Additive Manufacturing Letters 1 (2021) 100007

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Additive Manufacturing Letters

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

Large-scale additive manufacturing tooling for extrusion-compression

molds
Pritesh Yeole a,b,c, Seokpum Kim b, Ahmed Arabi Hassen b, Vipin Kumar b, Vlastimil Kunc b,
Uday Vaidya a,b,c,∗
a
Department of Mechanical, Aerospace, and Biomedical Engineering, University of Tennessee, Estabrook Rd, Knoxville, TN 37996, USA
b
Energy and Transportation Science Division, Oak Ridge National Laboratory, Knoxville, TN, 37932, USA
c
Institute for Advanced Composites Manufacturing Innovation (IACMI), 2370 Cherahala Blvd, Knoxville TN 37932, USA

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

Keywords: Carbon fiber reinforced polymer composites (CFPC) have been used in additive manufacturing (AM) due to
Thermal conductivity both the high-strength-to-weight and superior-stiffness-to-weight ratios. CF AM is being considered for tooling
Infill pattern applications. In AM, CFPCs are usually aligned along the deposition direction; however, it results in anisotropic
Extrusion deposition fabrication – additive
thermal properties which affect the heat transfer and warpage of the final part. In this study, three male molds
manufacturing
with different infill patterns were produced via the material extrusion additive manufacturing (EDF-AM) process.
These include (a) 0°: infill pattern along the printing direction; (b) 90°: infill pattern perpendicular to the printing
direction; and (c) 0°/90°: alternate layers along and perpendicular directions. The effect of the infill pattern on
thermal conductivity was analyzed and observed that 0° infill (surface temperature: 79.2°C) had the highest
conductivity; and 90° infill (surface temperature: 66.4°C) had the least.
Highlights (for Review): In Additive manufacturing, carbon fibers are usually aligned along the deposition di-
rection; however, it results in anisotropic thermal properties which affect the heat transfer and warpage of the
final part. In this study, three molds with different infill patterns were produced via the extrusion deposition
fabrication-additive manufacturing (EDF-AM) process. These include (a) 0°: infill pattern along the printing di-
rection; (b) 90°: infill pattern perpendicular to the printing direction; and (c) 0°/90°: alternate layers along and
perpendicular directions. Mold was used for extrusion compression molding and degradation of the mold was
analyzed using non-contact laser scanning device.

1. Introduction fordable (due to complex shapes) tool designs; and (iv) Increased ability
to customize parts [3]. Significant research has been focused on imple-
Computer numerical control (CNC) machining is a commonly used menting AM for tooling applications. Leal et al. [4] developed stamping
and highly reliable to produce dies and tools (molds). CNC machining AM tooling for the production of automotive body panels. Wu et al.
requires highly skilled labor, is time-consuming and expensive [1]. In [5] presented design optimization of AM for injection tooling. Mueller
the last decade alone, more than one-third of the tool and die companies et al. [6] developed sheet metal forming tools through AM.
have gone out of business in the US because of overseas migration due to The growth in AM over the last two decades has made significant
cost considerations [2]. Additive manufacturing (AM) enables creating changes in composite tooling. According to [7] AM of tooling inserts,
final parts through layer-wise printing. AM offers potential advantages dies should reduce the cost and time of manufacturing. Masood et al.
over traditional tool manufacturing process because of the following [8] used metal/polymer composite material in AM and proved its ap-
factors- (i) Lead time reduction: fabrication of tooling by AM can result plication for rapid prototype tooling. Recent developments in polymer
in time savings due to fewer labor inputs, machining steps, use of dig- extrusion AM have created significant attention for composite mold pro-
ital design files rather than two-dimensional (2D) paper drawings and duction. Printing outside an oven is possible due to the introduction
in-house tooling; (ii) Cost reduction: AM for tooling helps cost reduction of low thermal expansion coefficient carbon fiber (CF) in polymer AM,
due to decrease in material scrap resulting from machining, improving which provides not only stiff structures but also high dimensional sta-
product yield and reducing labor inputs; (iii) Improved functionality: bility [9-12]. Cincinnati Incorporated and Oak Ridge National Labora-
AM allows the manufacturing of previously unobtainable and/or unaf- tory (ORNL) in partnership have created a large-scale big area additive
manufacturing (BAAM) system (6 m × 2.5 m × 1.5 m) to manufacture

∗
Corresponding author.
E-mail address: [email protected] (U. Vaidya).

https://doi.org/10.1016/j.addlet.2021.100007
Received 25 July 2021; Received in revised form 18 August 2021; Accepted 21 August 2021
2772-3690/© 2021 The Author(s). 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/)
P. Yeole, S. Kim, A.A. Hassen et al. Additive Manufacturing Letters 1 (2021) 100007

Fig. 1. Schematic of AM extruder with fiber orientation profile inside the deposited bead. Fibers are aligned along the edge while randomly oriented inside the bead
[29].

AM parts which can deposit material at a rate of 45 kg/hr. The feed- bead [9]. Properties of fiber reinforced polymers (FRPs) depend on the
stock materials for BAAM are pellets, rather than wires, which signif- orientation of fibers [27]; therefore, the mechanical and thermal prop-
icantly reduces cost and also broadens the supply chain of materials erties of the composite material are influenced by the orientation of the
[13]. Kunc et al. [14] used BAAM system to fabricate autoclave molds deposited layer. In this manuscript, we assumed all fibers were highly
and showed less than 0.1 mm deformation after autoclave cycle. Has- aligned along the deposition direction.
sen et al. [15] manufactured AM mold for vacuum assisted resin transfer The performance in terms of surface finish, mechanical stability,
molding (VARTM) process to understand the durability of the composite dimensional accuracy of the EDF-AM parts depends on the individual
mold. bead, bonding between beads and the deposition strategy [28]. As the
Conventional manufacturing techniques for CF polymers include pre- fiber orientation is a function of bead deposition direction, printing
cursors such as PAN, mesophase pitch which then undergoes melt spin- strategies of the part need to be designed carefully to have the opti-
ning, oxidation, carbonization and graphitization to create an ordered mized fiber orientation in the desired directions. A typical individual
structure similar to single crystal graphite [16]. Therefore, CF polymer 2D layer during 3D printing is mainly divided into perimeter and in-
is a highly anisotropic material with different mechanical and thermal fill patterns. Perimeters also known as contours or shells usually outline
properties along transverse directions [17]. Thermal conductivity and the border of the structure and provide the scaffolding of the structure.
the coefficient of thermal expansion (CTE) are essential material proper- The infill pattern also known as raster’s pattern fill the area inside the
ties of CF polymer composites when used at elevated temperature envi- perimeters [29]. Aw et al. showed the direct relation of tensile proper-
ronments [16, 18-22]. At elevated temperature, CF polymer composites ties, dynamic storage modulus and inversely proportional loss modulus,
possess a wide range of elastic moduli, thermal expansion, and thermal damping factor with infill density [30]. Shemelya et al. [31] showed that
conductivity [23]. Pradere et al. [16] explained that the CTE of CF poly- thermal conductivity of AM structures can be controlled by a combina-
mers along the transverse direction varies from 5 × 10−6 K−1 – 10 × 10−6 tion of raster pattern and material design. As the whole structure can
K−1 ; however, along the longitudinal direction offers lower expansion be printed only using infill pattern by eliminating the perimeter lines,
with 1.6 × 10−6 K−1 – 2.1 × 10−6 K−1 based on the fiber properties. a very limited work is done to understand the effect of perimeter lines
Therefore, thermal conductivity and expansion (warpage) characteris- [32].
tics of chopped/short composites are highly influenced by the fiber ori- Engineering thermoplastic polymer (polyphenylene sulfide (PPS))
entation [24]. retain physical properties at high temperatures and offer thermal sta-
The extrusion deposition fabrication - additive manufacturing (EDF- bility for a long period of time [33-37]. Therefore, CF reinforced PPS
AM) system consists of a single screw extruder where the screw rotates was considered for this study. This research focuses on different infill
inside a heated barrel. The screw moves the material inside the barrel patterns within the 3D printed substrate and the effect of the fill pat-
feed section to the transition section where it is melted and transferred tern on the thermal conductivity and thermal expansion (warpage) of a
to a metering section. The material exits from a deposition nozzle under composite mold manufactured by the EDF-AM process. The molds were
pressure [25]. The flow kinematics of the fibers in the extruded bead heated through a conductive mechanism. The thermal effect (warpage of
is given in Fig. 1. Brenken et al. [26] reported that fibers are highly the mold) was monitored by comparing non-contact 3D digital imaging
aligned along the deposition direction at the wall of the nozzle due to of the molds before and after heating. Durability of mold was measured
high shear forces; however, are randomly oriented at the center of the by fabrication parts using extrusion compression molding (ECM).

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P. Yeole, S. Kim, A.A. Hassen et al. Additive Manufacturing Letters 1 (2021) 100007

Fig. 2. Schematic of 50CF-PPS printed dome-

shaped mold (a) male mold (b) female mold.
The molds were printed using BAAM with bead
width 13.97 mm (0.55”), and bead height: 5.08
mm (0.2”).

2. Materials and sample preparation 40% CF reinforced nylon 6 (40CF-PA6) pellets from Celanese were
used to fabricate parts from 50CF-PPS composite mold using extrusion
50% by weight CF reinforced polyphenylene sulfide (50CF-PPS) was compression molding (ECM) process. Impco B20 plasticator and Beck-
procured from Techmer PM. The melting point of PPS is 285°C, it is a wood – 100 tons hydraulic compression press was used for ECM pro-
semi-crystalline thermoplastic polymer with a high heat deflection tem- cess. The 40CF-PA6 parts were characterized by tensile test according
perature [38]. The BAAM extrusion system with 10.16 mm (0.4 in) noz- to ASMT 3039. FARO arm 3D scanner and Geomagic Control-X 2018
zle orifice diameter was used to print dome-shaped molds, as shown in software was used to monitor the degradation of the mold.
Fig. 2. The surface of the printed structure is beaded due to the nature of
the BAAM print, which leads to an extra post-processing step to obtain 3. Experimental setup
good quality surface. The mold was printed slightly bigger (2.54 mm)
than the target geometry using BAAM; then, machining was performed Each male mold was placed on the platen of the hydraulic compres-
to remove excess material and achieved the exact target surface finish. sion press (Beckwood – 100 tons) and subjected to conductive heating.
The BAAM screw extruder has five heating zones, and these were set as; Nine (9) thermocouples were placed on the mold surface and one on
zone 1: 305°C, zone 2: 321°C, zone 3: 326°C, zone 4: 337°C, zone 5 (tip): the platen to measure the temperature at various locations as shown in
337°C. The bead width: 13.97 mm (0.55”), and bead height: 5.08 mm Fig. 4. The temperature of the platen was maintained at 200°C (390°F),
(0.2”) was kept constant for all prints. The 3D printing was conducted by and the temperature profile for the mold surface was continuously moni-
using an acrylonitrile butadiene styrene (ABS) sheet to begin the print, tored for 5 hours. After 5 hours, the temperature reached an equilibrium.
and the bed temperature was maintained at 110°C to adhere to the ini- A baseline scan was performed at room temperature, and the second
tial layer. A thermal camera (FLIR A35) was positioned to monitor the scan was conducted at elevated temperature (after 5 hours) using a high
deposition temperature such that the interface temperature between the precision 3D measurement FARO arm. The arm consists of a FARO Laser
layers was always higher than the glass transition temperature (Tg ) of Line Probe (LLP), which provides non-contact 3D scanning capabilities.
PPS (85°C) [39]. The printing of 50CF-PPS was performed under inert The scans were compared and analyzed using Geomagic Control-X 2018
environment (argon), as extrusion under ambient temperature leads to software for dimensional variation. The experimental setup is shown in
significant accumulation of viscous material inside the extruder, which Fig. 4.
can degrade the polymer.
Perimeter (shell) 3D printing creates an external boundary added
4. Results and discussion
during part building as shown in Fig. 3. The perimeter is an essential
parameter for the uniform distribution of stresses to avoid premature
Heat conduction and warpage:
failure [40]. Every printed part should have at least one perimeter [32].
In this experiment, nine thermocouples were attached to the top sur-
Additional perimeters provide strength to the part; however, the in-
face of the mold using kapton tape to monitor/record temperature pro-
clusion of these perimeters also adds weight and leads to an increase
file. The position of thermocouple was shown in Fig. 4. These were K-
print in time. The infill pattern is the interior structure/geometry of the
type thermocouples, connected to the DAQ-system. The temperature dif-
printed cross-section (inside the perimeter). Infill density and geometric
ference between the three molds was attributed to the infill directions.
patterns have a significant effect on the mechanical performance of the
An extruded material has highly aligned fibers along the deposition di-
printed structure [41, 42]. As explained in Section 1, in BAAM printing,
rection, and therefore, the conductivity along the deposition direction is
fibers are aligned along the deposition direction. Therefore, the struc-
expected to be higher than in other directions [29]. Heat transfer in the
ture of the infill pattern is hypothesized to have significant influence on
mold was mainly in the direction from the bottom surface of the mold
the fiber orientation. The fiber orientation would therefore have an ef-
to the top surface of the mold. When the infill direction was parallel to
fect on the thermal conductivity and the warpage of the final part [43].
the heat transfer direction (0° infill), then due to the high conductivity
Three male molds were manufactured with three perimeters and dif-
along the heat transfer direction, the top surface held a high temper-
ferent infill patterns as shown in Fig. 2(a) The three molds feature an
ature (i.e., 79.2°C). When the infill direction was perpendicular to the
infill pattern of 0° (along the deposition direction), 90° (transverse to
heat transfer direction (i.e., 90° infill), then due to the low conductivity
the deposition direction) and 0°/90° (one layer along the deposition di-
along the heat transfer direction, the top surface held a low temperature
rection while the second transverse). The schematics of various infill
(i.e., 66.5°C). The average surface temperature of the 0°/90° infill pat-
patterns are shown in Fig. 3. Infill parameters: infill density: 50%, bead
tern mold was recorded as 73.6°C, in between 0° and 90° infill pattern
width: 12.7 mm (0.5”), extruder speed: 350 RPM.
molds.

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P. Yeole, S. Kim, A.A. Hassen et al. Additive Manufacturing Letters 1 (2021) 100007

Fig. 3. Infill pattern (a) 0° (b) 90° (c) 0°/90°. The bead width: 13.97 mm (0.55”) and bead.

Fig. 4. Mold placed on the platen (200°C) and

heated through conduction for 5 hours. Posi-
tion of thermocouples (position 1 to 10) repre-
sent the locations where the temperature was
recorded.

The reinforcing fibers aligned along the deposition direction leads Fig. 6 and Table 1 shows the three-dimensional (3D) deviation anal-
to non-uniform expansion of the printed structures [38]. Brenken et al ysis of 0°, 90°, and 0°/90° infill pattern molds for high-temperature scan
[44] studied the CTE variation of 50CF-PPS samples for large scale compared to room temperature scan. It was observed that average de-
BAAM structures in three principle directions and observed 2 × 10−6 flection was +0.385 / -0.244 mm representing total 0.314 mm for 0°,
m/(mK), 26.75 × 10−6 m/(mK) and 43.00 × 10−6 m/(mK) in X-, Y-, and +0.445 / -0.280 mm representing overall 0.363 mm for 90° and +0.397
Z-directions (representation of each direction is explained later in this / -0.262 mm representing total 0.329 mm for 0°/90° molds. Since the
section) respectively [45]. To understand the deflection/warpage of the deflection (due to heat) in all molds was carried out in Z-direction, and
mold due to heating, a 3D digital impression of the mold at room tem- the different infill patterns were presented in the X-Y plane, tempera-
perature and the elevated temperature was captured using a FARO arm. ture gradient (the temperature difference between the top and bottom
The scans were then accurately aligned and compared using Geomagic surface of the mold) was the main driving factor for the deviation. The
Control-X 2018 software. average temperature recorded (measured by 9 thermocouples placed as
The first layer for each mold was printed in the X-Y plane (0° infill shown in Fig. 4) at the mold top surface for 0°, 0°/90°, and 90°infill
in X-direction; 90° infill in Y-direction), and the three-dimensional mold pattern mold was 79.2°C, 73.6°C, and 66.5°C respectively. For each ex-
was fabricated by depositing successive layers in Z-direction. The infill periment, the platen temperature was kept constant (200°C). Therefore,
pattern in the X-Y plane holds the structure steady irrespective of the the temperature gradient between the bottom and top surface of the
infill lines. Therefore, it was observed from Fig. 5 that all molds were mold was highest in 90° infill followed by 0°/90° infill and least in 0°
warped in Z-direction only (positive deflection at the edges: green color, infill which correlate with the similar trend of deflection as 0° < 0°/90°
and negative deflection at the center: red color). < 90°.

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P. Yeole, S. Kim, A.A. Hassen et al. Additive Manufacturing Letters 1 (2021) 100007

Fig. 5. Aligned image of mold at room temperature and elevated temperature. All three molds showed similar pattern as warped along the Z-direction. Amount of
warpage was different for each mold.

Fig. 6. 3D deviation analysis of molds at room temperature and after keeping on heated (200°C) platen for 5 hours. Total average deflection for (a) 0°: 0.314 mm;
(b) 90°: 0.363 mm; (c) 0°/90°: 0.329 mm.

Table 1
Average top mold surface temperature and total average deflection for different infill pat-
terns.

Sr. No. Infill Pattern Avg. Top Surface Temperature (°C) Total AverageDeflection (mm)

1 0° 79.21 ± 6.48 0.314 ± 0.42

2 90° 66.45 ± 5.76 0.363 ± 0.46
3 0°/90° 73.60 ± 4.06 0.329 ± 0.42

Bagsik et al. [46] studied the compression behavior of extrusion long fiber thermoplastics)) can be a feedstock material for ECM. A hot,
printed samples build in vertical (0°) and horizontal (90°) direction. The molten charge is produced through extrusion which then transferred to
authors observed that the samples fabricated in the vertical direction the mold attached to hydraulic press. After the application of pressure,
failed with the bucking mode while horizontal direction samples failed charge flows to the desired shape of the mold. The details about ECM
due to interlayer shear. Similar results were observed by Motaparti et al. are given in [49-51]. The mold was mounted on the compression press,
[47]. The failure mechanism of the two orientations is shown in Fig. 7. and the platen heating was started. As shown previously (section 3.4.2),
Therefore, it can be assumed that a 0°/90° infill pattern has a more the mold warped upon heating. We believe that the mounting clamps
stable structure under compression due to alternate layers. The total de- constrained free motion of the tool and resulted in a crack at the cen-
viation of 0°/90° infill mold was only 4.8% higher than 0°. Also, 0°/90° ter, as shown in Fig. 8. To further explore the cracking and ways to
infill mold had more uniform heat distribution (standard deviation: ± eliminate it, a high-temperature epoxy 1096 obtained from FiberGlast
4.1 mm) as compared to the other molds. The non-uniform distribu- Development Corporation was used to fill the crack. The 1096 epoxy
tion of temperature may result in the uneven curing of composites [48]. is a thixotropic system. The two-part epoxy (1096) contains aluminum
Therefore, further efforts were made to characterize the performance of particles, and it is designed for high-temperature tooling applications.
0°/90° infill mold. A female mold with a 0°/90° infill pattern was fabri- The mold (after filling crack) was mounted back on the press, and heat
cated with the same processing conditions explained in Section 3.2 and was applied. After 5 hours, when the temperature reached equilibrium,
prepared for ECM operation. the mold was fixed using mounting clamps. The mold did not show any
crack after mounting.

5. Extrusion compression molding (ECM) with the 0°/90° infill

mold 5.2. Parts Fabrication

5.1. Mold Mounting The mold with a 0°/90° infill pattern was used to produce parts
using 40% by weight CF reinforced nylon 6 (40CF-PA6) pellets from
The 0°/90° infill mold was used for the ECM process. ECM process Celanese using the ECM process. Schematic of ECM process is given in
involves two main operations as extrusion and compression molding. Fig. 9. The molten charge was prepared using the Impco B20 plasticator
Any type of pellets (neat or reinforced (short fiber thermoplastics and where the heating zones were set to 257°C (495°F), 266°C (511°F), 277°C

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P. Yeole, S. Kim, A.A. Hassen et al. Additive Manufacturing Letters 1 (2021) 100007

Fig. 7. Failure mechanism of AM specimens under compression loading (a) Vertical direction (0°); (b) Horizontal direction (90°) (adapted from [46]).

Fig. 8. Failure (crack) in the 50CF-PPS additive manufactured mold due to application of pressure on heated warped mold (a) Male mold (b) Female mold.

Fig. 9. Schematic of ECM process.

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P. Yeole, S. Kim, A.A. Hassen et al. Additive Manufacturing Letters 1 (2021) 100007

Fig. 10. (a) Location of charge placed in the BAAM printed mold (b) the representative consolidated part of 40CF-PA6. The unfilled region on the consolidated part
due to the limitation of the plasticator to generate a bigger charge (Maximum charge length produced by plasticator was 304.8 mm).

Fig. 11. Deviation analysis of the two scans before and

after 20 parts fabrications. Maximum deformation was
observed at the 1096 epoxy region (blue area).

(530°F), 277°C (530°F) and charge size was maintained at 304.8 mm part; average tensile strength of 132.9 ± 11.6 MPa and modulus of 14.3
(12”) length × 50.8 mm (2”) diameter (this was the maximum charge ± 0.8 GPa was noted. Ning et al. showed that 18-35 % weight of CF
size possible with the Impco B20 plasticator). Three layers of McLube reinforced nylon 6 samples modulus varies from 6.5 - 14.7 GPa [52].
841 releasing agents were applied to the mold surface. The platen tem- From this, it can be concluded that the parts fabricated using AM mold
perature was maintained at 121°C (250°F), and the temperature at the were well consolidated.
mold surface was recorded to be in between 66°C – 71°C (150°F – 160°F)
(glass transition temperature of nylon 6). 5.3. Mold degradation
The hot charge from the plasticator was then placed on the mold,
as shown in Fig. 10 (a), and the part was prepared after the applica- A total of 20 parts were fabricated using the ECM process to deter-
tion of pressure. Initially, lower pressure was applied as 0.54 MPa (5 mine the durability of the mold. A 3D digital impression of the mold
tons) and prepared 10 parts. The pressure was increased to 0.86 MPa was captured by a laser scanner before and after 20 parts were fabri-
(8 tons), 1.3 MPa (12 tons), and finally 1.6 MPa (15 tons). Two panels cated. The two scans were aligned and compared using Geomagic Con-
were fabricated using 0.86 MPa and 1.3 MPa each while 6 panels using trol X-2018 software. Fig. 11 shows that the deformation occurred in
1.6 MPa pressure. It can be observed in Fig. 10 (b) that there were some the mold due to the manufacturing of 20 parts using 40CF-PA6. The av-
unfilled regions in the consolidated part. This was due to the limitation erage degradation of + 0.076 mm / – 0.093 mm was recorded. It can be
of the plasticator to generate a bigger size charge. Tensile samples were noticed that the maximum degradation was observed along the epoxy
extracted according to ASTM D 3039 standard from the flat region of region (blue color). This degradation was caused due to the flow of the

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P. Yeole, S. Kim, A.A. Hassen et al. Additive Manufacturing Letters 1 (2021) 100007

charge (40CF-PA6) at a high temperature, which created friction and [16] C. Pradere, C.J.C. Sauder, Transverse Longitud. Coeff. Thermal Expansion Carbon
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