Additive Manufacturing Letters 4 (2023) 100106

Contents lists available at ScienceDirect

Additive Manufacturing Letters

journal homepage: www.elsevier.com/locate/addlet

Short Communication

Thermal conductivity of 3D-printed continuous pitch carbon fiber

composites
Sinan Olcun, Yehia Ibrahim, Caleb Isaacs, Mohamed Karam, Ahmed Elkholy, Roger Kempers∗
Department of Mechanical Engineering, York University, Toronto, Canada

a r t i c l e i n f o a b s t r a c t

Keywords: A new method was developed to 3D print high-thermal-conductivity, pitch-based continuous carbon fiber com-
Thermal conductivity posites. This process uses a dual extruder to selectively print polylactic acid (PLA) or PLA-coated pitch carbon
3D printing fibers. The effective thermal conductivity of unidirectionally 3D-printed specimens was characterized experi-
Pitch carbon fiber
mentally for samples fabricated from fibers with different conductivities and at different volume fractions: Three
Composites
grades of pitch carbon fibers were used with conductivities ranging from 140 to 800 W/mK. Carbon fiber volume
fractions ranging from 6.25% to 11.7% were investigated. A maximum thermal effective thermal conductivity of
37.1 W/mK was measured for a 9.5% volume fraction of the K13D2U pitch carbon fiber which is significantly
higher than that of any 3D-printed carbon-based composites measured previously. However, the measured effec-
tive thermal conductivities were significantly lower than those predicted by the parallel model. Breakage of the
fibers post-printing was confirmed using micro-computed tomography and suggests that higher effective thermal
conductivities can be obtained by better mitigating fiber breakage during the printing process. Future directions
for this technology are discussed.

1. Introduction conductivity represents a limitation to the thermal performance of these

Thermal dissipation from electronics requires heat sinks and heat
exchangers with large surface areas, especially air-cooled technologies
where the convective heat transfer coefficients can be limited. How-
ever, large and heavy thermal management technologies are not accept-
able in many applications (e.g., automotive, electronics, aerospace, etc.)
[1,2,3,4].
Lightweight polymer heat exchangers and heat sinks are a growing
technology and, when appropriately designed, are suitable for many ap-
plications [5]. However, their limiting performance factor is typically
polymer thermal conductivity which limits their wider adoption [6].
The additively manufacturing (AM) of polymer composites can help ad-
dress the need for lightweight and effective heat exchangers in two ways:
First, thermally conductive polymer composites can offer a lightweight
alternative to metals because of their significantly lower density and
their thermal conductivity can be sufficiently high to spread heat from
the heat source to the extents of the heat sink for dissipation to the
surrounding fluid [7]. Secondly, AM affords design freedom to fabri-
cate complex geometries which can be used to enhance convective heat
transfer [8–11].
To this end, several studies have examined the 3D-printing of ther-
mally conductive discontinuous polymer composites for heat exchange
applications [12–15]. However, the relatively low solid-phase thermal
devices: the discontinuous nature of the filler limits effective thermal
conductivity due to the interfacial interaction and adhesion between
the particles (or chopped fibers) and the matrix [16,17]. To address this
shortcoming, continuous fillers such as fiber yarns can be used to fabri-
cate continuous fiber polymer composites (CFPCs).
Because the fibers are continuous, the composites to be better influ-
enced by the filler material [18] and the dominant factor defining the
composite properties is the fiber volume fraction. Analytical models can
predict the properties of CFPCs as a function of their matrix and fiber
properties the fiber volume fraction [19,20], however, because fibers
have a very high aspect ratio and significantly different properties in
different directions, CFPCs are highly anisotropic materials. The prop-
erties of these composites depend greatly on the direction of the fibers
relative to the applied stress for mechanical applications or direction of
heat flow for thermal applications [21,22]. As such, placement and ori-
entation of the fibers for a given application is crucial and 3D printing
can be leveraged to control fiber parameters.
Continuous fibers have been implemented in fused filament fabrica-
tion (FFF) to create robust CFPC components [23,24]. In FFF printers,
it is common to coat the fibers with a polymer layer prior to printing;
this allows the pre-coated fiber rasters to stick to adjacent printed layers
[25]. Several FFF approaches have been extensively used to print CFPCs
and can be broadly categorized into two main techniques: The first ap-

∗
Corresponding author.
E-mail address: kempers@yorku.ca (R. Kempers).

https://doi.org/10.1016/j.addlet.2022.100106
Received 22 June 2022; Received in revised form 24 November 2022; Accepted 26 November 2022
2772-3690/© 2022 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/)
S. Olcun, Y. Ibrahim, C. Isaacs et al.
proach uses a single nozzle to print pre-coated fiber filaments such as
in [26, 27]. In this technique, the printing process offers little control
over the volume fraction of the fibers and only simple structures can be
fabricated unless a cutting mechanism is utilized [28]. The second ap-
proach implements two printing nozzles where one extrudes the fibers
and the other extrudes the polymer matrix [29,30]. This technique has
been adopted by different commercial 3D printer manufacturers because
it offers more flexibility and control over fiber location and volume frac-
tion.
Characterization and improvement of mechanical properties have
been the primary focus of much of the research on 3D-printed CFPCs
with the focus on polyacrylonitrile (PAN) carbon fibers (CF) and glass
fibers [31,32]. However, some fibers have very attractive thermal prop-
erties, such as pitch-based CF and carbon nanotube yarns whose ther-
mal conductivity along the fiber axis can reach up to 1100 W/mK and
6000 W/mK, respectively [33].
The effective thermal conductivity of PAN CFPCs manufactured us-
ing the commercially available Markforged Mark One 3D printer was
investigated and shown to improve the thermal conductivity of the
composite material significantly in the direction of the fibers (up to
2.97 W/mK at a volume fraction of 32.2% compared with 0.265 W/mK
for the pure nylon samples) [34]. In another study, a modified open-
source FFF printer used a single nozzle to co-extrude continuous copper
wire with polylactic acid (PLA) to create continuous wire polymer com-
posites (CWPCs) which demonstrated thermal conductivities of up to
9.4 W/mK using a volume fraction of 2.7% [35]. In both studies, simple
thermal resistance network models were shown to accurately predict
the effective thermal conductivity of the 3D-printed composites, sug-
gesting that fiber conductivity and volume fraction play a direct role in
the effective thermal conductivity of the composite [34,35]. To illustrate
this, Ibrahim et al. [34] fabricated a proof-of-concept pitch-based car-
bon fiber hand layup sample which exhibited a thermal conductivity of
23.6 W/mK for a volume fraction of only 4.3% pitch CF and showed that
high effective thermal conductivities can be achieved using pitch-based
CF or other highly conductive fibers.
Here again, the ability to leverage 3D printing to directionally con-
trol the placement and quantity of continuous pitch-based carbon fiber
would allow for the design of components with high and direction-
ally controllable effective thermal conductivities. Together, these ad-
vantages would help further the development of high-performance,
lightweight heat exchange technologies such as heat sinks, heat ex-
changers, or low-temperature evaporators for thermosyphons and other
two-phase applications. In addition, 3D printing could afford control
over conductivity anisotropy, enabling the creation of heat exchangers
with thermal pathways customized for specific applications.
In this study, the first ever method for 3D printing CFPCs using high-
thermal-conductivity pitch-based CF is described and used to investigate
the effect of fiber conductivity and volume fraction on the effective ther-
mal conductivity of unidirectionally fabricated samples. An analytical
model is used to predict the thermal conductivity of the fabricated ma-
terials and deviations from the theoretical predictions are discussed.
2. Materials and methods
2.1. Materials
Three grades of pitch CF manufactured by Mitsubishi Chemical Car-
bon Fiber and Composites were investigated and are summarized in
Table 1. The polymer matrix used in this investigation was a transparent
PLA (1.75 mm PLA filament, ColorFabb, Netherlands). Despite being a
relatively low-temperature thermoplastic, PLA was used because of its
relative ease of processing and 3D-printing. From an application stand-
point, the composites printed using this method would be useful for low-
temperature heat sink applications or two-phase applications which use
low-boiling point refrigerants such as thermosyphons. For higher tem-
2
Additive Manufacturing Letters 4 (2023) 100106
perature applications, polyetherimide (PEI) or polyether ether ketone
(PEEK) could be employed.
2.2. Fiber pre-coating
Pitch-based CFs offer very high thermal conductivities, tensile
strength, and modulus. However, they have relatively very low flexural
strength which makes processing these fibers challenging. To facilitate
the 3D printing of the continuous pitch-based CFs in Table 1, the fiber
tows were first coated with molten PLA, as shown in Fig. 1a, to create
pre-coated carbon fiber filaments which are easier to handle and can be
extruded by the 3D printer. A pultrusion process was used to draw the
CF through a bath of molten PLA through a 0.8 mm diameter nozzle; the
CF was subsequently cooled to create a relatively stiff polymer-coated
CF filament. The temperature of the polymer bath was held constant at
235 °C to ensure that the PLA was completely molten and that minimal
shearing forces would result from the viscosity of the polymer. Upon
pultrusion, the coated CF filament tended to expand to approximately
1 mm in diameter. A cross-section of the coated fiber filament is shown
in Fig. 1b. The resulting filament was not uniformly round, and the fibers
tended to accumulate slightly more towards the outer perimeter of the
filament (this may be related to the slight expansion after exiting the
0.8 mm nozzle prior to cooling). The fibers were distributed relatively
evenly within the PLA in the azimuthal direction.
2.2. Printer modification & hotend design
In a previous study, Ibrahim et al. modified a low-cost printer to co-
extrude metal wires with a polymer to increase the tensile and flexural
strength of the printed components [37,38] and other researchers have
modified printers to print with continuous fibers [39,40]. In these stud-
ies, the continuous printed wires or fibers are extruded from the nozzle
at a 90° angle to the printing bed. This sharp angle can exacerbate fiber
breakage during the extrusion of pitch-based CF due to its lower flexu-
ral strength, especially compared with metal wires and PAN fibers used
in previous studies. Breakage of the continuous fibers must be avoided
because discontinuities reduce the effective thermal conductivity of the
fabricated composite.
An open-source FFF printer (Prusa MK2 i3, Prusa Research) was mod-
ified to print with the pre-coated pitch-based carbon fiber filaments de-
scribed above. To help address the challenge of pitch CF breakage, a
custom printing head angled at 45° to the printed bed was designed
to help lower fiber breakage by reducing the bending stress on the CF
filament during extrusion. The custom heating block was made of alu-
minum and designed to allow for the use of dual extrusion nozzles as
shown in Fig. 2b. The right nozzle was used to extrude the polymer ma-
trix at 90° to the bed, while the left nozzle printed the pre-coated fibers
at 45° In this way, the fibers were subjected to less bending stress during
printing, and the use of dual nozzles allowed for more control over the
fiber-to-polymer ratio and print quality.
A second feed motor allowed for independent control fiber and poly-
mer extrusion. The fiber feed motor was fixed directly in front of the
fiber printing heat sink, allowing for optimal control in feeding the fibers
into the printing nozzle, with the shaft of the motor wrapped in rubber
to ensure feeding traction. The coated fibers were fed through the heat
sink with a PTFE tube to guide the filament until it was extruded; this
insulated the fiber filament to ensure it did not melt and clog inside the
nozzle. The polymer was fed separately using the conventional Bowden
extruder mechanism specified by the Prusa multi-material expansion kit.
Standard 30 mm cooling fans were used to cool the polymer and fiber
filament heat sinks (not shown in Fig. 2a). Also, while the figure shows
both nozzles extruding simultaneously, in practice only one nozzle was
used at a time for a given layer, as explained below.
The fixed position of the extruders relative to the motion of the ho-
tend restricted fiber printing to the x-direction only and therefore af-
forded the creation of only unidirectional samples. One solution for this
S. Olcun, Y. Ibrahim, C. Isaacs et al. Additive Manufacturing Letters 4 (2023) 100106

Table 1
Pitch Carbon Fiber Grades [36].

Fiber Grade Fiber count per Single fiber diameter Tensile modulus Tensile strength Density (g/cm3 ) Thermal Conductivity
tow (𝜇m) (GPa) (MPa) (W/mK)

K1352U (52 U) 2000 10 620 3600 2.12 140

K1392U (92 U) 2000 10 760 3700 2.15 210
K13D2U (D2U) 2000 11 935 3700 2.20 800

Fig. 1. a) Fiber coating setup showing main components, b)

cross-sectional photo of a coated pitch CF filament.

limitation is to implement a rotating bed which would allow for fiber Table 2
placement in any direction in the x–y plane while keeping the CF ex- Printing Parameters.
truder at a 45° angle relative to the printing bed. Another potential op- Fiber filament diameter (mm) ≈1
tion is to mount the extruders to a 5- or 6-axis robotic arm which can
Fiber nozzle diameter (mm) 1.5
articulate to provide further control of the CF printing angle and di-
Fiber printing speed (mm/s) 50
rection and further minimize bending stress on the fibers during extru- Polymer filament diameter (mm) 1.75
sion. However, for the present study, the objective is limited to quantify- Polymer nozzle diameter (mm) 1
ing the effective thermal conductivity of simple unidirectionally printed Polymer printing speed (mm/s) 20
Extruder temperature ( °C) 200
samples.

2.3. Printing parameters

The printing parameters are summarized in Table 2. For the approx-
imately 1 mm coated fiber filament, a nozzle diameter of 1.5 mm was
used to help minimize friction between the fibers and the nozzle. A poly-
mer nozzle of 1 mm was selected to match the filament diameter; how-
ever, it can be changed to any size. The printing temperature was set to
200 °C which is recommended for PLA. The lower printing speed was
selected (20 mm/s) to allow for the solidification of the PLA within the
fiber filament while printing; it also helped the geometrical quality of
the printed components.
To facilitate full control over fiber and polymer layers, a fiber cutting
mechanism is often implemented [34]. However, for the unidirectional
samples printed in the present study, the fiber was sufficiently brittle
such that inclusion in the printing code of a sudden movement of the
printing head in the reverse direction was sufficient to break the fibers.
This allowed for the printing of different fibers and polymer rasters in
the same printing layer. In addition, the simplicity of the cutting mecha-
nism made it possible to print relatively thin fiber walls compared with
those printed by printers with cutting mechanisms [34].
2.4. Sample dimensions and configurations
Three samples with varying pitch fiber content were fabricated for
each of the fiber grades listed in Table 1. The sample dimensions and

3
S. Olcun, Y. Ibrahim, C. Isaacs et al. Additive Manufacturing Letters 4 (2023) 100106

Fig. 2. a) Dual nozzle hot end assembly, b) detailed view

of heating block.

Table 3 number of PLA layers, N, between the fiber layers, as shown in Fig. 3b.
Sample Parameters. The samples with the lowest volume fraction consisted of four layers of
Height (mm) 40 PLA between each layer of pitch CF (N = 4), the mid-volume faction
samples had N = 3 layers of PLA between the fiber layers, and the high-
Width (mm) 40
est volume fraction samples had N = 2 layers of PLA between each CF
Thickness (mm) 25
Polymer layer height (mm) 0.4 layer.
Polymer raster width (mm) 0.4 For each volume fraction, three grades of pitch-based carbon fiber
Fiber layer height (mm) 0.8 (listed in Table 1) were printed. All the samples were printed with a
Fiber raster width (mm) 1
transparent PLA matrix to easily differentiate between the polymer and
Infill percentage (%) 100
Fiber orientation (°) 0
the fibers.
Polymer orientation (°) 0
2.5. Thermal conductivity measurement

layer parameters are listed in Table 3, a photograph of sample and
schematics of the layer configurations is shown in Fig. 3a, and pho-
tographs of the cross-sections of each fiber volume fraction are presented
in Fig. 3b. The sample geometry was designed with a 40 × 40 mm cross-
sectional area to fit in the testing facility. A relatively large layer height
(0.4 mm) was used for the PLA layers to accommodate the large noz-
zle size (1 mm). For the pitch CF layers, a layer height of 0.8 mm was
sufficient to create uniform rasters with good adhesion to the polymer
layers below.
The printing G-code, which defined the printer movements and the
amount of the extruded material, was customized to fabricate samples
with the desired aspects. The code was generated using the default slic-
ing software of the printer (Sli3er) and then manually modified to fab-
ricate samples with the required dimensions.
The samples were fabricated with a range of pitch carbon fiber con-
tent to investigate the effect of the fiber volume fraction on the effective
thermal conductivity on the samples. This was achieved by varying the
The effective conductivity of the samples was measured using the ap-
paratus developed in [41] and [42] which directly quantifies the steady-
state thermal resistance within the sample and calculates thermal con-
ductivity using Fourier’s law of conduction.
A schematic of the apparatus is shown Fig. 4. Input power is con-
ducted from the primary heating block, through the sample, to the
primary cooling block. Two calibrated thermocouples are embedded
10 mm apart within each sample (denoted by Ta and Tb in Fig. 4).
This removes contact resistance from the conductivity measurement.
The thermal power is provided electrically by four cartridge heaters em-
bedded in the main heating block. To achieve a one-dimensional heat
flow through the sample and eliminate heat loss to the ambient, the pri-
mary heating block was enclosed by a secondary heating block which
served as a guard heater. The power supplied to the guard heater block
was independently controlled to achieve the same temperature as the
primary heating block, ensuring that all input power to the primary
heating block flowed through the sample. Consequently, at steady-state
conditions, the sample thermal resistance was measured using according

4
S. Olcun, Y. Ibrahim, C. Isaacs et al.
Fig. 3. a) Sample photograph and schematic of the build layer approach, b) cross-sectional photographs of the samples for the different volume fraction configurations.
Fig. 4. Schematic for the thermal conductivity measurement approach.
to
( )
𝑇𝑎 − 𝑇𝑏
𝑅𝑚𝑒𝑎𝑠 =
𝑄 ity, analytical models can be used to predict the effective thermal con-
where (Ta -Tb ) is the measured temperature drop within the sample, and
𝑄 is the input power to the primary heating block measured electrically
(𝑄 = 𝐼𝑉 ). Thus, the thermal conductivity can be calculated by rewrit-
Additive Manufacturing Letters 4 (2023) 100106
ing Eq. (1) as
𝐿
𝑘𝑚𝑒𝑎𝑠 = [ ] (2)
(𝑇 𝑎 − 𝑇 𝑏 )
𝐴 𝑄
where 𝐿 is the distance between the thermocouples (10 mm), and 𝐴 is
the sample cross-sectional area perpendicular to the heat flow.
Additional details regarding design, construction, and uncertainty
analysis for this apparatus are presented in [41,42].
2.6. Fiber breakage analysis
Micro-computed tomography (microCT) was used to investigate the
morphology of the printed samples and assess the existence and de-
gree of fiber breakage. A Bruker SkyScan 1272 MicroCT was used to
image the sample. Images of the printed samples had a resolution of
4904 × 3280 pixels with an individual pixel size of 0.5 μm in length.
In total, 3600 images were captured at rotational steps of 0.1°, with the
full scan taking 5 h to complete. Sample images were then reconstructed
into cross-sectional scans using NRecon (Bruker-MicroCT) to create 500
images perpendicular to the z-axis. These images were used to recon-
struct a 3D representation of the sample in which only the fibers were
visible; this could be further examined for printing errors.
3. Thermal conductivity modeling
(1) With knowledge of the fiber volume fraction and the directional-
ductivity of the composite material. Previous investigations of similarly
unidirectional PAN 3D-printed CFPCs and 3D-printed CWPCs show that
the parallel model predicts the effective thermal conductivity with good
agreement [34,35]. Because the fibers are aligned parallel with the heat
5
S. Olcun, Y. Ibrahim, C. Isaacs et al.
Fig. 5. Sample thermal conductivity (measured and predicted by the parallel model) as a function of fiber volume fraction for fiber grades a) 52 U, b) 92 U, c) D2U,
and d) comparison of measured thermal conductivity of all three fiber grades.
flow direction, as shown in Fig. 3a, the parallel model can be utilized to
compute the effective thermal conductivity of the sample as
( )
𝑘𝑒𝑓 𝑓 = 1 − 𝑣𝑓 𝑘𝑝 + 𝑣𝑓 𝑘𝑓 (3)
where vf is the fiber volume fraction, and kp and kf are the polymer and
fiber thermal conductivities, respectively. Here, the thermal conductiv-
ity value reported by the carbon fiber manufacturer was used (Table 1).
For the polymer, kp =0.2 W/mK was used in the model, according to
[42]. Volume percentage of carbon fiber in each sample was calculated
by finding the sum of the cross-sectional area of all the individual fibers.
A layer of carbon fiber found in the sample consisted of 40 rasters, with
each raster theoretically containing 2000 fibers. Three separate G-code
files were created with 16, 19, and 25 layers of CF evenly distributed
through the sample. With knowledge of the cross-sectional area of a
single fiber and the total number of fibers in the sample, the volume
percentage of the fibers was calculated.
4. Results and discussion
4.1. Effect of fiber grade and volume fraction
The three grades of pitch CF listed in Table 1 were each printed at
three different volume fractions using the layer configurations shown
in Fig. 3. Their effective thermal conductivity as a function of volume
fraction is shown in Fig. 5.
Generally, the samples with higher fiber conductivities tended to
have higher measured effective thermal conductivities at a given vol-
ume fraction. Also, broadly speaking, the effective conductivity of the
samples tended to increase with volume fraction. The highest measured
thermal conductivity was 37.1 W/mK for the D2U sample with a vol-
6
Additive Manufacturing Letters 4 (2023) 100106
ume fraction of 9.5% pitch CF. That said, the effective conductivities
tended to plateau (and slightly decrease in the case of the D2U fiber) at
the highest volume fraction.
The corresponding thermal conductivity predicted using the contin-
uous parallel thermal model (Eq. (1)) is also plotted in Fig. 5a–c and
predicts a linear variation in effective thermal conductivity as a function
of volume fraction. For all the samples tested, their measured thermal
conductivities are lower than that predicted by the parallel model: The
52 U samples had average keff values that were 33% lower than pre-
dicted by Eq. (1), the 92 U samples were on average 38% lower, and
the D2U samples were on average 61% lower.
One possible reason for the discrepancy between the experimental
results and model prediction may be the accuracy of the fiber ther-
mal conductivity or cross-sectional area—number of fibers and diame-
ter—specified by the manufacturer (fiber diameters are particularly im-
portant because this parameter is squared). These parameters should be
independently quantified.
The parallel model (Eq. (3)) represents an idealized thermal model
where there is no breakage of fibers and therefore no discontinuity in
the conduction paths. Because pitch-based CF are relatively brittle com-
pared with PAN fibers, the deviation between the model and the ex-
perimental results is conjectured to be caused by fiber breakage during
the coating and/or printing process, causing discontinuities in the fibers
of the 3D-printed CFPC samples and therefore fewer continuous path-
ways for effective conduction. There are several points during the pro-
cess where breakage to the fibers may occur (including the fiber coat-
ing/impregnation process, the printer feeding mechanism, and at the
exit from the extrusion nozzle where the fibers make a 45° turn) and
the effect of each of these steps should be investigated systematically
to assess their effect on fiber continuity. The relative deviations from
S. Olcun, Y. Ibrahim, C. Isaacs et al.
Fig. 6. Photograph comparing the layers upon which the pitch CF layers are printed for a) the lowest and b) highest volume fraction samples, highlighting difference
in relative roughness.
Fig. 7. MicroCT images of Sample D2U at 9.5% fiber volume fraction showing fiber breakage.
the model predictions suggest that the relative degree of fiber break-
age depends on the grade of fiber used: The pitch-based CF grades with
lower thermal conductivities and tensile modulus exhibit less breakage
than the samples printed with CF with higher thermal conductivity and
tensile modulus.
Another notable feature of the results is the plateau or relative de-
crease in effective thermal conductivity at the highest volume fractions
for every fiber grade (Fig. 5d). Fig. 6 compares the layers upon which
the pitch CF layers are printed for the lowest and the highest volume
fraction samples. For the low vf samples, the four polymer layers left
a smooth surface for the next CF layer. However, at the highest vol-
ume fraction, there are fewer polymer layers (N = 2), and the CF print
surfaces remain relatively rough, likely contributing to additional fiber
breakages in the higher vf samples.
4.2. Analysis of fiber breakage
An 8 mm x 8 mm x 20 mm section of the 3D-printed D2U sam-
ple (9.5% vf ) was cut from the larger 3D-printed sample for microCT
scanning. Images of the 9.5% vf D2U sample are shown in Fig. 7. Here,
fiber breakage and misalignment are distinctly visible. This provides a
reasonable explanation for the somewhat lower keff measurements than
predicted by the parallel rule-of-mixture model. Analysis of the images
revealed that breakage of the pitch CF tended to occur more on the upper
side of the CF layers, which is hypothesized to be due to forces exerted
7
Additive Manufacturing Letters 4 (2023) 100106
by the polymer extruder passing over the layers and pushing down on
the previously printed CF layer causing the breakage.
4.3. Comparison with other 3D-Printed carbon composites
Many investigations have 3D-printed polymer composites which
contain some type of carbon-based filler; however, most of these have
focused on the mechanical properties of the printed components. Several
studies characterized the thermal conductivity of 3D-printed carbon-
based composite samples, and the maximum thermal conductivity from
these investigations are summarized in Table 4.
In all cases, the thermal conductivity of the 3D-printed composite
was higher than the base matrix material. Most previous studies used
discontinuous filler particles which were premixed with the matrix ma-
terials in the desired volume fraction prior to extrusion. This allowed
for good control over the filler fraction and generally required mini-
mal modification to the printing hardware itself. Investigations which
combined CF with other filler materials, such as graphene nanoplatelets
(GNP) [46] or alumina [48] exhibited somewhat higher measured ther-
mal conductivities (e.g., up to 7.46 W/mK measured by Ji et al. [48]).
In the study by Ibrahim et al. [34], 3D-printed composites which used
continuous CF yielded a maximum effective thermal conductivity of
2.97 W/mK but required a volume fraction of 32.2% because of the
relatively low thermal conductivity of the PAN fibers used.
The present work differs from [34] by using nominally continuous
pitch CF, which have significantly higher thermal conductivities than
S. Olcun, Y. Ibrahim, C. Isaacs et al. Additive Manufacturing Letters 4 (2023) 100106

Table 4
Summary of Thermal Conductivities of 3D-Printed Carbon-Based Composites.

Fiber/Filler Material(s) Matrix Material Filler Type Filler Fraction Max. Thermal Conductivity Ref.
(W/mK)

Carbon Fiber PLA Discontinuous Unspecified (Robo 3D) 0.36 [41,42]

Carbon Fiber PLA Discontinuous ≈15% by wt. (Protopasta) 0.502 [41,42]
Carbon fiber Acrylonitrile butadiene styrene Discontinuous 1.7% by vol. 0.22 [43]
(ABS)
Graphite ABS Discontinuous 4.3% by vol. 0.37 [43]
Carbon fiber Polyether ether ketone (PEEK) Discontinuous 30% by wt. 0.61 (at 25 °C) [44]
Carbon fiber Polypropylene (PP) Discontinuous 10% by vol. 0.869 [45]
Graphite nanoplatelets EPON 862 Discontinuous 7.6% CF and 9.3% graphite by 1.83 (at 25 °C) [46]
(GNPs) and carbon fiber wt.
GNPs and carbon Polyamide 12 (PA12) Discontinuous 15% GNP and 0.73 (at 30 °C) [47]
nanotubes (CNTs) 1% CNT by wt.
Carbon fiber and Silicone rubber Discontinuous 12% CF and 30% alumina by 7.36 [48]
alumina vol.

CNTs Polyphenylene sulfide (PPS) Discontinuous 0.9% by wt. 0.264 [49]

CNTs ABS Discontinuous 6% by wt. ≈0.19 (at 25 °C) [50]
≈0.21 (at 75 °C)
Nano-graphite PLA and thermoplastic Discontinuous 12.5% by wt. 0.47 [51]
polyurethane (TPU)
Short carbon fiber (SCF) Polycarbonate (PC) Discontinuous 10% by vol. ≈0.22 [52]
Carbon fiber Polyethylene terephthalate glycol Discontinuous Unspecified (Nanovia PETG CF) 0.2146 [53]
(PETG)
Carbon fiber (milled) PLA Discontinuous 30% by wt. 0.209 (at 70 °C) [54]
0.212 (at 90 °C)
CNTs PLA Discontinuous 12% by wt. 0.320 - 0.365 [55–58]
GNPs PLA Discontinuous 12% by wt. 0.662 - 0.664 [55–58]
PAN carbon fiber Nylon Continuous 32.2% by vol. 2.97 [34]
Pitch carbon fiber PLA Continuous 9.5% by vol. 37.1 Present Work

PAN fibers and therefore require less fiber volume fraction filler to
achieve 3D-printed composites with higher effective thermal conduc-
tivity. However, the main drawback of this approach is the increased
brittleness of the fiber, which results in a significant degree of break-
age during printing and limits the thermal conductivity of the samples.
However, despite having lower than predicted values, the thermal con-
ductivities measured herein are significantly higher than any previously
3D-printed carbon-based composite and show promise for potential heat
transfer applications. For example, the thermal conductivities of the
D2U 3D-printed composites are significantly higher than those of stain-
less steel (k ≈ 18 W/mK).
5. Summary and outlook
A method for 3D printing pitch-based continuous CF was developed
and used to fabricate unidirectional pitch carbon fiber and PLA compos-
ites. The effective thermal conductivities of 3D-printed CFPC samples
fabricated from fibers of different conductivities and at different vol-
ume fractions were characterized experimentally and compared to the
parallel effective conductivity model. The key findings are:
• Effective thermal conductivity increased with pitch fiber conductiv-
ity.
• Sample thermal conductivity generally increased with fiber volume
fraction; however, for the highest volume fractions, keff tended to
plateau due to rougher layers on which the CF layers were printed.
• A maximum effective thermal conductivity of 37.1 W/mK was mea-
sured using a 9.5% volume fraction of pitch carbon fiber.
• The parallel thermal model overpredicted the effective thermal con-
ductivity of the samples due to suspected fiber breakage occurring
during the printing process.
• MicroCT analysis confirmed a degree of breakage in the printed fiber
rasters.
Future research should address improving the thermal conductivity
of the printed parts by developing a better understanding of factors af-
fecting fiber breakage and to improve the pitch CF extrusion process to
mitigate fiber breakage.
In addition, the design freedom and motion control offered by more
advanced 3D-printing platforms (e.g., 6-axis robotic arm [59–61]) can
be fully leveraged with high-conductivity fibers to create composites
with strategically designed fiber orientations to control anisotropy and
offer heat transfer directionality control and conductive pathways for
specific heat exchange applications.
Funding
Natural Sciences and Engineering Research Council of Canada, Grant
No. RGPIN-2018-05879.
Declaration of Competing Interest
On behalf of all authors, the corresponding author states that there
is no conflict of interest.
Data Availability
Data will be made available on request.
Acknowledgment
The authors acknowledge the support of the Natural Sciences and
Engineering Research Council of Canada (NSERC).
References
[1] P. Samudre, S.V. Kailas, Thermal performance enhancement in open-pore metal
foam and foam-fin heat sinks for electronics cooling, Appl. Therm. Eng. 205 (2022)
pp117885, doi:10.1016/j.applthermaleng.2021.117885.
[2] X. Lai, C. Wang, D. Peng, H. Yang, Z Wei, Analysis of heat transfer characteris-
tics of a heat exchanger based on a lattice filling, Coatings 11 (9) (2021) 1089,
doi:10.3390/coatings11091089.
[3] Q. Liu, G. Xu, J. Wen, Y. Fu, L. Zhuang, B Dong, Multivariate design and analysis of
aircraft heat exchanger under multiple working conditions within flight envelope,
ASME. J. Thermal Sci. Eng. Appl. June 2022; 14 (6) (October 13, 2021) 061003,
doi:10.1115/1.4052342.

8
S. Olcun, Y. Ibrahim, C. Isaacs et al.
[4] S. Narumanchi, M. Mihalic, G. Moreno, K. Bennion, Design of light-weight, single-
phase liquid-cooled heat exchanger for automotive power electronics, in: 13th In-
terSociety Conference on Thermal and Thermomechanical Phenomena in Electronic
Systems, 2012, pp. 693–699, doi:10.1109/ITHERM.2012.6231495.
[5] I.O. Mikulionok, Use of polymer materials in heat exchangers (review of patents),
Chem. Petrol. Eng. 55 (2019) 687–695, doi:10.1007/s10556-019-00680-z.
[6] A.R.J. Hussain, et al., Review of polymers for heat exchanger applications: Factors
concerningthermal conductivity, Applied Thermal Engineering 113 (2017) 1118–
1127, doi:10.1016/j.applthermaleng.2016.11.041.
[7] M.A. Vadivelu, C. Ramesh Kumar, G.M. Joshi, Polymer compos-
ites for thermal management: a review, Compos. Interface. (2016),
doi:10.1080/09276440.2016.1176853.
[8] H. Moon, K. Boyina, N. Miljkovic, W.P. King, Heat transfer enhancement
of single-phase internal flows using shape optimization and additively man-
ufactured flow structures, Int. J. Heat Mass Transf. 177 (2021) 121510,
doi:10.1016/j.ijheatmasstransfer.2021.121510.
[9] O. Al-Ketan, M. Ali, M. Khalil, R. Rowshan, K.A. Khan, R.K Abu Al-Rub, Forced con-
vection computational fluid dynamics analysis of architected and three-dimensional
printable heat sinks based on triply periodic minimal surfaces, ASME. J. Thermal
Sci. Eng. Appl. April 2021; 13 (2) (2020) 021010, doi:10.1115/1.4047385.
[10] Y.S. See, J.Y. Ho, K.C. Leong, T.N. Wong, Experimental investigation of a topology-
optimized phase change heat sink optimized for natural convection, Appl. Energy
314 (2022) 118984, doi:10.1016/j.apenergy.2022.118984.
[11] S. Unger, M. Beyer, H. Pietruske, L. Szalinski, Uwe Hampel “Air-side
heat transfer and flow characteristics of additively manufactured finned
tubes in staggered arrangement, Int. J. Therm. Sci. 106752 (161) (2021),
doi:10.1016/j.ijthermalsci.2020.106752.
[12] K. Timbs, M. Khatamifar, E. Antunes, W. Lin, Experimental study on the heat
dissipation performance of straight and oblique fin heat sinks made of ther-
mal conductive composite polymers, Therm. Sci. Eng. Progr. 22 (2021) 100848,
doi:10.1016/j.tsep.2021.100848.
[13] B. Ahmadi, S. Bigham, Performance evaluation of hi-k lung-inspired 3D-
printed polymer heat exchangers, Appl. Therm. Eng. 204 (2022) 117993,
doi:10.1016/j.applthermaleng.2021.117993.
[14] M.A. Arie, D.M. Hymas, F. Singer, A.H. Shooshtari, M. Ohadi “An additively man-
ufactured novel polymer composite heat exchanger for dry cooling applications”
International Journal of Heat and Mass Transfer, Volume 147, 2020, 118889.
doi:10.1016/j.ijheatmasstransfer.2019.118889.
[15] David C. Deisenroth, Ramin Moradi, Amir H. Shooshtari, Farah Singer, Avram Bar-
Cohen, Michael Ohadi (2018) “Review of Heat Exchangers Enabled by Polymer
and Polymer Composite Additive Manufacturing” Heat Transfer Engineering, 39:19,
1648-1664, doi:10.1080/01457632.2017.1384280.
[16] Y. Qin, et al., Interfacial interaction enhancement by shear-induced 𝛽-cylindrite
in isotactic polypropylene/glass fiber composites, Polymer (Guildf) 100 (2016)
111–118 June 2018.
[17] K. Yu, M. Wang, J. Wu, K. Qian, J. Sun, X. Lu, Modification of the interfacial interac-
tion between carbon fiber and epoxy with carbon hybrid materials, Nanomaterials
6 (12) (2016) 89.
[18] P.J. Herrera-Franco, A. Valadez-González, Mechanical properties of continuous nat-
ural fibre-reinforced polymer composites, Compos. Part A Appl. Sci. Manuf. 35 (3)
(2004) 339–345.
[19] H. Ku, H. Wang, N. Pattarachaiyakoop, M. Trada, 217.A review on the tensile prop-
erties of natural fiber reinforced polymer composites, Compos. Part B Eng. 42 (4)
(2011) 856–873.
[20] Y.-.M. Chen, J.-.M. Ting, Ultra high thermal conductivity polymer composites, Car-
bon N. Y. 40 (2002) 359–362.
[21] L. Ibos, J. Dumoulin, V. Feuillet, Determination of anisotropic properties of carbon
fiber composites for civil engineering applications using infrared thermography with
periodic excitation, 12th Int. Conf. Quant. InfraRed Thermogr, 2014.
[22] J. Schuster, D. Heider, K. Sharp, M. Glowania, Thermal conductivities of three-
-dimensionally woven fabric composites, Compos. Sci. Technol. 68 (9) (2008)
2085–2091.
[23] P. Parandoush, D. Lin, A review on additive manufacturing of polymer-fiber com-
posites, Compos. Struct. 182 (2017) 36–53.
[24] X. Wang, M. Jiang, Z. Zhou, J. Gou, D. Hui, 3D printing of polymer matrix compos-
ites: a review and prospective, Compos. Part B Eng. 110 (2017) 442–458.
[25] G.D. Goh, et al., Characterization of mechanical properties and fracture mode of ad-
ditively manufactured carbon fiber and glass fiber reinforced thermoplastics, Mater.
Des. 137 (2018) 79–89.
[26] N. Li, Y. Li, S. Liu, Rapid prototyping of continuous carbon fiber reinforced poly-
lactic acid composites by 3D printing, J. Mater. Process. Technol. 238 (2016) 218–
225.
[27] X. Tian, T. Liu, C. Yang, Q. Wang, D. Li, Interface and performance of 3D printed con-
tinuous carbon fiber reinforced PLA composites, Compos. Part A Appl. Sci. Manuf.
88 (2016) 198–205.
[28] T.H.J. Vaneker, Material extrusion of continuous fiber reinforced plastics using com-
mingled yarn, Procedia CIRP 66 (2017) 317–322.
[29] T. Liu, X. Tian, M. Zhang, D. Abliz, D. Li, G. Ziegmann, Interfacial performance and
fracture patterns of 3D printed continuous carbon fiber with sizing reinforced PA6
composites, Compos. Part A Appl. Sci. Manuf. 114 (2018) 368–376 September.
[30] G.W. Melenka, B.K.O. Cheung, J.S. Schofield, M.R. Dawson, J.P. Carey, Evaluation
and prediction of the tensile properties of continuous fiber-reinforced 3D printed
structures, Compos. Struct. 153 (2016) 866–875.
[31] J. Justo, L. Távara, L. García-Guzmán, F. París, Characterization of 3D printed long
fibre reinforced composites, Compos. Struct. 185 (2018) 537–548 October 2017.
Additive Manufacturing Letters 4 (2023) 100106
[32] C. Oztan, et al., Microstructure and mechanical properties of three dimension-
al-printed continuous fiber composites, J. Compos. Mater. (2018).
[33] C.I. Idumah, A. Hassan, Recently emerging trends in thermal conductivity of polymer
nanocomposites, Rev. Chem. Eng. (2016).
[34] Y. Ibrahim, A. Elkholy, J. Schofield, G.W. Melenka, R. Kempers, Effective ther-
mal conductivity of 3D-printed continuous fiber polymer composites, Adv. Manuf.:
Polym. Composit. Sci. 6 (2020) 17–28.
[35] Y. Ibrahim, R. Kempers, Effective thermal conductivity of 3D-printed
continuous wire polymer composites, Progr. Addit. Manuf. (2021),
doi:10.1007/s40964-021-00256-5.
[36] Mitsubishi Chemical Carbon Fiber and Composites, Inc., 2021, Pitch Fiber, accessed
2021-11-11 (http://mccfc.com/pitch-fiber/).
[37] Y. Ibrahim, G.W. Melenka, R. Kempers, Additive manufacturing of continuous wire
polymer composites, Manuf. Lett. 16 (2018) 49–51 April.
[38] Y. Ibrahim, G.W. Melenka, R. Kempers, Fabrication and tensile testing of 3D printed
continuous wire polymer composites, Rapid Prototyp. J. (2018) October.
[39] H. Prüß, T. Vietor, Design for fiber-reinforced additive manufacturing, J. Mech. Des.
137 (11) (2015) 111409.
[40] S. Liu, Y. Li, N. Li, A novel free-hanging 3D printing method for continuous carbon
fiber reinforced thermoplastic lattice truss core structures, Mater. Des. 137 (2018)
235–244.
[41] A. Elkholy, R. Kempers, An accurate steady-state approach for characterizing the
thermal conductivity of additively manufactured polymer composites, Case Stud.
Therm. Eng. 31 (2022) 101829, doi:10.1016/j.csite.2022.101829.
[42] A. Elkholy, M. Rouby, R. Kempers, Characterization of the anisotropic thermal con-
ductivity of additively manufactured components by fused filament fabrication,
Progr. Addit. Manuf. 4 (2019) 497–515.
[43] Corey Shemelya, Angel De La Rosa, Angel R. Torrado, Kevin Yu, Jennifer Do-
manowski, Peter J. Bonacuse, Richard E. Martin, Michael Juhasz, Frances Hurwitz,
Ryan B. Wicker, Brett Conner, Eric MacDonald, David A. Roberson, "Anisotropy
of thermal conductivity in 3D printed polymer matrix composites for space
based cube satellites" Additive Manufacturing, Volume 16, 2017, Pages 186–196,
doi:10.1016/j.addma.2017.05.012.
[44] A.A. Stepashkin, et al., 3D-printed PEEK-carbon fiber (CF) composites: struc-
ture and thermal properties, Compos. Sci. Technol. 164 (2018) 319–326,
doi:10.1016/j.compscitech.2018.05.032.
[45] M. Spoerk, et al., Anisotropic properties of oriented short carbon fibre filled
polypropylene parts fabricated by extrusion-based additive manufacturing, Com-
posit. Part A 113 (2018) 95–104, doi:10.1016/j.compositesa.2018.06.018.
[46] N. Nguyen, et al., Direct printing of thermal management device us-
ing low-cost composite ink, Macromol. Mater. Eng. 302 (2017) 1700135,
doi:10.1002/mame.201700135.
[47] Z. Zhang, et al., 3D printing processability of a thermally conductive compound
based on carbon nanofiller-modified thermoplastic polyamide 12, Polymers 14
(2022) 470, doi:10.3390/polym14030470.
[48] J. Ji, et al., Enhanced thermal conductivity of alumina and carbon fibre
filled composites by 3-D printing, Thermochim Acta 690 (2020) 178649,
doi:10.1016/j.tca.2020.178649.
[49] S. Pan, et al., Effect of carbon nanotube on thermal, tribological and mechanical
properties of 3D printing polyphenylene sulfide, Addit. Manuf. 47 (2021) 102247,
doi:10.1016/j.addma.2021.102247.
[50] A. Dorigato, et al., Electrically conductive nanocomposites for fused deposition mod-
elling, Synth. Met. 226 (2017) 7–14, doi:10.1016/j.synthmet.2017.01.009.
[51] R. Guo, et al., Electrical and thermal conductivity of polylactic acid (PLA)-based
biocomposites by incorporation of nano-graphite fabricated with fused deposition
modeling, Polymers (Basel) 11 (2019) 549, doi:10.3390/polym11030549.
[52] A. Gupta, et al., Thermal characterization of short carbon fiber reinforced high tem-
perature polymer material produced using the fused filament fabrication process, J.
Manuf. Process. 80 (2022) 515–528, doi:10.1016/j.jmapro.2022.06.024.
[53] S. Valvez, et al., Optimization of printing parameters to maximize the mechani-
cal properties of 3D-printed PETG-based parts, Polymers (Basel) 14 (2022) 2564,
doi:10.3390/polym14132564.
[54] I. Blanco, et al., Specific heat capacity and thermal conductivity measurements of
PLA-based 3D-printed parts with milled carbon fiber reinforcement, Entropy 24
(2022) 654, doi:10.3390/e24050654.
[55] P. Lamberti, et al., Evaluation of thermal and electrical conductivity of carbon-
based PLA nanocomposites for 3D printing, AIP Conf. Proc. (1981) 020158 2018,
doi:10.1063/1.5046020.
[56] G. Spinelli, et al., Nanocarbon/Poly(Lactic) acid for 3D printing: effect of fillers con-
tent on electromagnetic and thermal properties, Materials (Basel) 12 (2019) 2369,
doi:10.3390/ma12152369.
[57] G. Spinelli, et al., Dielectric spectroscopy and thermal properties of poly(lactic) acid
reinforced with carbon-based particles: experimental study and design theory, Poly-
mers (Basel) 12 (2020) 2414, doi:10.3390/polym12102414.
[58] G. Spinelli, et al., Thermal and dielectric properties of 3D printed parts based on
polylactic acid filled with carbon nanostructures, Macromol. Symp. 405 (2022)
2100244, doi:10.1002/masy.202100244.
[59] P. Urhal, A. Weightman, C. Diver, P. Bartolo, Robot assisted additive manufacturing:
a review, Robot Comput. Integr. Manuf. 59 (2019) 335–345.
[60] A. İpekçi, B. Ekici, Experimental and statistical analysis of robotic 3D printing pro-
cess parameters for continuous fiber reinforced composites, J. Compos. Mater. 55
(19) (2021) 2645–2655.
[61] S. Miri, et al., Tensile and thermal properties of low‑melt poly aryl ether ketone
reinforced with continuous carbon fiber manufactured by robotic 3D printing, Int.
J. Adv. Manuf. Technol. 122 (2022) 1041–1053, doi:10.1007/s00170-022-09983-7.