AccScience Publishing / MSAM / Online First / DOI: 10.36922/MSAM026310075
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ORIGINAL RESEARCH ARTICLE

Comparative study of process structure property relationships and melt flow behavior of CNT GO-reinforced PLA nanocomposites fabricated via fused granular fabrication and material extrusion

Isam Ridha Kazem Alhailo1† Mehran Mahboubkhah1†* Reza Najjar2
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1 Department of Mechanical Engineering, University of Tabriz, Tabriz , Iran
2 Chemistry Department, University of Tabriz, Tabriz , Iran
†These authors contributed equally to this work.
Received: 1 August 2026 | Revised: 20 August 2026 | Accepted: 25 August 2026 | Published online: 9 September 2026
© 2026 by the Author(s). This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution 4.0 International License ( https://creativecommons.org/licenses/by/4.0/ )
Abstract

This study offers a systematic process structure property comparison of polylactic acid (PLA) nanocomposites reinforced with hybrid carbon nanotubes (CNT) and graphene oxide (GO), fabricated via pellet-fed fused granular fabrication (FGF) and conventional filament-based material extrusion (MEX). Nanocomposites were prepared via a dissolution assisted route to ensure homogeneous filler dispersion while mitigating thermal degradation. To bridge formulation and extrudability, the melt flow index (MFI) was introduced as a critical processability metric alongside standardized thermal (TGA/DSC) and mechanical (tensile/flexural) characterization. Hybrid reinforcement, through complementary CNT and GO mechanisms, significantly enhanced thermal stability, elevating the onset degradation temperature from 305.0 °C to 319.8 °C, and promoted crystallization, increasing the degree of crystallinity from ∼7.5% to 21.5%. Tensile strength improved by 8–22% and elongation at break by up to 82% , despite a moderate reduction in elastic modulus (7–29%) . Flexural modulus increased by up to 41% (MEX) and 28% (FGF), while FGF specimens exhibited markedly higher bending compliance and deformation capability, correlating with slightly higher interlayer porosity from FESEM. MFI decreased with nanofiller addition, with the MWCNT-rich formulation showing the largest viscosity increase, while FGF feedstocks exhibited higher MFI than MEX filaments due to reduced thermomechanical history. FGF achieved thermal, rheological, and mechanical performance comparable to MEX, with microstructural differences providing a beneficial stiffness-ductility trade-off. This work provides the first comparative dataset incorporating MFI for identical hybrid formulations across both processing routes, establishing pellet-fed FGF as a scalable, cost-effective, and environmentally friendlier alternative to filament-based MEX for high-performance additive manufacturing.

Keywords
Polylactic acid
Carbon nanotubes
Graphene oxide
Fused granular fabrication
Material extrusion
Melt flow index
Additive manufacturing
Nanocomposites
Funding
No funding was received for conducting this research, analysis, or preparation of this manuscript.
Conflict of interest
The authors declare they have no competing interests.
References
  1. Dananjaya SAV, Chevali VS, Dear JP, Potluri P, Abeykoon C. 3D printing of biodegradable polymers and their composites – Current state-of-the-art, properties, applications, and machine learning for potential future applications. Prog Mater Sci. 2024;146:101336. doi: 10.1016/j.pmatsci.2024.101336
  2. Patel R, Desai C, Kushwah S, Mangrola MH. A review article on FDM process parameters in 3D printing for composite materials. Mater Today Proc. 2022;60:2162-2166. doi: 10.1016/j.matpr.2022.02.385
  3. Suvanjumrat C, Chansoda K, Chookaew W. Additive manufacturing advancement through large-scale screw-extrusion 3D printing for precision parawood powder/PLA furniture production. Clean Eng Technol. 2024;20:100753. doi: 10.1016/j.clet.2024.100753
  4. Liu H, Gong K, Portela A, Cao Z, Dunbar R, Chen Y. Granule-based material extrusion is comparable to filament-based material extrusion in terms of mechanical performances of printed PLA parts: A comprehensive investigation. Addit Manuf. 2023;75:103744. doi: 10.1016/j.addma.2023.103744
  5. Guo H, Lv R, Bai S. Recent advances on 3D printing graphene-based composites. Nano Mater Sci. 2019;1(2):101-115. doi: 10.1016/j.nanoms.2019.03.003
  6. Fenta EW, Mebratie BA. Advancements in carbon nanotube-polymer composites: Enhancing properties and applications through advanced manufacturing techniques. Heliyon. 2024;10(16):e36490. doi: 10.1016/j.heliyon.2024.e36490
  7. Agarwala S, Goh GL, Goh GD, Dikshit V, Yeong WY. 3D and 4D printing of polymer/CNTs-based conductive composites. In: 3D and 4D Printing of Polymer Nanocomposite Materials: Processes, Applications, and Challenges. Amsterdam, Netherlands: Elsevier; 2019:297-324. doi: 10.1016/B978-0-12-816805-9.00010-7
  8. Batakliev T, Georgiev V, Ivanov E, et al. Nanoindentation analysis of 3D printed poly(lactic acid)-based composites reinforced with graphene and multiwall carbon nanotubes. J Appl Polym Sci. 2019;136(13):47260. doi: 10.1002/app.47260
  9. De Bortoli LS, de Farias R, Mezalira DZ, Schabbach LM, Fredel MC. Functionalized carbon nanotubes for 3D-printed PLA-nanocomposites: Effects on thermal and mechanical properties. Mater Today Commun. 2022;31:103402. doi: 10.1016/j.mtcomm.2022.103402
  10. Ivanova R, Kotsilkova R, Ivanov E, et al. Composition dependence in surface properties of poly(lactic acid)/graphene/carbon nanotube composites. Mater Chem Phys. 2020;249:122702. doi: 10.1016/j.matchemphys.2020.122702
  11. Mohammed YS. Investigating the effect of build direction on mechanical properties in pellet based 3D printing. Master's thesis. Rochester, NY: Rochester Institute of Technology; 2025. Axxessed September 2, 2026. https://repository.rit.edu/theses/12430
  12. Yu WW, Zhang J, Wu JR, Wang XZ, Deng YH. Incorporation of graphitic nano-filler and poly(lactic acid) in fused deposition modeling. J Appl Polym Sci. 2017;134(15):44703. doi: 10.1002/app.44703
  13. Arora N, Dua S, Singh VK, Singh SK, Senthilkumar T. A comprehensive review on fillers and mechanical properties of 3D printed polymer composites. Mater Today Commun. 2024;40:109617. doi: 10.1016/j.mtcomm.2024.109617
  14. Hanon MM, Dobos J, Zsidai L. The influence of 3D printing process parameters on the mechanical performance of PLA polymer and its correlation with hardness. Procedia Manuf. 2021;54:244-249. doi: 10.1016/j.promfg.2021.07.038
  15. Kiendl J, Gao C. Controlling toughness and strength of FDM 3D-printed PLA components through the raster layup. Compos Part B Eng. 2020;180:107562. doi: 10.1016/j.compositesb.2019.107562
  16. Mohammadi Zerankeshi M, Sayedain SS, Tavangarifard M, Alizadeh R. Developing a novel technique for the fabrication of PLA-graphite composite filaments using FDM 3D printing process. Ceram Int. 2022;48(21):31850-31858. doi: 10.1016/j.ceramint.2022.07.117
  17. Saleh M, Anwar S, AlFaify AY, Al-Ahmari AM, Abd Elgawad AEE. Development of PLA/recycled-desized carbon fiber composites for 3D printing: Thermal, mechanical, and morphological analyses. J Mater Res Technol. 2024;29:2768-2780. doi: 10.1016/j.jmrt.2024.01.267
  18. Patel KS, Shah DB, Joshi SJ, Patel KM. Developments in 3D printing of carbon fiber reinforced polymer containing recycled plastic waste: A review. Clean Mater. 2023;9:100207. doi: 10.1016/j.clema.2023.100207
  19. Gonzalez-Calderon JA, Castrejon-Gonzalez EO, Medellin-Rodriguez FJ, Stribeck N, Almendarez-Camarillo A. Functionalization of multi-walled carbon nanotubes (MWCNTs) with pimelic acid molecules: effect of linkage on β-crystal formation in an isotactic polypropylene (iPP) matrix. J Mater Sci. 2015;50(3):1457-1468. doi: 10.1007/s10853-014-8706-1
  20. Pandey A, Singh J, Singh M, Singh G, Parmar AS, Chaudhary S. Graphene oxide/polylactic acid composites with enhanced electrical and mechanical properties for 3D-printing materials. J Mol Struct. 2025;1329:141420. doi: 10.1016/j.molstruc.2025.141420
  21. Henrichs NN, Sehrt JT, Brinkmann T, Bürgel LPM, Berger DM. Influence of flowability on the processability of thermoplastics in additive manufacturing: Comparison of fused layer modeling (FLM) and fused granulate fabrication (FGF). J Appl Polym Sci. 2026;143(35):e71048. doi: 10.1002/app.71048
  22. Wu MYT, Mak SL, Tang WF, Li CH, Chan TW. A Review on Melt Flow Index Characteristics of Polylactide (PLA) for Recycle Use in 3-D Printing. J Test Eval. 2022;50(4):2260-2267. doi: 10.1520/JTE20210314
  23. Singh S, Attri RK, Trivedi S. Optimization of nano-graphene loading in PLA-graphene composites for fused deposition modeling based application. J Mech Sci Technol. 2024;38(6):2901-2908. doi: 10.1007/s12206-024-0510-5
  24. Vidakis N, Petousis M, Maniadi A, Koudoumas E, Vairis A, Kechagias J. Sustainable additive manufacturing: Mechanical response of acrylonitrile-butadiene-styrene over multiple recycling processes. Sustainability. 2020;12(9):3568. doi: 10.3390/su12093568
  25. Hulea R, Stefan R, Kiss IA, Ariesan RA. Combined influence of 3D printing parameters and thermal conditioning on the tensile strength of FGF-Printed PLA components. J Polym Res. 2025;32(11):387. doi: 10.1007/s10965-025-04620-9
  26. Ancio F, Tavara L, Ferreira LM. Process-Induced Anisotropy and Fracture Behavior of Pellet-3D Printed PLA and PLA/Flax Biocomposites. Polym Compos. 2026. doi: 10.1002/pc.71361
  27. Feng P, Yang F, Shi X, Peng S, Pan H, Shuai C. Carbon nanotubes perpendicularly grown on graphene oxide nanosheets derived from metal-organic frameworks: Synergistic reinforcement of poly(l-lactic acid) scaffold. J Mater Res Technol. 2024;33:892-905. doi: 10.1016/j.jmrt.2024.09.137
  28. Angili SN, Morovvati MR, Vatandoust Y, Fotouhi M, Bodaghi M. Investigating mechanical enhancement and vibrational response of additive manufactured PLA scaffolds with carbon nanotube and graphene oxide: Fabrication and multi-scale simulation. Compos Struct. 2025;369:119320. doi: 10.1016/j.compstruct.2025.119320
  29. Wang S, Capoen L, D'hooge DR, Cardon L. Can the melt flow index be used to predict the success of fused deposition modelling of commercial poly(lactic acid) filaments into 3D printed materials? Plast Rubber Compos. 2018;47(1):9-16. doi: 10.1080/14658011.2017.1397308
  30. Cobos CM, Fenollar O, Martinez JL, Ferrandiz S, Garzón L. Effect of Maleinized Linseed Oil (MLO) on thermal and rheological properties of PLA/MWCNT and PLA/HNT nanocomposites for additive manufacturing. Rapid Prototyp J. 2020;26(6):1027-1033. doi: 10.1108/RPJ-08-2019-0217
  31. Hussain M, Khan SM, Shafiq M, et al. Comparative study of PLA composites reinforced with graphene nanoplatelets, graphene oxides, and carbon nanotubes: Mechanical and degradation evaluation. Energy. 2024;308:132917. doi: 10.1016/j.energy.2024.132917
  32. Wu Y, Neto V, Valente R, Cavalcanti DKK, Gomes T. Mechanical Characterization of CNT/PLA Parts via FFF Additive Manufacturing. Polym Eng Sci. 2026;66(4):2726-2738. doi: 10.1002/pen.70384
  33. Coppola B, Cappetti N, Di Maio L, Scarfato P, Incarnato L. 3D Printing of PLA/clay Nanocomposites: Influence of Printing Temperature on Printed Samples Properties. Materials. 2018;11(10):1947. doi: 10.3390/ma11101947
  34. Caminero MA, Chacon JM, Garcia-Moreno I, Reverte JM. Interlaminar bonding performance of 3D printed continuous fibre reinforced thermoplastic composites using fused deposition modelling. Polym Test. 2018;68:415-423. doi: 10.1016/j.polymertesting.2018.04.038
  35. Chen Q, Mangadlao JD, Wallat J, De Leon A, Pokorski JK, Advincula RC. 3D Printing Biocompatible Polyurethane/Poly(Lactic Acid)/Graphene Oxide Nanocomposites: Anisotropic Properties. ACS Appl Mater Interfaces. 2017;9(4):4015-4023. doi: 10.1021/acsami.6b11793
  36. Dul S, Fambri L, Pegoretti A. Fused deposition modelling with ABS–graphene nanocomposites. Compos Part A Appl Sci Manuf. 2016;85:181-191. doi: 10.1016/j.compositesa.2016.03.013
  37. Gnanasekaran K, Heijmans T, van Bennekom S, et al. 3D printing of CNT- and graphene-based conductive polymer nanocomposites by fused deposition modeling. Appl Mater Today. 2017;9:21-28. doi: 10.1016/j.apmt.2017.04.003
  38. Kaya H, Arıcı Ş, Bulut O, Bilgili F, Ege D. CNT incorporation improves the resolution and stability of porous 3D printed PLGA/HA/CNT scaffolds for bone regeneration. Biomed Mater. 2023;18(5):055028. doi: 10.1088/1748-605X/acf25d
  39. Adam HM. Emerging advantages and transformative applications of nanocomposites in additive manufacturing: A literature review. Next Res. 2025. doi: 10.1016/J.NEXRES.2025.101155
  40. Kim Y, Kim JS, Lee SY, Mahajan RL, Kim YT. Exploration of hybrid nanocarbon composite with polylactic acid for packaging applications. Int J Biol Macromol. 2020;144:135-142. doi: 10.1016/j.ijbiomac.2019.11.239
  41. Hashim N. Thermal and biodegradable properties of poly(lactic acid)/carbon-based nanocomposites. PhD thesis. Pahang, Malaysia: Universiti Malaysia Pahang; 2020. Axxessed September 2, 2026. https://efind.ump.edu.my/cgi-bin/koha/opac-detail.pl?biblionumber=92626
  42. Ribeiro dos Anjos EG, Marini J, Santos Gomes NA, Rezende MC, Passador FR. Synergistic effect of adding graphene nanoplates and carbon nanotubes in polycarbonate/acrylonitrile-styrene-butadiene copolymer blend. J Appl Polym Sci. 2022;139(37):e52873. doi: 10.1002/app.52873
  43. Wang X, Deng J, Zhao R, Shen L, Wang Z. Compressive response and energy absorption of 3D-printed cellular structures: advances and challenges. Virtual Phys Prototyp. 2026;21(1):e2638085. doi: 10.1080/17452759.2026.2638085
  44. Alibeyoglu F. Mechanical, Thermal, and Microstructural Characterization of FDM-Printed PLA/Obsidian Composites. Polymers. 2026;18(13):1563. doi: 10.3390/polym18131563
  45. Cobos CM, Ferrandiz S, Garzón L, López J, Rayon E. Exploring the mechanical response of PLA/MWCNT and PLA/HNT composites obtained by additive manufacturing. Rapid Prototyp J. 2025;31(11):179-188. doi: 10.1108/RPJ-07-2024-0308
  46. Fathi A, Mahboubkhah M. Surface inclination effects on accuracy and finish in 3-Axis and 5-Axis FDM: toward high-fidelity additive manufacturing. Prog Addit Manuf. 2026;11(6):5321-5335. doi: 10.1007/s40964-026-01612-z
  47. Fathi A, Mahboubkhah M, Entezari Maleki A, Dumlu A, Ayten KK, Kalınay G. Enhanced performance in additive manufacturing: a comparative study of multi-axis and 3-axis FDM for tubular parts. Prog Addit Manuf. 2025;10(11):9923-9938. doi: 10.1007/s40964-025-01219-w
  48. Mahboubkhah M, Khabazi Barab F, Akhbari S. Experimental investigation of the quality and time of supportless printing by 5DoF FDM 3D-printer based on parallel mechanism. J Mech Eng Univ Tabriz. 2026;55(4):13-18. [In Persian] doi: 10.22034/jmeut.2025.67646.3570
  49. Farajian J, Hatami O, Bakhtiari M, Darabinajand B, Mahboubkhah M. Investigation of Mechanical Properties of 3D-Printed PLA Coated with PU/MWCNTs in a Corrosive Environment. Arab J Sci Eng. 2024;49(8):11181-11193. doi: 10.1007/s13369-023-08632-9
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Materials Science in Additive Manufacturing, Electronic ISSN: 2810-9635 Published by AccScience Publishing