International Journal of Plastics Technology (December 2019) 23(2):195–206

https://doi.org/10.1007/s12588-019-09248-1

RESEARCH ARTICLE

A comprehensive investigation of the mechanical behavior

and the dielectrics of pure polylactic acid (PLA) and PLA with graphene
(GnP) in fused deposition modeling (FDM)
N. Vidakis1 · M. Petousis1   · K. Savvakis1 · A. Maniadi1 · E. Koudoumas2

Received: 17 February 2019 / Accepted: 31 October 2019 / Published online: 26 November 2019
© Central Institute of Plastics Engineering & Technology 2019

Abstract
In this work, the mechanical response of fused deposition modeling (FDM) specimens made of polylactic acid (PLA) and
polylactic acid nanocomposite with graphene (PLA GnP) filler is experimentally determined. A wide variety of standard
tests was performed. Test results were assessed to depict quantitatively the mechanical properties of the materials tested.
Comprehensive comparison of the mechanical strength between FDM-printed PLA and PLA GnP polymers was carried
out to illustrate the filler’s impact. Effect of the FDM process in these materials’ properties arises by comparing them to the
ones of the bulk or injection molded specimens, in quantitative and qualitative terms. Comparison demonstrates that both
polymers exhibit similar behavior in every case, with slight domination of the PLA to the PLA GnP composite. Test results
were correlated with the patterns of the specimens’ fractured surfaces, obtained through scanning electron microscopy. Effect
of graphene in the dielectrics of the material is also evaluated, with the measurements showing a significant increase in the
dielectric values, with the addition of this specific nanocomposite in the material.

Keywords  Nanopolymer composites · 3D printing · Fused deposition modeling (FDM) · Polylactic acid (PLA) · PLA with
graphene (PLA GnP) · Mechanical properties

Introduction method. The results of the corresponding experimental stud-

Poly(lactic acid) or polylactic acid or polylactide (PLA) is
a biodegradable aliphatic polyester, derived mainly from
renewable resources. Due to its physical, chemical and
mechanical properties, PLA is the leading and most utilized
biomaterial for numerous applications in medicine. Besides
this use, the specific polymer and its derivatives are widely
employed in industry, since it can effectively replace con-
ventional petrochemical-based polymers [1–5]. PLA is also
extensively employed in fused deposition modeling (FDM),
and therefore a lot of research has been carried out about the
modification of its bulk properties owing to this fabrication
* M. Petousis
petousis@emttu.org
1 PLA test specimens was measured to be at 4017 J/m2, a
Mechanical Engineering Department, Technological
Education Institute of Crete, Estavromenos,
71004 Heraklion, Crete, Greece
2
Electrical Engineering Department, Technological Education
Institute of Crete, Heraklion, Crete, Greece
ies vary significantly due to the printing parameters set and
of the anisotropic nature of FDM-made PLA parts or speci-
mens. In particular, mechanical properties, such as tensile,
compressive and flexural strength, have been studied [1, 2,
4, 6, 7], and the respective results indicated that there is a
direct dependency of them on the building process param-
eters, such as the layer thickness and the printing orientation
[2, 6]. The derived properties were compared to the ones of
specimens made by injection molding [4].
Moreover, the fracture resistance of FDM-made PLA
specimens has also been extensively studied [3, 4, 8, 9].
The dominant testing method was the Izod one [8], while
Charpy’s tests have been conducted to printed PLA com-
posites [9–11]. The mechanical behavior of PLA specimens
was also compared to the one of ABS polymer. Hereby, the
maximum fracture energy (fracture resistance) of printed
value close to the fracture resistance of bulk ABS. In addi-
tion, the fracture resistance for both materials was found
to be increased by increasing the printing temperature [3].

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Another mechanical property of PLA and PLA compos-
ites, i.e., their hardness or microhardness, has been examined
in former investigations. Hereto, it was proven that when the
Rockwell-R testing setup is chosen, the quality and printing
parameters of the 3D-printed specimens significantly affect
the hardness of the polymers, whereas the degree of crystal-
linity induces a negligible impact on the materials’ hardness
[12, 13]. Regarding the Vickers microhardness, it was shown
that specimens printed with a filament made of bulk PLA
illustrated superior microhardness measurements, compared
to the ones of specimens printed with filament made of PLA
composites [14, 15].
Furthermore, since the addition of graphene induces
electrical conductivity to the normally nonconductive bulk
PLA, deep research has been carried out focusing on the
conductivity of PLA-graphene composites versus various
parameters for FDM-printed specimens [16, 17, 20]. On the
other hand, the investigation of the mechanical properties for
PLA-graphene composites is rather poor and fragmentary.
Hereto, just a few mechanical properties, i.e., the tensile
strength, the Izod impact strength and the viscoelastic behav-
ior, have been investigated [16–20]. However, the impact of
the graphene addition on the overall mechanical response
of PLA nanocomposites compared to the one of PLA made
with FDM is not thoroughly and spherically investigated.
The mechanical properties of pure PLA are already
described in detail in the literature. However, for applica-
tions such as cable insulators [21], components in an electri-
cal measurement setup or even as a functional material itself
in an electronic device [22], the electric and dielectric prop-
erties of PLA [23–28] and its composites [29] in 3D-printed
mode are not sufficiently investigated.
In the current work, the mechanical properties of FDM-
made PLA and PLA GnP specimens were studied compre-
hensively, employing tension, compression, flexion, impact,
hardness and microhardness investigations. Although the
mechanical properties of FDM-printed PLA have been stud-
ied in the literature, this specific grade has not been reported
yet. The experimental results of this study have mainly been
employed for the evaluation of the mechanical properties of
the PLA GnP material, in which for most cases studied in
this work (compression tests, flexural tests, hardness and
microhardness measurements) no results are available in the
literature so far.
The experimental course was also supported with scan-
ning electron microscopy, in order to identify also fracture
patterns. The aim of the current research is to illustrate (1)
the importance of a thorough and supervisory overview of
the mechanical properties for polymers and their composites
and (2) a comprehensive comparison between the mechani-
cal responses of FDM-printed specimens, made of bulk PLA
and PLA GnP filaments. The comparison was carried out by
means of commercial filaments, available in the market, and
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International Journal of Plastics Technology (December 2019) 23(2):195–206
the corresponding specimens were printed with the same
printing parameters for every test case, using a low-cost
desktop FDM printer.
The comparison proved a marginally better overall
mechanical response of the PLA polymer for the specific
commercial grades. On the other hand, this slight superiority
of the bulk polymer when compared to the PLA-graphene
composite is not significant enough to overcome the indus-
trial merit and importance of the graphene addition in order
to convert PLA to a conductive composite, which is widely
used in 3D printing of electronics. Moreover, the dielectric
constant of the materials tested was also measured to evalu-
ate the effect of graphene in the dielectric properties of the
PLA material. It was found that the addition of graphene in
the material significantly increases the dielectric constant,
as expected.
Experimental methodology
Materials and processing
Polylactic acid (PLA) filament was procured by XYZprint-
ing (Kinpo Group, Taiwan). Filament had a diameter of
1.75 mm. PLA composite with graphene (PLA GnP) was
acquired from Haydale (UK) [30], and the filament had a
diameter of 1.75 mm as well. Specimens were 3D-printed
by employing a XYZ da Vinci 3-in-1 Pro, a low-cost desktop
printer using the same building parameters for both materi-
als tested, i.e., full infill (solid), a rectilinear infill type (45°
deposition orientation), a layer thickness of 0.25 mm and an
extrusion speed of 20 mm/sec.
Particularly, for the printing temperature, the instructions
of the filaments’ vendors have been applied, i.e., for PLA
polymer nozzle temperature of 195 °C and table temperature
of 50 °C, whereas for the PLA GnP composite a nozzle tem-
perature of 210 °C and table temperature of 60 °C. For each
specific standard test, the orientation and the layering strat-
egy is schematically described in the corresponding figures
below. Each specimen was checked for the printing quality
and the accuracy of its geometry before being tested so that
the ensemble of the specimens was found to be within the
error margin of each standard. The environmental conditions
(temperature, humidity, etc.) were identical for each separate
test according to the specification of the relative standard.
Scanning electron microscopy
In cases that the fracture mode of the tested materials was
to be further documented (especially in tension and impact
tests), scanning electron microscopy (SEM) characterization
was carried out. The SEM analysis was performed using a
JEOL JSM 6362LV electron microscope in high-vacuum
International Journal of Plastics Technology (December 2019) 23(2):195–206 197
mode at 5 kV acceleration voltage on uncoated samples.
Both PLA and PLA GnP samples were proved to be enough
conductive for low-magnification SEM imaging with-
out coating. In any case, the electrical conductivity of the
composite material was enhanced with respect to the pure
one, since its SEM images had better quality, especially for
magnifications larger than × 500, where PLA charging was
strong, not permitting an accurate analysis.
Tension experiments methodology
The specimens for the tensile tests were fabricated accord-
ing to the ASTM D638-02a standard. Figure 1a illustrates
the geometry and printing specifications. In order to meet
the requirements of the standard, seven specimens were pre-
pared for both filament types, since the characterization of
each material requires five successful repeats (within the
limit of the standard deviation).
The tension tests were carried out using an Imada
MX2 test device, employing standardized grips, as shown
in Fig.  1b, c. The test device measures and records the
applied tensile force versus the elongation of the specimen
tested. For every experimental repeat, the same machine
chuck speed of 10 mm/min was set. The assessment of the
Fig. 1  Specimens’ geometry, fabrication conditions and the test
device used for the tensile tests
experimental data offers essential mechanical properties,
such as the tensile strength and the elasticity modulus.
Compression experiments methodology
The specimens for the compression tests were prepared
according to the ASTM D695-02a standard. Figure  2a
illustrates the geometry and the printing specifications as
well, whereas Fig. 2b shows the testing principle. Seven
specimens made of PLA and seven more made of PLA GnP
were prepared. The compressive tests were performed using
a Schenk Trebel Co device, equipped with CLG-2B load
cells (20 kN capacity, 10 N sensitivity and 0.5% accuracy
for the applied load).
To measure the shortening of the specimens, a Sokki
Kenkyujo Co sensor was used, and to prove the measure-
ments, an additional SDP-100c strain gauge (capacity
100 mm, sensitivity 10 μm and nonlinearity 0.2% RO) was
also used to record strain. The test device’s chuck speed was
set to 5 mm/min, according to the standard. The compression
strength and the compression modulus of elasticity of the
tested specimens were calculated in this work.
Flexion experiments methodology
The specimens for the flexion tests were 3D-printed accord-
ing to the specifications of ASTM D790 (three-point bend-
ing of plastics). Figure 3a illustrates the geometry and print-
ing specifications of the specimens. Also, for this test case,
seven specimens made of PLA and seven more made of PLA
GnP were fabricated. The flexion tests were performed by
means of an Imada MX2 tensile test machine, with a setup
complying with the requirements of the standard. The test
setup is demonstrated in Fig. 3b, c for PLA (white) and PLA
Fig. 2  Specimens’ geometry, fabrication conditions and the principle
of the compression tests
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Fig. 3  Specimens’ geometry, fabrication conditions and the test
device used for the three-point bending test of plastics
GnP (black) specimens, respectively. The bending probe’s
speed was set at 10 mm/min.
Experimental data of force versus displacement of the
specimen’s midspan were recorded and logged in a file at a
2000 Hz sampling rate. The bending load F and the deflec-
tion were measured from the instant of contact of the cylin-
drical bearing onto the specimen, up to the termination of
the test (breakage of the examined specimen). The results
of the flexion tests were used to determine critical flexural
strength parameters, such as fractural stress, maximum bend-
ing moment, flexural modulus of rupture, bending strain and
elastic flexural modulus, using standard equations [31, 32].
Impact experiments methodology
Material fracture toughness can be effectively measured
with standardized impact testing techniques, such as Izod or
Charpy’s, using a hammer pendulum. These two techniques
are similar, with their main difference being at the fixture
of the specimen on the apparatus. The specimens for the
impact tests were 3D-printed according to the regulations of
ASTM D6110. Figure 4a illustrates the geometry and print-
ing specifications of the specimens. In this test case, seven
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International Journal of Plastics Technology (December 2019) 23(2):195–206
Fig. 4  Specimens’ geometry, fabrication conditions and the experi-
mental setup used in the Charpy’s apparatus for the impact tests
specimens made of PLA and seven more made of PLA GnP
were fabricated as well.
All specimens had the ASTM standard’s impact notch.
In these series of experiments, a Terco MT 220 Charpy’s
apparatus was employed and the experimental setup is illus-
trated in Fig. 4b for one test case. The apparatus’s ham-
mer was released from the same height at an initial angle
of 162° for each test, in order to depict the absorbed impact
energy. In the Charpy’s experiments, the dynamic energy of
the Charpy’s hammer Ed (J), the absorbed energy (J) by the
specimen owing to the impact and the fracture toughness
(kJ/m2) of the tested materials are derived, by means of the
standard equations [33–36].
Hardness and microhardness methodology
The specimens for hardness tests were 3D-printed, according
to the ASTM D785-08 regulation for the indentation depth.
In the specific case, their dimensions were 50 mm in length,
15 mm in width and 10 mm in thickness. Seven specimens
from each material were built. The hardness standard for
plastics employed in this work was the Rockwell-R. The
experiments were implemented with the aid of an Albert
Gnehm Rockwell apparatus. Testing was performed by ini-
tially preloading the steel ball indenter into the polished
surface of the specimens, using a load of 100 N. The load
was then increased by 500 N and then decreased back to
the level of the minor load. The overall indenter’s load was
600 N. The machine provided directly the Rockwell-R hard-
ness measurements.
Regarding the microhardness following the specifications
of the ASTM E384-17 standards, the applied method was
the micro-Vickers one, with 0.2 kg force scale (1.962 N) and
10 s indentation time. The typical Vickers diamond pyra-
mid was used as indenter (apex angle of 136°), which was
forced onto a polished surface of the specimens. The area
International Journal of Plastics Technology (December 2019) 23(2):195–206 199
of the remaining indentation, after the removal of the dia-
mond pyramid, is calculated directly by the device, from the
remaining imprint’s mean average of the diagonals. Experi-
ments were held with the aid of an Innova Test 400-Vickers
apparatus.
Broadband dielectric spectroscopy
Electrical characterization of the nanocomposites was also
performed by means of broadband dielectric spectroscopy
(BDS) in the frequency range of 0.1 Hz to 1 MHz, per-
formed using a TH2829C LCR precision bridge capable.
Measurements were taken in the frequency range of 20 Hz
to 1 MHz.
Results and discussion
Tensile results and evaluation
Figure 5a illustrates typical load–displacement diagrams for
two (out of ten) random specimens, one made of PLA fila-
ment and the other one by PLA GnP filament. The diagram
contains also two photographs showing the two specimens
Fig. 5  Force versus elongation and stress versus strain typical dia-
grams for PLA and PLA GnP materials, produced by tensile tests
after their failures at the completion of the corresponding
tensile test (Fig. 5c, d). Both materials experience a notable
plastic deformation up to their failures.
According to the predictions of the ASTM D638-02a,
each specimen was measured after its fabrication, in order
to depict its actual cross-sectional area, whereas the actual
initial length is measured after its fixation to the chunk of the
tensile device. By means of these real magnitudes, the afore-
mentioned diagrams were turned into the stress–strain ones
inserted in Fig. 5b. In these diagrams, pictures of the same
as above specimens are also inserted, after their dismount-
ing from the test device (Fig. 5e). Despite the similarity of
the stress–strain diagrams, the pure PLA material exhibits
a stiffer mechanical response than the PLA GnP composite,
a behavior that was further documented by the other four
repeats of the experiment.
Figure 6 summarizes the findings of the tensile experi-
mental course for the tested materials. Figure 6a presents the
mean average tensile strength of 3D-printed specimens made
of PLA and PLA GnP. As mentioned above, the pure PLA is
slightly more tensile resistant than the graphene composite,
when both materials are FDM printed with the same print-
ing strategy, so as to produce directly comparable results.
Besides this direct comparison between the tested inherent
materials, the same diagram includes a further comparison
with results presented in other investigations [1, 2, 17], as
well as with the claims of the materials vendor [30] for the
mold and the filament PLA GnP.
Fig. 6  Tensile strength and modulus of elasticity findings herein com-
pared to corresponding results from the literature and provided ones
for PLA GnP by the filament’s vendor
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More specifically, current research depicted a tensile
strength value for PLA-made specimens of 47.7  MPa
(test deviation ± 2.39 MPa) and for the PLA GnP ones
of 46.0  MPa (± 1.5  MPa, respectively). In addition,
Chacón et al. [2] reported a value of 36 MPa for PLA
FDM-printed specimens, while Shady et al. [1] reported
a value of 59.0 MPa for bulk PLA. Regarding PLA-gra-
phene composites, values reported for the tensile strength
of specimens built with FDM are restricted. Zhang et al.
[17] reported values from 51 MPa, up to 62 MPa for FDM
PLA GnP specimens, varying according to the %(wt) of
graphene to the composite. On the other hand, the fila-
ment’s vendor [30] reports values for molded PLA GnP
specimens as 41 MPa, whereas 53 MPa for the filament
(not a standard test executed for filament).
The comparison of the aforementioned values proves
the tensile strength of pure printed PLA to be higher than
the results found by Chacón et al. [2] and slightly higher
than the corresponding one of the PLA GnP found in
here. It is interesting that the PLA’s tensile strength is
even higher than the claims of the PLA GnP filament’s
vendor for molded specimens [30]. On the other hand, the
tensile strength of PLA GnP found herein is also slightly
higher than the claim of the filament’s vendor for molded
specimens as well.
Furthermore, Fig. 6b illustrates the same comparison,
but for the mean average tensile modulus of elasticity of
the tested 3D-printed plastics. The pure PLA exhibits also
a quite stiffer tensile response than the composite one. In
addition, the specific values for the elastic modulus derived
herein are also compared with the corresponding results of
the same literature as above.
More specifically, a tensile modulus of elasticity
was determined herein to be at 1069.7 MPa (test devia-
tion ± 41.10  MPa) for PLA, whereas at 893.8  MPa
(± 35.6 MPa, respectively) for PLA GnP composite, both
FDM printed. Regarding corresponding results in the litera-
ture, Chacón et al. [2] reported a value of 1009 MPa for PLA
FDM-printed specimens, while Shady et al. [1] reported a
value of 1280 MPa for bulk PLA. Regarding PLA-graphene
composites, Zhang et al. [17] reported values for the elastic-
ity modulus from 1091 MPa, up to 1818.18 MPa for FDM
PLA GnP specimens, varying according to the %(wt) of
graphene to the composite as well. On the other hand, the
filament’s vendor [30] reports values for molded PLA GnP
specimens 2600 MPa, whereas 2900 MPa for the filament
(not a standard test executed for filament).
It is notable that the tensile modulus of elasticity found
herein for printed PLA is considerably higher than the cor-
responding one of the PLA GnP composite, proving a stiffer
response of the pure polymer. On the other hand, the value
of the filament’s vendor for PLA GnP (for molded speci-
mens) seems too high, since it is 290% higher than the one
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International Journal of Plastics Technology (December 2019) 23(2):195–206
found in this investigation, for printed specimens of the same
composite.
Based on the aforementioned tensile properties for
3D-printed PLA and PLA GnP found herein, which docu-
ment a stiffer response of the pure polymer, a more ductile
failure mode was expected for the composite. Therefore,
failed specimens by the tensile test were inspected in SEM
to prove such an expectation. The SEM aspects of Fig. 7a,
c exhibit the fracture surfaces (specimen cross-sectional
view) using a magnification of ×25. The fracture surface of
PLA GnP is evident that had experienced a massive plas-
tic deformation before failure, which proves a more ductile
failure pattern, compared to the more brittle one of the pure
polymer. This behavior is even more evident in the higher
magnification aspects (×1000) that are inserted in Fig. 7b, d.
Compression results and evaluation
According to the presentation of the tensile results, Fig. 8a
illustrates typical load–displacement diagrams for two (out
of ten) random specimens, one made of PLA filament and
the other by PLA GnP one. The diagram contains also a
photograph showing a PLA GnP specimen at the initiation
of its test (Fig. 8c, d). It is evident that the pure PLA required
a higher load in order to experience plastic deformation.
The same response was observed for the ensemble of the
five test repetitions performed for each material. The bar
chart inserted also in the same diagram (Fig. 8c) proves this
behavior, since it contains the mean average maximum load
and the tests’ deviation value for each material.
According to the predictions of the ASTM D695-02a,
each specimen was measured after its fabrication, in order
to depict its actual cross-sectional area and initial length.
Fig. 7  SEM inspection of the failure patterns occurring in tensile
tests of the examined materials proving the PLA as a more brittle
material when printed
International Journal of Plastics Technology (December 2019) 23(2):195–206 201
Fig. 8  Force versus shortening and stress versus strain typical dia-
grams for PLA and PLA GnP materials, produced by tensile tests
By means of these actual magnitudes, the aforementioned
diagrams were transformed to the stress–strain ones inserted
in Fig. 8b. In these diagrams, pictures of PLA specimens
after their failures are also inserted, indicating the typical
brittle failure of the specific polymer. Also, in compression,
the stress–strain diagrams indicate the pure PLA as a more
robust and stiffer material compared to PLA GnP composite,
a behavior that was further documented by the other four
repeats of the experiment.
Figure 9 summarizes the findings of the compression tests
for both materials. Figure 9a presents the mean average com-
pression strength of 3D-printed specimens made of PLA
and PLA GnP. As mentioned above, the pure PLA is more
compression resistant than the graphene composite. Both
materials are FDM printed with the same printing strategy
as well. Besides this direct comparison between the tested
plastics herein, the same diagram includes a further com-
parison with results presented in third-party research [4].
The current work depicted a compression strength
value for PLA-made specimens of 71.2 MPa (test devia-
tion ± 1.3 MPa) and for the PLA GnP ones of 64.4 MPa
(± 1.1  MPa, respectively). In addition, Song et  al. [4]
reported a value of 84.17  MPa for PLA FDM-printed
Fig. 9  Compressive strength and modulus of elasticity findings herein
compared to corresponding results from the literature
specimens and 73.86 MPa for bulk PLA. It has to be noted
that there are not any compression strength values reported
in the literature so far, for PLA/graphene composites.
Furthermore, Fig. 9b contains a comparison for the mean
average compression modulus for the tested 3D-printed plas-
tics. The pure PLA exhibits also a quite stiffer compres-
sive response than the tested composite. In addition, the
specific values for the compression modulus of elasticity
found herein are also compared with the corresponding
results of the same researchers. More specifically, the com-
pression modulus of elasticity was proved herein to be at
2025.6 MPa (test deviation ± 161.2 MPa) for PLA, whereas
at 1403.9 MPa (± 119.1 MPa, respectively) for PLA GnP
composite, both FDM printed. Regarding corresponding
results in the literature, Song et al. [4] reported a value of
3420 MPa for PLA FDM-printed specimens and 3200 MPa
for PLA molded.
A similar comparative response between PLA and PLA
GnP that was observed in tensile tests was found also in
compression ones. The pure polymer was proved to be more
compression resistant and stiffer in compression than the
composite material when both are 3D-printed with the same
building parameters.
Flexion results and evaluation
Figure 10a includes typical load–displacement diagrams for
two (also out of ten) random specimens, made of PLA and
PLA GnP, respectively. The diagram contains also pictures
showing two aspects of PLA and PLA GnP specimens put
aside (Fig. 10c, d), after the completion of their flexion tests.
The results indicate also a stiffer and a higher flexion resist-
ance of PLA compared to PLA GnP composite. On the other
hand, the specimens’ picture clearly shows the more ductile
response of the composite, since at the completion of its test
developed some microcracks in comparison with the pure
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202
Fig. 10  Bending force versus midspan deflection and stress versus
strain typical diagrams for PLA and PLA GnP materials, derived by
flexion tests
PLA, in which a visible brittle macrocrack took place. The
same observation was repeated for the entire test course for
both materials tested.
According to the instructions of the ASTM D790-02, each
specimen was also measured after its print, in order to depict
its actual cross-sectional dimensions to enable the conver-
sion of load–displacement diagrams to flexion stress–strain
ones, using the standard equations [31, 32]. The stress–strain
diagrams for the same test cases are inserted in Fig. 10b. The
flexion stress–strain diagrams also prove pure PLA to be a
stiffer material compared to PLA GnP composite, able to
withstand higher bending loads. An identical behavior was
repeated throughout the flexion tests course.
Figure 11 summarizes the results of the flexion test proce-
dure for both tested materials. Figure 11a presents the mean
average flexural strength of 3D-printed specimens made of
PLA and PLA GnP. As mentioned above, the pure PLA is
again more bending resistant than the graphene composite
when FDM was printed with the same printing parameters.
Besides this direct comparison between the tested materi-
als in this work, the same diagram includes a comparison
with results found in the literature [1, 2, 17] where avail-
able or applicable, as well as with the ones provided by the
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International Journal of Plastics Technology (December 2019) 23(2):195–206
Fig. 11  Flexural strength and modulus of elasticity findings herein,
compared to corresponding results from the literature and the pro-
vided ones for PLA GnP by the filament’s vendor
materials vendor [30] for the mold and the filament PLA
GnP accordingly.
More specifically, the current research depicted a flexural
strength value for PLA-made specimens of 82.9 MPa (test
deviation ± 1.4 MPa) and for the PLA GnP ones of 78.1 MPa
(± 2.0 MPa, respectively). In addition, Chacón et al. [2]
reported a value of 46.3 MPa for PLA FDM-printed speci-
mens, while Shady et al. [1] reported a value of 106.0 MPa
for bulk PLA. Regarding PLA-graphene composites, there
are not any former works so far in the literature for flexural
strength. On the other hand, the filament’s vendor [30] offers
flexural strength values neither for molded PLA GnP nor for
the filament, since it is not applicable to rods.
Furthermore, Fig. 11b illustrates the flexural modulus
of elasticity that was calculated herein to be 2026.7 MPa
(test deviation ± 74.7  MPa) for PLA and 2088.1  MPa
(± 79.4  MPa, respectively) for PLA GnP. In addition,
Chacón et al. [2] reported a value of 1326 MPa for PLA
FDM-printed specimens. Regarding PLA-graphene compos-
ites, there are not any former works so far in the literature for
flexural elasticity modulus. On the other hand, the filament’s
vendor [30] provides flexural elasticity for molded PLA GnP
up to 2800 MPa but not for filament for the same reason.
Impact results and evaluation
The impact test results as derived by the execution of
standard Charpy’s tests are summarized in Fig. 12a. The
International Journal of Plastics Technology (December 2019) 23(2):195–206 203

In order to interpret better the impact results, the cross-

sectional fracture area of specimens printed with PLA poly-
mer and PLA GnP composite was further investigated using
SEM. Figure 12b illustrates such aspects for both materials
tested (in ×100 magnification). The expected more brittle
failure pattern of the PLA polymer compared to the PLA
GnP composite also appears in this test. The addition of the
nanographene platelets affects positively the ductility of the
pure polymer, but at the same time decreases considerably
the strength of the composite against impact loading.

Hardness and microhardness results and evaluation

A rigorous but at the same time informative test commonly

used in plastics, i.e., the Rockwell hardness test, allows the
rapid characterization of the inspecting material regarding
its resistance against a local load able to produce a massive
plastic deformation. In addition, the wear resistance of plas-
tics can also be evaluated. Figure 13 summarizes the results
of Rockwell-R tests that were performed in both materi-
als. The printed PLA GnP exhibits at this test a marginally
higher hardness, i.e., HRR 99.75 ± 2.09, whereas one of the
Fig. 12  Fracture toughness of PLA and PLA GnP, SEM analysis and PLA polymers was found to be HRR 97.91 ± 2.55.
comparison with former impact investigations for similar materials The hardness results derived herein were further com-
pared to the ones of former research works of the corre-
sponding literature. Perego et  al. [12] presented results
Charpy’s test, among others, depicts the impact resistance for printed specimens made of pure PLA up to HRR 88.8,
of the notched specimen’s material in terms of the fracture whereas Vian et al. [13] measured HRR 110, also for pure
toughness (kJ/m2). This magnitude expresses the amount printed PLA. There are not any former investigations or
of impact energy that is absorbed by the specimen, in order reports for the hardness of PLA-graphene composites. It
to cause its fracture. Hereby, the PLA-printed specimens was proved here that the compound macrohardness of the
indicated a mean average fracture toughness at 20.28 kJ/ printed specimens is not affected somehow by the graphene
m2(test deviation ± 1.72 kJ/m2), whereas the correspond- addition.
ing value for PLA GnP is 13.19  kJ/m 2 (± 0.79  kJ/m 2, On the other hand, when micro-indentations were per-
respectively). formed, the behavior of the composite is significantly
The impact results derived herein were further compared
to the ones of former investigations with Charpy’s tests, car-
ried out by third-party researchers. Slapnik et al. [9] reported
impact strength for pure PLA bulk material equal to 12.5 kJ/
m2 and for PLA FDM a value of 11 kJ/m2. On the other
hand, Tian et al. [10] reported a fracture toughness value
of 20.0 kJ/m2 for printed PLA-notched specimens, which
is more fitting to the corresponding finding of the present
paper. The impact resistance of PLA-graphene composites
has not been investigated so far by other researches. There-
fore, the value of 13.19 kJ/m2 found herein for printed PLA
GnP is the first reported one. Tian et al. [10] found also a
fracture toughness value of 34.5 kJ/m2 for FDM PLA rein-
forced with carbon fibers specimens. It is remarkable that the
graphene nanoplatelets worsen the impact resistance of PLA
(a 35% reduction for the composite of this work), whereas
the carbon fibers improve considerably the same polymer (a Fig. 13  Rockwell-R hardness measurements for PLA and PLA GnP
72.5% increase for the composite of [10]). compared to values reported in the literature

13

204 International Journal of Plastics Technology (December 2019) 23(2):195–206

modified. More specifically, Fig. 14 presents the results of

Vickers microhardness tests for the plastics investigated in
the present work. FDM-printed pure PLA specimens are
proved to be harder up to 74% compared to the PLA GnP,
i.e., micro-HV 16.68 ± 2.56 versus micro-HV 9.59 ± 0.73,
respectively. In the relevant literature, microhardness Vick-
ers measurements have been reported by Li et al. [14] at
micro-HV 18.52 and by Ostafinska et al. [15] at micro-HV
16.5, for bulk PLA and FDM-printed PLA, respectively.
Microhardness results for PLA-graphene composites are
not reported in the corresponding literature.

Overall assessment of the mechanical response

of materials tested

The ensemble of the results and quantitative findings of the

present work was inserted in the supervisory form of radar
diagrams, one per material tested. Figure 15 illustrates such
a visual comparison between FDM-printed PLA and PLA
GnP material, for the specific grade tested. The hard result
of this comparison is that the addition of graphene nano-
platelets in PLA does not improve the combined mechanical
response of the composite, contrarily; it reduces more or
less the mechanical properties of the pure PLA, in terms of
FDM-printed tests’ specimens. Besides this rather qualita-
tive remark, the quantitative data summarized by this radar
chart allow the implementation of precise studies or FEA
simulations to complicated geometries which are to be pro-
duced with FDM printing techniques.
On the other hand, the conversion of the pure PLA to
a highly conductive composite when graphene is added is
a major accomplishment that plays a dominant role in the
electronics industry. Hereby, conductive circuits (test pro-
totypes and/or commercial products) can be rigorously and
cost-effectively 3D-printed. Therefore, the selection of pure
Fig. 15  Comparison of the overall mechanical response of FDM-
printed PLA polymer versus PLA GnP composite
PLA or PLA GnP is a strongly case-dependent procedure
and decision.
Broadband dielectric spectroscopy
In this work, 500 Hz was set as a reference frequency for the
evaluation of the dielectric constant. The dielectric constant
of the samples measured at 500 Hz is presented in Table 1
and compared to findings in the corresponding literature.
As can be seen from the results of Table 1, the incor-
poration of graphene nanoplatelets in the PLA matrix sig-
nificantly increases the dielectric constant of the specimens
at 500 Hz to 1 MHz. A similar response was found for the
frequencies up to 1 MHz, with the actual dielectric constant
value becoming slightly smaller as the frequency increases.
Comparing the results derived from this work with the
literature, it is evident that minor logical variations in dielec-
tric constant exist, which is the cause of the differences in

Table 1  Dielectric constant results at 500 MHz for PLA, PLA FDM

and PLA GnP FDM

Material Dielectric constant ε

PLA bulk [21] 3.10

PLA FDM [28] 2.95
PLA FDM [27] 2.85–3.20
PLA FDM 3.45
PLA GnP FDM 4.50
Fig. 14  Vickers microhardness of PLA and PLA GnP compared to
PLA conductive FDM [29] 6.41
values reported in the literature

13
International Journal of Plastics Technology (December 2019) 23(2):195–206 205
printing parameters and the PLA materials’ structural vari-
ations. Also, it has to be mentioned that the dielectric con-
stant is directly affected by frequency.
Comparing 3D-printed PLA and 3D-printed PLA with
graphene results to the literature, and specifically to PLA
conductive and magnetic filaments [29], it is proven that
carbon-based fillers, such as graphene or carbon nanotubes,
significantly increase the dielectric constant of the printed
samples and their conductivity.
Conclusions
The tension, compression, flexion and impact mechanical
responses accompanied with macro- and microhardness
investigations of fused deposition modeling parts manu-
factured by polylactic acid (PLA) and PLA with graphene
nanoplatelets (PLA GnP) were thoroughly studied and com-
prehensively compared in this work. For the implementation
of the characterization course, commercial-grade filaments
for both materials have been utilized. In terms of mechanical
response and strength, the comparison of the two plastics
proved the PLA polymer performs better than the PLA GnP
composite. For the same printing parameters, the PLA speci-
mens exhibited higher stiffness, increased values of criti-
cal stresses and a more brittle fractural behavior. Also, the
dielectric constant of the materials tested was measured to
evaluate the effect of the addition of graphene in pure PLA,
with the results showing as expected a significant increase
in the dielectric constant, while the 3D printing process
does not affect significantly the dielectric properties of the
material.
To expand the validity of the research presented herein,
a wide literature survey was performed, in cases where rel-
evant results were reported in third-party investigations.
The current research work enriches the literature, induc-
ing a variety of quantitative mechanical properties for both
materials that were yielded by the execution of a laborious
volume of standardized tests. Particularly for the case of the
PLA GnP material, no similar results have been presented
in the literature for most cases studied in this work, i.e.,
compression tests, flexural tests, hardness and microhard-
ness measurements. The results presented in this work hold
significant scientific, technological and industrial merit since
the proper selection of the filament to be utilized in FDM
printing is a high case-dependent task. On the other hand,
quantitative values for the mechanical properties of the
materials tested herein can support and document compli-
cated simulations and FEA analyses for the optimization of
complex geometries to be printed. Further research is to be
implemented to test other grades of graphene compositions
within the PLA matrix, as well as for different 3D printing
technologies and/or printing strategies.
Acknowledgements  Authors would like to thank Dr. Mirella Suchea
(IMT Bucharest) for the SEM support. This research did not receive
any specific grant from funding agencies in the public, commercial, or
not-for-profit sectors.
Funding  No funding was received for this work.
Compliance with ethical standards 
Conflict of interest  The authors declare that they have no conflict of
interest.
Ethical approval  This article does not contain any studies with human
participants or animals performed by any of the authors.
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