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. 2022 Sep 26;14(19):4022.
doi: 10.3390/polym14194022.

Polylactide/Carbon Black Segregated Composites for 3D Printing of Conductive Products

Olha Masiuchok  1   2   3   4 , Maksym Iurzhenko  3   4 , Roman Kolisnyk  3 , Yevgen Mamunya  3   4 , Marcin Godzierz  1   2 , Valeriy Demchenko  3   4 , Dmytro Yermolenko  3 , Andriy Shadrin  3
Affiliations

Polylactide/Carbon Black Segregated Composites for 3D Printing of Conductive Products

Olha Masiuchok et al. Polymers (Basel). .

Abstract

One of the most important directions in the development of additive manufacturing or three-dimensional (3D) printing technologies is the creation of functional materials, which allow not only prototyping but also the manufacturing of products with functional properties. In this paper, poly-lactide acid (PLA) /carbon black (CB) composites with segregated (ordered) structure have been created. Computer simulation based on the Mamunya geometrical model showed that the CB content within φ = 2.5-5 vol.% in the polylactide matrix leads to the formation of a continuous electrically conductive phase with an increase of electrical conductivity σdc above the percolation threshold. The simulation results were experimentally confirmed by optical microscopy and studies of the electrical conductivity of the composites. It was found that increasing CB content from φ = 1 vol.% to φ = 7 vol.% in the composites causes insignificant (due to the segregated structure) phase changes in the polylactide matrix and improves the thermal properties of composites. Electrically conductive filaments for Fused Deposition 3D Printing (FDM) were developed from PLA/CB composites and then 3D printed. A correlation between the electrical conductivity σdc and the CB content φ for base composites, filaments produced from them, and final 3D samples, has been found. Conductivity varies within σdc = 3.1·10-11 - 10·10-3 S/cm for the filaments and σdc = 3.6·10-11 - 8.1·10-4 S/cm for the final 3D-products.

Keywords: FDM 3D printing; electrical conductivity; morphology; poly (lactic acid)/carbon black composites; segregated structure; thermal behavior.

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Conflict of interest statement

The authors declare no conflict of interest.

Figures

Figure 1
Figure 1
SEM images of the carbon black (CB) ENSACO 250G (a,b).
Figure 2
Figure 2
Scheme of the formation process of the segregated polymer composites by the method of hot compaction, where d—diameter of the CB particles, D—diameter of the PLA particles.
Figure 3
Figure 3
Mamunya geometrical model of the framework structure of the segregated polymer system. Reprinted from Ref. [32]. Model parameters: D = L + nd, where L is the size of an excluded volume of the polymer, n is the number of layers of the conductive particles in the framework, D—size of the polymer particles, d—size of the filler particles.
Figure 4
Figure 4
Results of computer modeling of the segregated structure of PLA/CB composite depending on evolution of CB content φ: 1 vol.% (a), 2.5 vol.% (b), 5 vol.% (c), and 7 vol.% (d).
Figure 4
Figure 4
Results of computer modeling of the segregated structure of PLA/CB composite depending on evolution of CB content φ: 1 vol.% (a), 2.5 vol.% (b), 5 vol.% (c), and 7 vol.% (d).
Figure 5
Figure 5
Optical images of the cross-sections of cylindrical specimens PLA + 1 vol.% CB (a). PLA + 2.5 vol.% CB (b), PLA + 5 vol.% CB (c), PLA + 7 vol.% CB (d).
Figure 5
Figure 5
Optical images of the cross-sections of cylindrical specimens PLA + 1 vol.% CB (a). PLA + 2.5 vol.% CB (b), PLA + 5 vol.% CB (c), PLA + 7 vol.% CB (d).
Figure 6
Figure 6
Optical images of the transversal cross-sections of the filaments PLA + 1 vol.% CB (a), PLA + 2.5 vol.% CB (b), PLA + 5 vol.% CB (c), PLA + 7 vol.% CB (d).
Figure 6
Figure 6
Optical images of the transversal cross-sections of the filaments PLA + 1 vol.% CB (a), PLA + 2.5 vol.% CB (b), PLA + 5 vol.% CB (c), PLA + 7 vol.% CB (d).
Figure 7
Figure 7
Images of the longitudinal section of the filament with the CB content φ = 2.5 vol%: (a) optical microscopy, (b) SEM.
Figure 8
Figure 8
SEM images of the transverse cross-section of the specimen’s 3D printed with filaments: PLA + 1 vol.% CB (a), PLA + 2.5 vol.% CB (b), PLA + 5 vol.% CB (c), PLA + 7 vol.% CB (d).
Figure 9
Figure 9
DSC curves of the unfilled PLA filament and the filled composite filaments: PLA + 1 vol.% CB; PLA + 2.5 vol.% CB; PLA + 5 vol.% CB and PLA + 7 vol.% CB. The numbers near the curves indicate the content of CB in composites.
Figure 10
Figure 10
DSC curves (Ⅰ run) of the 3D-printed specimens, obtained from the composite filaments with various CB content.
Figure 11
Figure 11
DSC curves (Ⅱ run) of the 3D-printed specimens, obtained from the composite filaments with various CB content.
Figure 12
Figure 12
WAXS patterns of the composite filaments with various CB content φ.
Figure 13
Figure 13
WAXS patterns of the 3D specimens, obtained from the composite filaments with various CB content φ, inset in the figure shows patterns for PLA/CB composites with 5 and 7 vol.% of CB.
Figure 14
Figure 14
Dependences of electrical conductivity σdc of specimens on the CB content.
Figure 15
Figure 15
Dependences of mechanical strength of specimens on CB content.
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