conditions (% Importance Distribution).</p>
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<p>Prediction performance of advanced computational models for bio-hybrid films’ technical properties after exposure to environmental conditions (The red dashed line represents the ideal prediction line (y = x), where predicted values perfectly match actual values. The proximity of data points to this line indicates model accuracy, with deviations reflecting prediction errors.).</p>
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23 pages, 3575 KiB  
Article
Novel Carvacrol@activated Carbon Nanohybrid for Innovative Poly(lactide Acid)/Triethyl Citrate Based Sustainable Active Packaging Films
by Vassilios K. Karabagias, Aris E. Giannakas, Areti A. Leontiou, Andreas Karydis-Messinis, Dimitrios Moschovas, Nikolaos D. Andritsos, Apostolos Avgeropoulos, Nikolaos E. Zafeiropoulos, Charalampos Proestos and Constantinos E. Salmas
Polymers 2025, 17(5), 605; https://doi.org/10.3390/polym17050605 - 24 Feb 2025
Viewed by 557
Abstract
It has been well known for the past decade that the accumulation of food E-preservatives in the human body has harmful consequences for human health. Furthermore, scientists have realized that despite the convenience offered by petrochemical-derived polymers, a circular economy and sustainability are [...] Read more.
It has been well known for the past decade that the accumulation of food E-preservatives in the human body has harmful consequences for human health. Furthermore, scientists have realized that despite the convenience offered by petrochemical-derived polymers, a circular economy and sustainability are two current necessities; thus, the use of biodegradable alternative materials is imposed. The food packaging sector is one of the most rapidly changing sectors in the world. In recent years, many studies have focused on the development of active packaging films to replace old non-ecofriendly techniques with novel environmentally friendly methods. In this study, a novel self-healable, biodegradable active packaging film was developed using poly(lactic acid) (PLA) as a biopolymer, which was incorporated with a nanohybrid solid material as a natural preservative. This nanohybrid was derived via the absorption of carvacrol (CV) essential oil in an activated carbon (AC) nanocarrier. A material with a high carvacrol load of 71.3%wt. into AC via a vacuum-assisted adsorption method, functioning as a natural antioxidant and an antibacterial agent. The CV@AC nanohybrid was successfully dispersed in a PLA/triethyl citrate (TEC) matrix via melt extrusion, and a final PLA/TEC/xCV@AC nanocomposite film was developed. The study concluded that x = 10%wt. CV@AC was the optimum nanohybrid amount incorporated in the self-healable PLA/TEC and exhibited 277% higher ultimate strength and 72% higher water barrier compared to the pure PLA/TEC. Moreover, it remained ductile enough to show the slowest CV release rate, highest antioxidant activity, and significant antibacterial activity against Staphylococcus aureus and Salmonella enterica ssp. enterica serovar Typhimurium. This film extended the shelf life of fresh minced pork by four days, according to total viable count measurements, and decreased its lipid oxidation rate. Finally, this novel film preserved the nutritional value of porkby maintaining a higher heme iron content and showed a higher level of sensory characteristics compared to commercial packaging paper. Full article
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<p>(<b>a</b>) XRD plots of (1) AC as received, and (2) CV@AC nanohybrid, and (<b>b</b>) FTIR plots of (1) pure CV, (2) AC as received, and (3) CV@AC nanohybrid.</p>
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<p>CV desorption isotherm kinetic plots (in triplicates) for CV@AC nanohybrid (<b>a</b>) 50 °C/323 K, (<b>b</b>) 70 °C/343 K, (<b>c</b>) 90 °C/363 K, and (<b>d</b>) 11 °C/383 K. The simulation plots according to the second-order pseudokinetic model are depicted by a red line diagram.</p>
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<p>Plot of ln(1/k<sub>2</sub>) values as a function of (1/T) for the CV@AC nanohybrid.</p>
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<p>(<b>a</b>) XRD plots and (<b>b</b>) FTIR plots of (1) pure PLA/TEC, (2) PLA/TEC/5AC, (3) PLA/TEC/10AC, (4) PLA/TEC/15AC, (5) PLA/TEC/5CV@AC, (6) PLA/TEC/10CV@AC, and (7) PLA/TEC/15CV@AC films.</p>
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<p>SEM images of surface (<b>a</b>,<b>c</b>,<b>e</b>,<b>g</b>,<b>i</b>,<b>k</b>) and cross-section (<b>b</b>,<b>d</b>,<b>f</b>,<b>h</b>,<b>j</b>,<b>l</b>) nanocomposite films of PLA/TEC/5AC (<b>a</b>,<b>b</b>), PLA/TEC/5CV@AC (<b>c</b>,<b>d</b>), PLA/TEC/10AC (<b>e</b>,<b>f</b>), PLA/TEC/10CV@AC (<b>g</b>,<b>h</b>), PLA/TEC/15AC (<b>i</b>,<b>j</b>), PLA/TEC/15CV@AC (<b>k</b>,<b>l</b>).</p>
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<p>(<b>a</b>) Storage modulus plots, (<b>b</b>) Tan delta plots of all PLA/TEC/xAC and PLA/TEC/xCV@AC packaging films, as well as the pure PLA/TEC film.</p>
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<p>CV desorption isotherm kinetic plots (in triplicates) for (<b>a</b>) PLA/TEC/5CV@AC, (<b>b</b>) PLA/TEC/10CV@AC, and (<b>c</b>) PLA/TEC/15CV@AC films.</p>
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<p>Column bar diagram of calculated TVC mean values for minced pork wrapped with the commercial Ayfantis company package (Control), PLA/TEC, and PLA/TEC/10CV@AC films during the 10 days of storage at 4 ± 1 °C. Different letters in each column indicate statistically significant differences at a confidence level of <span class="html-italic">p</span> &lt; 0.05 (see also <a href="#app1-polymers-17-00605" class="html-app">Figure S7 and Table S4</a>).</p>
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<p>(<b>a</b>) TBARS mean values and (<b>b</b>) heme iron mean values for minced pork wrapped with the commercial Ayfantis package (Control), PLA/TEC, and PLA/TEC/10CV@AC films during 10 days of storage at 4 ± 1 °C. Different letters in each column indicate statistically significant differences at a confidence level of <span class="html-italic">p</span> &lt; 0.05 (see also <a href="#app1-polymers-17-00605" class="html-app">Figures S8 and S9 and Tables S5 and S6</a>).</p>
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19 pages, 5397 KiB  
Article
Novel Processes for the Production of Continuous Carbon Fiber-Reinforced Thermoplastic Polymers via Additive Manufacturing and Comparisons
by Simon Zeidler, Nikolas Matkovic, Florian Kößler, Alexander Puchta and Jürgen Fleischer
Polymers 2025, 17(5), 584; https://doi.org/10.3390/polym17050584 - 22 Feb 2025
Viewed by 348
Abstract
Continuous fiber-reinforced polymer (CoFRP) parts offer significant potential for reducing future product consumption and CO2 emissions due to their high tensile properties and low density. Additive manufacturing enables the tool-free production of complex geometries with optimal material utilization, making it a promising [...] Read more.
Continuous fiber-reinforced polymer (CoFRP) parts offer significant potential for reducing future product consumption and CO2 emissions due to their high tensile properties and low density. Additive manufacturing enables the tool-free production of complex geometries with optimal material utilization, making it a promising approach for creating load-path-optimized CoFRP parts. Recent advancements have integrated continuous fibers into laser sintering processes, allowing for the support-free production of complex parts with improved material properties. However, additive manufacturing faces challenges such as long production times, small component dimensions, and defects like high void content. New processes, including Arburg Polymer Freeforming (APF), robotic direct extrusion (DES) and the integration of thermoplastic tapes, and laser sintering, have enabled the production of CoFRPs to address these issues. A comparison of these new processes with existing material extrusion methods is necessary to determine the most suitable approach for specific tasks. The fulfillment factor is used to compare composites with different matrix and fiber materials, representing the percentage of experimentally achieved material properties relative to the theoretical maximum according to the Voigt model. The fulfillment factor varies significantly across different processes and materials. For FFF processes, the fulfillment factor ranges from 20% to 77% for stiffness and 14% to 84% for strength, with an average of 52% and 37%, respectively. APF shows a high fulfillment factor for stiffness (94%) but is lower for strength (23%), attributed to poor fiber–matrix bonding and process-induced pores. The new DES process improves the fulfillment factor due to additional consolidation steps, achieving above-average values for strength (67%). The CoFRP produced by the novel LS process also shows a high fulfillment factor for stiffness (85%) and an average fulfillment factor for strength (39%), influenced by suboptimal process parameters and defects. Full article
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<p>Different methods of co-fiber (black) integration in fused filament fabrication (polymer depicted in blue): (<b>a</b>) extrusion of pre-impregnated continuous fiber filament, (<b>b</b>) separate feeding of fiber and filament with in situ impregnation, (<b>c</b>) dual-nozzle extrusion with separate nozzles for fiber and filament [<a href="#B15-polymers-17-00584" class="html-bibr">15</a>,<a href="#B20-polymers-17-00584" class="html-bibr">20</a>].</p>
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<p>Mechanical properties of FFF-produced CoFRP [<a href="#B13-polymers-17-00584" class="html-bibr">13</a>,<a href="#B33-polymers-17-00584" class="html-bibr">33</a>,<a href="#B34-polymers-17-00584" class="html-bibr">34</a>,<a href="#B35-polymers-17-00584" class="html-bibr">35</a>,<a href="#B36-polymers-17-00584" class="html-bibr">36</a>,<a href="#B37-polymers-17-00584" class="html-bibr">37</a>,<a href="#B38-polymers-17-00584" class="html-bibr">38</a>] in [<a href="#B6-polymers-17-00584" class="html-bibr">6</a>].</p>
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<p>Fiber Integration Unit in Arburg Polymer Freeforming [<a href="#B39-polymers-17-00584" class="html-bibr">39</a>].</p>
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<p>(<b>a</b>) Hybridization process; (<b>b</b>) concept hybrid end effector for DES and consolidation; (<b>c</b>) consolidation tool [<a href="#B15-polymers-17-00584" class="html-bibr">15</a>].</p>
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<p>Overview of the robotic system for DES with continuous fiber reinforcement [<a href="#B15-polymers-17-00584" class="html-bibr">15</a>].</p>
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<p>Main effect diagrams of Consolidation I for PA6 with carbon fibers [<a href="#B15-polymers-17-00584" class="html-bibr">15</a>].</p>
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<p>Process schematic of laser sintering [<a href="#B6-polymers-17-00584" class="html-bibr">6</a>].</p>
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<p>Process schematic (<b>top</b>, [<a href="#B6-polymers-17-00584" class="html-bibr">6</a>]) and fiber integration unit (<b>bottom</b>, ©KIT, Amadeus Bramsiepe) of the developed process.</p>
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25 pages, 6107 KiB  
Article
Valorization of Biochar as a Reinforcement Agent in Polyethylene Terephthalate Glycol for Additive Manufacturing: A Comprehensive Content Optimization Course
by Nikolaos Bolanakis, Emmanuel Maravelakis, Vassilis Papadakis, Dimitrios Kalderis, Nikolaos Michailidis, Apostolos Argyros, Nikolaos Mountakis, Markos Petousis and Nectarios Vidakis
J. Manuf. Mater. Process. 2025, 9(2), 68; https://doi.org/10.3390/jmmp9020068 - 19 Feb 2025
Viewed by 329
Abstract
This study aimed to develop a biochar-modified polyethylene terephthalate glycol (PETG) composite for 3D printing. Biochar prepared from olive tree prunings was compounded with PETG at different loadings and then processed into filaments through a controlled extrusion process. The resultant filaments were used [...] Read more.
This study aimed to develop a biochar-modified polyethylene terephthalate glycol (PETG) composite for 3D printing. Biochar prepared from olive tree prunings was compounded with PETG at different loadings and then processed into filaments through a controlled extrusion process. The resultant filaments were used to print test specimens, which were characterized thoroughly by mechanical, thermal, morphological, and rheological methods. The tensile strength (17.8%), flexural strength (15.9%), impact resistance (20.9%), and thermal stability of the biochar-reinforced composites were substantially improved. Overall, the 6.0 wt.% biochar compound exhibited the highest improvement. Scanning electron microscopy and energy-dispersive X-ray spectroscopy confirmed the excellent dispersion of biochar in the PETG matrix. The results demonstrated that biochar is an effective, environmentally friendly material to use as a reinforcing agent for additive manufacturing. The PETG/biochar composites have a promising future for various industrial applications, offering sustainable alternatives with superior performance characteristics. Full article
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<p>A photographic summary of the preparation and testing procedures of PETG/biochar composites: (<b>A</b>) raw materials, (<b>B</b>) Drying process, (<b>C</b>) Filament extrusion, (<b>D</b>) Filament drying, (<b>E</b>) Filament quality control, (<b>F</b>) Filament tensile testing, (<b>G</b>) 3D printing, (<b>H</b>) Quality control of the samples, (<b>I</b>) Mechanical testing–flexural test, (<b>J</b>) Mechanical testing–impact test, (<b>Κ</b>) Rheological properties measurement, (<b>L</b>) Morphological characterization with SEM.</p>
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<p>Printing parameters and dimensions of the specimens used for mechanical testing of PETG/biochar composites. The table on the left lists the various parameters used during the 3D printing process, including biochar content, printing orientation, nozzle temperature, bed temperature, layer thickness, number of perimeters, fill density, and travel speed. The right side shows the dimensions and standards of the flexural, tensile, and Charpy notched specimens used for testing, with representative images of the printed specimens at the bottom. The lines and arrows within the geometry indicate the infill pattern used to build the geometry [<a href="#B83-jmmp-09-00068" class="html-bibr">83</a>,<a href="#B84-jmmp-09-00068" class="html-bibr">84</a>,<a href="#B85-jmmp-09-00068" class="html-bibr">85</a>].</p>
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<p>TGA and DSC of PETG/biochar composites with varying biochar content. (<b>a</b>) TGA curves showing the weight loss of pure PETG and PETG composites in different concentrations with biochar content as a function of temperature. The inset displays the residual weight percentage at 550 °C for different biochar concentrations. (<b>b</b>) DSC curves indicating the heat flow of the composites. The inset displays the glass transition temperature (T<sub>g</sub>) in relation to the biochar content.</p>
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<p>(<b>a</b>) Raman spectra from pure PETG, PETG/biochar (2, 4, 6, 8, and 10 wt.%). (<b>b</b>) Raman spectral differences of PETG/biochar (2, 4, 6, 8, and 10 wt.%) from pure PETG.</p>
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<p>Rheological behavior of PETG/biochar composites at 240 °C and 250 °C. (<b>a</b>) Viscosity (solid lines) and shear stress (dotted lines) as functions of shear rate for pure PETG and PETG composites with 2.0%, 4.0%, 6.0%, 8.0%, and 10.0% biochar content (per weight) at 240 °C. (<b>b</b>) Melt flow rate (MFR) of the composites as a function of biochar content at 250 °C, showing the maximum MFR and its decline with increasing biochar percentage.</p>
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<p>(<b>a</b>,<b>c</b>) display the visual comparison of the filament surface for pure PETG and PETG with 4.0 wt.% biochar, respectively, with consistent diameters indicating stable extrusion over time. (<b>b</b>,<b>d</b>) present the mechanical properties of the PETG/biochar composites.</p>
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<p>Comparison of mechanical properties for PETG pure and PETG/biochar composites. (<b>a</b>) Stress vs. strain graphs. (<b>b</b>) Average tensile strength and deviation, and (<b>c</b>) average Young’s modulus and deviation.</p>
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<p>Flexural performance of PETG/biochar composites. (<b>a</b>) Stress–strain curves for pure PETG and PETG composites with varying biochar content. (<b>b</b>) Flexural strength (average values and deviation) (σ) of PETG composites with different biochar percentages, showing a maximum increase of 15.9% at 6.0% biochar content. (<b>c</b>) Flexural modulus (average values and deviation) (E) of the composites, with a maximum increase of 10.5% observed at 6.0% biochar content.</p>
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<p>Evaluation of tensile toughness, impact resistance and hardness of PETG/biochar composites (average values and deviation). (<b>a</b>) Toughness (T) of PETG composites with varying biochar content. (<b>b</b>) Impact strength of the composites in the Charpy test. (<b>c</b>) Vickers microhardness (M-H) of the composites.</p>
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<p>SEM and EDS analysis of biochar particles. SEM image at magnification (<b>a</b>) 1000× and (<b>b</b>) 5000×; (<b>c</b>) high-magnification SEM image at 30,000×, highlighting fine details of the particles. (<b>d</b>) Elemental mapping of the biochar indicating the distribution of key elements (carbon). (<b>e</b>) EDS spectrum and corresponding table showing the elemental composition of the biochar, with a focus on oxygen (O), carbon (C), calcium (Ca), and potassium (K).</p>
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<p>SEM images of PETG/biochar composites at different magnifications. (<b>a</b>,<b>d</b>,<b>g</b>) 4.0 wt.%, (<b>b</b>,<b>e</b>,<b>h</b>) 8.0%, and (<b>c</b>,<b>f</b>,<b>i</b>) 10.0%. (<b>a</b>–<b>c</b>) show vertical surface views at 150× magnification; (<b>d</b>–<b>f</b>) show cross-sectional views at 27× magnification; and (<b>g</b>–<b>i</b>) show detailed views of the fracture surfaces at 3000× magnification.</p>
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<p>SEM images of the PETG/biochar 6 wt.% composites at different magnifications (<b>a</b>) lateral surface at 27× magnification, and fracture surface at magnifications of (<b>b</b>) 300×, (<b>c</b>) 1000×, (<b>d</b>) 27×, (<b>e</b>) 3000× and (<b>f</b>) 20,000×.</p>
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<p>Radar charts summarizing the mechanical performance of PETG/biochar composites. (<b>a</b>) Tensile strength (<math display="inline"><semantics> <mrow> <msubsup> <mi>σ</mi> <mi>Β</mi> <mi>Τ</mi> </msubsup> </mrow> </semantics></math>) in MPa; (<b>b</b>) Tensile modulus (E<sup>T</sup>) in MPa; (<b>c</b>) Flexural strength (<math display="inline"><semantics> <mrow> <msubsup> <mi>σ</mi> <mi>Β</mi> <mi>F</mi> </msubsup> </mrow> </semantics></math>) in MPa; and (<b>d</b>) Flexural modulus (E<sup>F</sup>) in GPa for pure PETG and composites with 2.0%, 4.0%, 6.0%, 8.0%, and 10.0% biochar content.</p>
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31 pages, 1754 KiB  
Review
Advancing Sustainability in Modern Polymer Processing: Strategies for Waste Resource Recovery and Circular Economy Integration
by Ionut-Cristian Radu, Andreea-Mihaela Vadureanu, Derniza-Elena Cozorici, Erika Blanzeanu and Catalin Zaharia
Polymers 2025, 17(4), 522; https://doi.org/10.3390/polym17040522 - 17 Feb 2025
Viewed by 459
Abstract
By the late 1970s, plastics had emerged as the most widely used materials globally. The discovery, development, and processing of diverse polymeric materials have profoundly shaped modern life and driven the expansion of numerous industries. Given the widespread interest in the utilization of [...] Read more.
By the late 1970s, plastics had emerged as the most widely used materials globally. The discovery, development, and processing of diverse polymeric materials have profoundly shaped modern life and driven the expansion of numerous industries. Given the widespread interest in the utilization of these materials, it has become increasingly imperative to design their life cycles from the outset. This approach aims to maximize their utility while minimizing their environmental footprint. This review aims to identify and analyze the key challenges in polymer processing applicable to both additive and formative manufacturing methods, emphasizing the relationship between processing and recycling within the framework of sustainability. Modern polymer processing techniques play a crucial role in enhancing the sustainability of polymer products by improving recycling potential (with consideration of polymer type, source, and additives), cost-effectiveness, carbon footprint, and key properties such as durability, lifespan, performance, and environmental impact. It will also explore the concept of the circular economy and its integration into modern processing methods, including extrusion, injection molding, and 3D printing. Additionally, current polymer recycling methods are analyzed with respect to their effectiveness, sustainability, and compatibility with the original materials. Moreover, the discussion emphasizes the benefits of a circular economy compared to a linear one by exploring the concepts of closed-loop and open-loop systems, along with their diverse applications depending on the material and the initial processing method employed. To ensure that humanity continues to benefit from polymer materials while striving for a waste-free environment, it is essential to integrate the principles of sustainable development from the very beginning. Full article
(This article belongs to the Section Circular and Green Polymer Science)
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<p>A holistic approach illustrating the relationship between modern polymer processing techniques, recycling strategies, and circular economy integration to advance sustainability.</p>
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<p>Schematic of an injection molding system with sustainability-focused enhancements.</p>
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<p>Sustainability in extrusion: optimization and circularity.</p>
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<p>Strategic approaches to enhancing sustainability through various 3D-printing techniques.</p>
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17 pages, 2367 KiB  
Article
Effect of Filament Material and Printing Temperature on 3D Printing Extrusion Force
by Daša Krapež, Muhammed Jusufagić, Murčo Obućina, Manja Kitek Kuzman and Mirko Kariž
Appl. Sci. 2025, 15(4), 2046; https://doi.org/10.3390/app15042046 - 15 Feb 2025
Viewed by 443
Abstract
In this study, a modified 3D printer hotend equipped with a load cell, attached to the feeding system, was used to evaluate the effects of filament material composition and printing parameters on the extrusion force required. Four different materials (commercial PLA, pure PLA, [...] Read more.
In this study, a modified 3D printer hotend equipped with a load cell, attached to the feeding system, was used to evaluate the effects of filament material composition and printing parameters on the extrusion force required. Four different materials (commercial PLA, pure PLA, wood-PLA with different ratios of wood particles, and wood-PLA with different ratios of thermally modified wood particles) were used for 3D printing, and the feeding resistance was measured. The filament feeder was connected to the extruder hotend via a load cell, which measured the forces required to push the filament through the extruder and the nozzle. Three printing nozzle temperatures of 200, 210, and 220 °C were used. The results show that the printing temperature and the material influence the required extrusion forces, which varied between 1 and 8 N, but the variation was high. With proper optimization and integration into the printer firmware, this setup could also be used to detect nozzle clogging during printing, modify printing parameters during the process, and prevent the uneven extrusion of composite filaments. Full article
(This article belongs to the Special Issue Recent Advances in 3D Printing and Additive Manufacturing Technology)
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<p>(<b>a</b>) Extrusion force measuring setup on modified extruder head on 3D printer—schematic, (<b>b</b>) working setup right.</p>
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<p>Typical measurement of extrusion forces for PLA filament (T = 200 °C, printing speed 20 mm/s).</p>
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<p>Force measurements—example of PLA-beech with 20% wood, 200 °C.</p>
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<p>(<b>a</b>) Force measurements—small peaks in each printing layer—B20, T200 s20, (<b>b</b>) schematic of printing layers in slicer software right-red and green lines present outer walls printing lines, yellow are infill printing lines.</p>
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<p>Average extrusion forces for different materials and three printing temperatures: 200, 210, and 220 °C.</p>
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<p>Comparison of average extrusion forces for wood-PLA filaments with different wood ratios during printing at 200 °C.</p>
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<p>Comparison of average complex viscosity for different materials at oscillation frequency of 100 rad/s and 200 °C, measured with parallel plate rheometer and average extrusion force at 200 °C.</p>
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<p>Extrusion force—first layer vs. rest of the layers (ratio) for different materials and printing temperatures.</p>
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<p>Extrusion force—printing on previous layer vs. printing in air (ratio between forces) for different materials and printing temperatures.</p>
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14 pages, 2831 KiB  
Article
Upscaled Multilayer Dispersion Coating Application for Barrier Packaging: PLAX and bioORMOCER®
by Eetu Nissinen, Adina Anghelescu-Hakala, Roosa Hämäläinen, Pauliina Kivinen, Ferdinand Somorowsky, Jani Avellan and Rajesh Koppolu
Coatings 2025, 15(2), 214; https://doi.org/10.3390/coatings15020214 - 11 Feb 2025
Viewed by 571
Abstract
The shift from fossil-based packaging materials to more sustainable alternatives is driven by evolving environmental regulations aiming for enhanced recyclability and biodegradability. Dispersion coatings, as opposed to extrusion-based approaches, offer significant advantages by reducing the coat weights, but generally, multiple coating layers are [...] Read more.
The shift from fossil-based packaging materials to more sustainable alternatives is driven by evolving environmental regulations aiming for enhanced recyclability and biodegradability. Dispersion coatings, as opposed to extrusion-based approaches, offer significant advantages by reducing the coat weights, but generally, multiple coating layers are needed to meet functional performance requirements. This study explores the application of upscaled multilayer dispersion coatings comprising polylactic acid-based coating (PLAX) and hybrid nanomaterial lacquer (bioORMOCER®) on commercial base papers for barrier packaging using semi-pilot reverse gravure and industrial-scale rod coaters. One multilayer structure demonstrated a low water vapour transmission rate (WVTR), achieving a WVTR of 12 g/(m2·day) under standard conditions and a 78% reduction of WVTR compared to the substrate under elevated humidity. The other multilayer structure exhibited an excellent oxygen transmission rate (OTR) of 2.3 cc/(m2·day·bar) at dry conditions, which is comparable to conventional high-performance alternatives. Both multilayer coatings enhanced the grease and mineral oil barriers significantly, as heptane vapour transmission rate (HVTR) reductions exceeded 97%. The multilayer coatings demonstrated strong potential for scalable production of sustainable, high-barrier packaging materials. These findings highlight the capability of dispersion coatings to replace traditional fossil-based barriers, advancing the development of environmentally friendly packaging solutions. Full article
(This article belongs to the Special Issue Sustainable Coatings for Functional Textile and Packaging Materials)
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<p>Images from the coating process. (<b>a</b>) bioORMOCER<sup>®</sup> is poured into the coating station. (<b>b</b>) PLA-X dispersion at the coating station. (<b>c</b>) Visual appearance of A-PO. (<b>d</b>) SutCo-line during the coating run of S-POP.</p>
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<p>Coat weights and thicknesses of coating layers of A-POP and S-POP.</p>
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<p>SEM cross-cut images of the samples (<b>a</b>) A-POP and (<b>b</b>) S-PO with 5000x magnification.</p>
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<p>Barrier performance of coated samples. (<b>a</b>) Comparison of water vapour transmission rates (WVTR) of coated samples related to base papers at 23 °C and 50% RH and (<b>b</b>) at 23 °C and 80% RH. (<b>c</b>) Oxygen transmission rates (OTR) of the samples S-POP and A-POP at 23 °C and 0/50% RH. (<b>d</b>) Heptane vapour transmission rates (HVTR) of the samples S-POP and A-POP and base papers at 23 °C and 50% RH.</p>
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28 pages, 26850 KiB  
Article
Deep Learning Utilization for In-Line Monitoring of an Additive Co-Extrusion Process Based on Evaluation of Laser Profiler Data
by Valentin Lang, Christian Thomas Ernst Herrmann, Mirco Fuchs and Steffen Ihlenfeldt
Appl. Sci. 2025, 15(4), 1727; https://doi.org/10.3390/app15041727 - 8 Feb 2025
Viewed by 451
Abstract
Additive manufacturing is gaining importance in a number of application areas, and there is an increased demand for mechanically resilient components. A way to improve the mechanical properties of parts made of thermoplastics is by using reinforcing material. The study demonstrates the development [...] Read more.
Additive manufacturing is gaining importance in a number of application areas, and there is an increased demand for mechanically resilient components. A way to improve the mechanical properties of parts made of thermoplastics is by using reinforcing material. The study demonstrates the development of a monitoring procedure for a fused filament fabrication-based co-extrusion process for manufacturing wire-reinforced thermoplastic components. Test components in two variants are produced, and data acquisition is carried out with a laser line scanner. The collected data are employed to train deep neural networks to classify the printed layers, aiming for the deep neural networks to be able to classify four different classes and identify layers with insufficient quality. A dedicated convolutional neural network is designed taking into account various factors such as layer architecture, data pre-processing and optimization methods. Several network architectures, including transfer learning (based on VGG16 and ResNet50), with and without fine-tuning, are compared in terms of their performance based on the F1 score. Both the transfer learning model with ResNet50 and the fine-tuning model achieve an F1 score of 84% and 83%, respectively, for the decisive class ‘wire bad’ classifying inadequate reinforcement. Full article
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<p>Setup of the experimental equipment consisting of a 3-axis machine platform with a co-extrusion head for wire-reinforced thermoplastics strand deposition.</p>
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<p>Flowchart of an in situ monitoring routine based on classification of height information of printed layers using convolutional neural networks.</p>
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<p>Display of all part configurations of the components in the four distinguished classes ‘solid’, ‘infill’, ‘wire good’ and ‘wire bad’ (visualization based on scanned, unprocessed data).</p>
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<p>(<b>a</b>) Raw data file: all height measurement values recorded with laser line scanner in a CSV. (<b>b</b>) Area of interest: area specified via the interface. (<b>c</b>) Pre-processed data: output file before splitting into patches. (<b>d</b>) Processed output: split patches (numbers 1–9) in format 224 × 224 pixels appropriate for model learning.</p>
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<p>(<b>a</b>) Serial color coding of the normalized CSV data using the height information. (<b>b</b>) Coding of the height information in two channels parallel to each other. (<b>c</b>) Example image output dataset, (<b>d</b>) Example image serial coding. (<b>e</b>) Example image parallel coding.</p>
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<p>Top-layer architecture of the employed transfer learning models.</p>
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<p>Training progress for learning rates <math display="inline"><semantics> <mrow> <mn>1</mn> <mo>×</mo> <msup> <mn>10</mn> <mrow> <mo>−</mo> <mn>4</mn> </mrow> </msup> </mrow> </semantics></math>, <math display="inline"><semantics> <mrow> <mn>1</mn> <mo>×</mo> <msup> <mn>10</mn> <mrow> <mo>−</mo> <mn>5</mn> </mrow> </msup> </mrow> </semantics></math>, and <math display="inline"><semantics> <mrow> <mn>1</mn> <mo>×</mo> <msup> <mn>10</mn> <mrow> <mo>−</mo> <mn>6</mn> </mrow> </msup> </mrow> </semantics></math> for the ResNet50 model with (<b>a</b>) dataset 1 (seed 456) and (<b>b</b>) with dataset 2 (seed 456).</p>
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<p>(<b>a</b>) Validation accuracy and (<b>b</b>) validation loss as metrics for the training progress of the fine-tuning models.</p>
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<p>Confusion matrix of the FT3 model for seed 42.</p>
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<p>Misclassifications regarding the corresponding images from the dataset illustrating deficiencies in effectiveness of proposed method: (<b>a</b>) true: infill, prediction: wire bad, (<b>b</b>) true: wire bad, prediction: infill, (<b>c</b>) true: wire good, prediction: infill, (<b>d</b>) true: wire good, prediction: infill, (<b>e</b>) true: infill, prediction: wire good, (<b>f</b>) true: wire good, prediction: infill, (<b>g</b>) true: infill, prediction: wire good, and (<b>h</b>) true: wire bad, prediction: infill.</p>
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18 pages, 5693 KiB  
Article
Mechanical Characterization and Modeling of Glass Fiber-Reinforced Polyamide Built by Additive Manufacturing
by Massimiliano Avalle and Mattia Frascio
Materials 2025, 18(4), 745; https://doi.org/10.3390/ma18040745 - 8 Feb 2025
Viewed by 430
Abstract
Additive manufacturing (AM) is an emerging technology with the greatest potential impact on many engineering applications. Among the AM technologies, material extrusion is particularly interesting for plastic components due to its versatility and cost-effectiveness. There is, however, a limited knowledge of design methods [...] Read more.
Additive manufacturing (AM) is an emerging technology with the greatest potential impact on many engineering applications. Among the AM technologies, material extrusion is particularly interesting for plastic components due to its versatility and cost-effectiveness. There is, however, a limited knowledge of design methods to predict the mechanical strength of parts built by material extrusion. The materials are polymers, sometimes also reinforced, and deposited in layers like in laminated composites. Therefore, the mechanical behavior and strength can be characterized and modeled with methods already known for composite materials. Such tools are the classical lamination theory (CLT) and the failure criteria for composites. This paper addresses an analysis of a composite material made of long-fiber glass in a polyamide matrix built by additive manufacturing; in this relatively new technique, a continuous fiber is inserted between layers of polyamide deposited from a wire with a fused filament fabrication (FFF) 3D printer. The mechanical behavior was studied from tensile tests that were carried out to demonstrate the feasibility of modeling with the mentioned tools, and the material properties for predicting the stiffness and strength of components built with that technique were identified. The results show that the classical models for the mechanical behavior of composite materials are well-suited for this material to predict the influence of the main building parameters. Full article
(This article belongs to the Section Mechanics of Materials)
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<p>Specimen generation and 3D printing process.</p>
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<p>Geometry and layering scheme of the used specimen: (<b>a</b>) plane top section of the specimen, thickness 3.2 mm; (<b>b</b>) sample with fibers aligned at 0° orientation, image from Eiger™ slicing software; (<b>c</b>) fibers at ±23°; (<b>d</b>) fibers at ±45°; (<b>e</b>) fibers at ±67°; (<b>f</b>) fibers at 90°.</p>
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<p>Example of some samples with the laminations described in <a href="#materials-18-00745-t002" class="html-table">Table 2</a>, shown next to a Vernier caliper for comparison.</p>
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<p>Typical stress–strain results from the tensile tests on the layered samples reinforced with glass fibers: (<b>a</b>) unidirectional 0°; (<b>b</b>) angle-ply ±23°; (<b>c</b>) angle-ply ±45°; (<b>d</b>) angle-ply ±67°; (<b>e</b>) unidirectional 0°; (<b>f</b>) comparison of the tested laminations.</p>
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<p>Samples reinforced with glass fibers after tensile tests: (<b>a</b>) unidirectional 0°; (<b>b</b>) angle-ply ±23°; (<b>c</b>) angle-ply ±45°; (<b>d</b>) angle-ply ±67°; (<b>e</b>) unidirectional 90°.</p>
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<p>Experimental results of the tests on Onyx/GF samples in tension: analysis of the elastic properties.</p>
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<p>Experimental results of the tests on Onyx/GF samples in tension. Analysis of the strength and criteria: (<b>a</b>) Tsai–Wu model; (<b>b</b>) Christensen model; (<b>c</b>) LaRC05 model; (<b>d</b>) Hashin model.</p>
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