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Materials Science in Additive Manufacturing                          Natural composite filaments for 3D-Print



            another study, the crystallization behavior was further   polymeric wastes were developed by considering cocoa
            investigated to probe into the effect of the addition of   bean  shells  and  recycled  polypropylene,  respectively.
            plasticizer, namely polyethylene glycol (PEG), on the   The combination of these two materials in the filament
            mechanical and physical properties of filament materials   production was found to result in a reduced shrinkage
            produced  through the fused filament  fabrication (FFF)   and warping behavior, thereby further enhancing the
            technique.  The addition of PEG plasticizer was found   dimensional stability of the sample during the 3D printing
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            to result in 3D-printed parts with crystallinity values   process. 68
            of  up to 18%  greater  as  compared to neat  PLA,  which   Moreover, the development of biodegradable composites
            also translated into improved mechanical and physical   through 3D printing technology from the derivatives of
            characteristics.  The inferior mechanical properties   natural fibers, namely cellulose, hemicellulose, and lignin,
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            observed in neat poly(3-hydroxybutyrate) and PLA (PHB/  has also been realized in the recent past.  For instance, the
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            PLA) blends were found to be significantly improved   optimum amounts of other naturally derived components,
            upon the addition of plasticized blends based on esters of   namely hemicellulose and lignin, which could be added in
            citric acid.  Moreover, the inclusion of such plasticizers   the preparation of composite filament for 3D printing, were
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            in the filament material blend led to a notable increase   found to be 25% and 5%, respectively. 69,85  In other studies,
            in the softening effect in the filament structure, thereby   cellulose-based composite filament wire was successfully
            resulting in a significant increase in their elongation at   prepared by combining cellulose nanofiber (CNF) and
            break. 64                                          PLA.  In contrast to pure PLA filament wires, the inclusion
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            4. Fibers and matrix selection for                 of cellulose reinforcement in the PLA-composite filament
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            biodegradable NFRCFs                               wires was found to yield an increase in its tensile strength.
                                                               Besides improvement in their mechanical properties,
            In previous studies, diverse types of natural fibers have been   CNF-based biocomposite filament was also found to have
            considered in the production of natural fiber-reinforced   enhanced thermal stability. 67
            composite filaments.  Examples of such natural fibers
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            consisted of rice straw, bamboo, hemp, sugarcane, and flax   4.1. Challenges of using natural fibers in NFRCFs for
            fibers. 63,73,78-80  The fiber content by weight in the NFRCFs   fused deposition modeling
            was found to range between 15% and 30%. 63,73,78-80  Table 3   The challenges associated with the consideration of natural
            summarizes the specification, composition, characteristics,   fibers in the fabrication of biodegradable composite
            and applications of commonly used composite-based non-  filaments and their utilization are further discussed in this
            biodegradable filament materials  for 3D  printing. Even   section. One of the main concerns observed when dealing
            though  the  filament  material  developed  in  these  studies   with natural fiber-based filament material during the
            displayed satisfactory mechanical performance, they   AM process is the lack of homogeneity in the deposited
            were not fully biodegradable as a result of their polymeric   layers. 73,86  The lack of homogeneity was found to arise due
            matrix, which lacked the degradability trait. ABS is one   to the combined effects of several factors originating from
            such  example that has  poor  degradable  characteristics   the printer hardware, printing parameters, and material
            but nonetheless displays high tensile strength while being   composition as outlined in Figure 7. For instance, it is to
            resistant to physical impacts. 49,81               be noted that the homogeneity of 3D-printed structures
              Besides the use of natural fibers, many studies have   is normally affected by the print direction, which has a
            considered fibers in powdered form as an alternative   significant impact on their load-bearing capacity, thereby
                                                                                            21,87,88
            reinforcement component for filament fabrication. One   resulting in an orthotropic behavior.
            example  is bamboo-plastic  composite wires,  which  were   In terms of material composition, the inhomogeneous
            developed through the  FDM  technique  by  considering   mix of natural fiber composite for filament material can
            printed wires made of bamboo flour, PLA matrix, and   lead to a lack of homogeneity in the final product. As
            plasticizers.  Another powder-based material, namely   reported in previous studies, it is unfeasible to achieve
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            wood flour, was considered to produce wood flour-PLA   a near-perfect homogeneous mixture of natural fiber
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            filament  at  a  composition  ratio  of  1:2.3.   Before  the   composite  for  filament  material  in  line  with  existing
            filament fabrication, sieved wood flour from 140-mesh   technologies. It is thus common to have an agglomeration
            to 160-mesh size was mixed with PLA and distilled water,   of the reinforcement components or particles in the
            while experimental reagents, namely glycerol and TBC,   composite mix, thereby further contributing to the
            were considered and added as plasticizer.  In another study,   inhomogeneous and anisotropic nature of the 3D-printed
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            3D printing composite filaments from agro-industrial and   parts.  Other issues that could potentially arise during the
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            Volume 4 Issue 1 (2025)                         8                              doi: 10.36922/msam.8533
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