Additive Manufacturing 32 (2020) 101102

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Additive Manufacturing
journal homepage: www.elsevier.com/locate/addma

Full Length Article

A mechanistic model for tensile property of continuous carbon fiber T

reinforced plastic composites built by fused filament fabrication
Fuji Wanga, Zhongbiao Zhanga, Fuda Ningb,*, Gongshuo Wanga, Chuanhe Donga
a
School of Mechanical Engineering, Dalian University of Technology, Dalian, 116023, China
b
Department of Systems Science and Industrial Engineering, State University of New York at Binghamton, Binghamton, NY, 13902, USA

ARTICLE INFO ABSTRACT

Keywords: Lightweight and high-strength continuous carbon fiber reinforced plastic (C-CFRP) composites have become
Continuous carbon fiber reinforced plastic (C- promising materials for aerospace, automotive, and sports applications. Recently, fused filament fabrication
CFRP) composites (FFF) technology enables the production of geometrically complex C-CFRP components that are difficult to
Material extrusion fabricate using conventional manufacturing processes. In this study, a novel mechanistic model to predict tensile
Fused filament fabrication
strength and elastic modulus of C-CFRP parts built by a co-extrusion based FFF process was developed for the
Mechanistic model
first time. The fiber-matrix impregnation behavior, physical gap ratio, and fiber orientation within the as-built C-
Tensile property
CFRP were also considered. In order to verify the model, C-CFRP parts were fabricated using different matrix
materials including PA, PC, PETG, PLA, and short carbon fiber reinforced PA (SCF/PA) for tensile testing. The
comparative results showed that the prediction errors for tensile strength and elastic modulus were less than 5 %
and 10 %, respectively. C-CFRP with the matrix of SCF/PA exhibited the largest tensile strength of 288.65 MPa,
while C-CFRP with PLA matrix possessed the highest elastic modulus of 29.12 GPa. This study provided an
insight into the material-process-impregnation-property relationship during co-extrusion based FFF of C-CFRP
components.

1. Introduction
Carbon fiber reinforced plastic (CFRP) composites have become one
of the most demanding and widely used structural materials in the
aerospace, automotive, wind energy, and sports fields due to their low
density, high strength, excellent fatigue resistance, and outstanding
corrosion resistance [1–4]. Typically, CFRP components used in these
applications possess geometrically complex structures. Traditional
molding processes (such as compression molding, injection molding,
etc.) are usually applied to fabricate CFRP to a near-net shape, which
would be followed by the subtractive processes. However, this ap-
proach results in high manufacturing cost and low production efficiency
[5]. On the other hand, welding and bolting the individual parts can be
another approach to build CFRP components with complex structures,
while such a joining method hardly meets the requirements of high
dimensional accuracy and also causes weak joints between every two
individual parts [6–8].
Fused filament fabrication (FFF), as one of the promising additive
manufacturing technologies, allows for the rapid manufacturing of
complex-structural parts without the need for expensive molds [9–11].
In recent years, FFF technology has been extensively utilized for
printing short carbon fiber reinforced plastic (S-CFRP) to enhance the
mechanical property of FFF-built pure plastic prototypes. The in-
vestigations of Ning et al. [12], Shofner et al. [13], and Tekinalp et al.
[14] have been mainly focused on the additions of short carbon fiber
with different contents and lengths into the pure ABS plastic and their
effects on the tensile and flexural properties (such as strength, modulus,
toughness, ductility, etc.) of the FFF-fabricated S-CFRP parts have been
studied. However, the findings of these works indicate a limited en-
hancement of mechanical behavior that is still below the requirements
of actual engineering applications.
In recent years, there is a growing interest in manufacturing con-
tinuous carbon fiber reinforced plastic (C-CFRP) using FFF process to
significantly address the restriction. Two types of method for additively
manufacturing of C-CFRP have been found in the literature, as shown in
Fig. 1. Type one is to extrude the matrix and continuous carbon fiber
separately from two individual nozzles using the MarkForged printer
(defined as “dual-extrusion”, as shown in Fig. 1a) [15–17], while type
two employs a single nozzle for the extrusion where the impregnation
between the matrix and fiber occurred inside (defined as “co-extru-
sion”, as shown in Fig. 1b) [18–22]. Mori et al. [23] compared these
two methods for FFF printing of C-CFRP parts. The comparative results

⁎
Corresponding author.
E-mail address: fning@binghamton.edu (F. Ning).

https://doi.org/10.1016/j.addma.2020.101102
Received 26 August 2019; Received in revised form 12 November 2019; Accepted 30 January 2020
Available online 31 January 2020
2214-8604/ © 2020 Elsevier B.V. All rights reserved.
F. Wang, et al.
Fig. 1. The FFF process of C-CFRP in (a) dual-extrusion and (b) co-extrusion
manners.
showed that the mechanical property achieved in the co-extrusion
process was almost twice that in the dual-extrusion process due to the
better fiber-matrix interfacial bonding. The works of Tian et al. [24]
and Liu et al. [25] indicated that gap existed among fibers, and the
fiber-matrix impregnation was not fully generated in the co-extrusion
based FFF. However, good impregnation could be achieved by properly
monitoring and controlling the quality during the co-extrusion process
[26]. In order to improve the fiber-matrix impregnation performance,
Tian et al. [27] proposed a recycling and remanufacturing process for
FFF of C-CFRP and then they experimentally verified the feasibility. The
results showed that the recycled-continuous carbon fibers could im-
prove fiber-matrix impregnation behavior, which further effectively
enhanced the mechanical properties. In addition, Li et al. [28] em-
ployed a pretreatment process to modify continuous carbon fibers using
polylactic acid sizing agent for the purpose of better fiber-matrix
bonding. Compared with the original C-CFRP parts, the modified ones
were proved to possess the increased tensile strength and flexural
strength by 13.8 % and 164 %, respectively. Yamawaki et al. [18] and
Mei et al. [29] treated the FFF-fabricated C-CFRP parts using hot
pressing and they found that the fiber-matrix impregnation perfor-
mance was improved, resulting in the significant improvement of ten-
sile strength and elastic modulus. It can be concluded from the litera-
ture that the impregnation behavior plays a significant role in
determining the mechanical properties of FFF-built C-CFRP parts.
On the other hand, investigation on the prediction of mechanical
properties of FFF-fabricated C-CFRP parts is still in its infancy. Juan
et al. [16] proposed a modified rule-of-mixtures (ROM) method to
predict elastic modulus of C-CFRP composites built by dual-extrusion
based FFF process. The errors between experimental results and pre-
dicted ones were 11 % and 33 % when the fiber content was 1 % and 60
%, respectively. Yu et al. [30] used the dual-extrusion based FFF pro-
cess to fabricate C-CFRP with concentric and isotropic filling patterns
and employed a stiffness averaging method to predict the elastic
modulus of C-CFRP. The average error in this work turned out to be
around 20 %. The aforementioned investigations were relevant to the
2
Additive Manufacturing 32 (2020) 101102
mechanical property prediction in C-CFRP built by the dual-extrusion
based FFF process rather than the co-extrusion type. The mechanical
property prediction considering fiber-matrix impregnation behavior
was thus overlooked, failing to uncover the underlying mechanism in
co-extrusion based FFF process of C-CFRP parts.
In this paper, for the first time, we develop a novel mechanistic
model to predict mechanical properties (tensile strength and elastic
modulus) of C-CFRP built by the co-extrusion based FFF. Fiber-matrix
impregnation behavior, fiber orientation coefficient, and physical-gap
between fibers are considered in this model to disclose influences of
impregnation phenomenon on the mechanical properties. In order to
verify the theoretical model, C-CFRP composites with different matrix
(including PA, PC, PETG, PLA, and SCF/PA) are fabricated individually
in the experiments. After that, the optical microscope and scanning
electron microscope are used to observe the cross-sectional morphology
of printed parts. Moreover, image processing techniques are employed
to better quantitatively characterize the impregnation phenomenon. A
universal tester is utilized to experimentally measure tensile properties
for the comparisons with the predicted values. This paper can provide
an insight into the relationship among polymer material, process, im-
pregnation behavior, and mechanical property during co-extrusion
based FFF of C-CFRP composite parts.
2. Theoretical model development
2.1. Approach to model development
In this work, the established model can be used to predict both
tensile strength and elastic modulus based on given input variables
including matrix material property, carbon fiber performance, and FFF
process parameters. The main approach to develop this mechanical
property prediction model involves theoretical calculations and ex-
perimental measurements. The specific modeling procedure for pre-
dicting tensile strength and elastic modulus is organized in Fig. 2.
Apart from the known value of Ef, the strength f 1 and f 2 of the
carbon fiber will be calculated based on the fiber fracture analysis in
Sections 2.4 and 2.5. The intermediate variables including k as well as
Vg , Vf 1, and Vf 2 in the C-CFRP sample fabricated by FFF process can be
obtained by the function of Fast Fourier Transform (FFT) and image
processing technology, respectively, as illustrated in Section 3.4. In
addition, m* and Em of the C-CFRP with different matrix materials will
be measured and the result is shown in Section 4.3. Finally, all the
variables can be integrated into the mechanistic model to predict the
ultimate tensile strength and elastic modulus of C-CFRP part fabricated
by this AM technology.
2.2. Assumptions in model development
In this study, several reasonable assumptions about conditions for
fiber property analysis in model development are proposed as follows:
(1) The monofilament in the carbon fiber bundle is identical to each
other;
(2) The strands are uniformly distributed in the final C-CFRP part;
(3) Tensile load is generated in the axial direction of the carbon fiber
regardless of the radial direction;
(4) The impregnated carbon fiber will not debond from the matrix;
(5) The site where carbon fiber subjected to the stress concentration
will become the point of failure.
2.3. Overall analysis of tensile strength and elastic modulus
According to the classic rule of mixture (ROM), tensile strength and
elastic modulus of the unidirectional C-CFRP composite can be typically
expressed by [32]:
F. Wang, et al. Additive Manufacturing 32 (2020) 101102

Fig. 2. Modeling procedures for predicting tensile strength and elastic modulus.

c = f Vf + *
m (1 Vf ) gap conditions, fiber orientation, and impregnation behavior. There-
Ec = Ef Vf + Em (1 Vf ) fore, the ROM has been modified accordingly in Eq. (2) to obtain the
(1)
expressions for the tensile strength and elastic modulus of the specific
FFF-fabricated C-CFRP samples:
where, c and f are the tensile strength of C-CFRP and carbon fiber,
respectively; m* represents the matrix stress at the failure strain of the = f 1 Vf 1 + f 2 Vf 2 + *
c m (1 Vf 1 Vf 2 V g)
carbon fiber; Vf is the volume fraction of carbon fiber; Ec , Ef , and Em
Ec = kEf (Vf 1 + Vf 2) + Em (1 Vf 1 Vf 2 Vg ) (2)
are the elastic modulus of C-CFRP composite, carbon fiber, and matrix,
respectively.
where, indexes of 1 and 2 denote unimpregnated carbon fiber and
Fig. 3 illustrates the morphologies of the single composite strand
impregnated carbon fiber, respectively. Vg represents the gap ratio
and its fiber-matrix impregnation behavior. The bundle of loose carbon
within the extruded strand and k is the fiber orientation coefficient,
fibers, as reinforcing feedstock materials for C-CFRP fabrication, is
both of which will be measured in Section 3.4. It can be seen from Eq.
shown in Fig. 3a. It is notable that some portion of the monofilaments is
(2) that the existence of unimpregnated fiber, impregnated fiber, phy-
misaligned due to the lack of sufficient tension, which may lead to the
sical gap, and fiber orientation factors within the FFF-fabricated C-
reduction of the axial load-bearing capability of the carbon fiber in the
CFRP samples have been considered and involved in the calculation for
FFF-built C-CFRP composite part. In order to better quantitatively
both tensile strength and elastic modulus.
characterize unidirectional tensile properties of the carbon fiber, fiber
orientation coefficient k is proposed to achieve the effective load-
bearing components of fibers along with the printing direction, and its 2.4. Tensile strength f1 of unimpregnated carbon fibers
mathematical meaning is the cosine value of the average angle between
the actual fibers and the printing direction, which will be measured in Unimpregnated carbon fiber bundle consists of many independent
Section 3.4. monofilaments, and the probability of monofilament fracture obeys the
In addition, differing from the conventional unidirectional CFRP, Weibull distribution [33]:
the FFF-fabricated C-CFRP composite contains a certain amount of f
unimpregnated carbon fibers, as shown in Fig. 3b. The carbon fibers F ( f) = 1 exp[ L( ) ]
0 (3)
completely infiltrated by the matrix material are defined as im-
pregnated carbon fibers, and the remaining fibers in the bundle are where, is the probability of fiber failure in the range of the stress lower
treated as unimpregnated carbon fibers. The unimpregnated and im- than f ; L is the ratio between the fiber clamped length l and a reference
length l 0 (L = l ); 0 is the average tensile strength of a monofilament,
l
pregnated carbon fibers must be considered as two different phases due
0
to the involvement of matrix. Thus, the tensile strength of unim- and is the shape parameter.
pregnated and impregnated carbon fibers will be separately calculated. For a bundle of unimpregnated carbon fibers composing of i carbon
It can also be found in Fig. 3b that physical gaps exist within the carbon fiber monofilaments, the tensile strength and offset angle of the ith
fiber bundle. The elastic modulus of carbon fiber is an inherent prop- (1≤i≤n) fiber are expressed by x i and i , respectively. Thus, the hor-
erty, while the ultimate tensile strength of fiber changes with internal- izontal component of tensile strength of the monofilaments, from the

Fig. 3. Schematic of (a) top view and (b) cross-sectional view of FFF-fabricated C-CFRP part.

3
F. Wang, et al. Additive Manufacturing 32 (2020) 101102

smallest to the largest, is sorted as follows: always be aligned with the axis, causing the fibers with different offset
angles to present varied strengths during the tensile test. In this work,
x1 cos 1 … xi cos i … xn cos n (4)
the fiber is offset by a certain angle in order to ensure that the model
Due to the external load, the weakest fiber breaks first, and the well matches with the actual conditions, as shown in Fig. 5. When a
remaining n-1 fibers evenly bear the load. As the load increases, the single fiber breaks, the shear stress is then transmitted through the
second weakest fiber continues to break, and the load is evenly dis- matrix, and the fiber nearby the fractured fiber endures larger load
tributed again. Then the fiber fracture process continues until the induced by the concentrated stress.
strongest carbon fiber finally breaks, achieving the maximum strength As shown in the magnified region in Fig. 5, the broken and un-
of the carbon fiber bundle. Hence, the tensile strength of unim- broken fibers are numbered as a and b, respectively. The shear stress
pregnated carbon fibers can be expressed by: acts on the cylindrical surface of the fiber, while the tensile stress acts
n+1 i 1 on the cross section of the fiber. Thus, the equilibrium equation of the
Xn' = max{x1 cos 1, ···, x i cos i , ···,( ) x cos n} fiber along the axial direction x can be expressed by:
n n n (5)
In Eq. (5), it is difficult to determine the exact distribution function rd a
a =0
of . In order to characterize the influence of fiber offset phenomenon, 2 dx
the overall offset of the fiber bundle rather than the offset calculation of d
r b + b =0
every single monofilament is used. Therefore, Eq. (5) can be simplified dx (14)
to: where, a and b represent the axial tensile stresses on the fibers a and b,
n+1 i 1 respectively; a and b are the shear stresses on the surface of fibers a
Xn' = max{x1, ···, x i , ···,( ) x }cos o = Xn cos o and b, respectively.
n n n (6)
In areas far from carbon fiber fracture, the load in the axial direction
where, cos o is the average offset of the overall unimpregnated carbon is evenly shared by each monofilament [38]. Thus,
fiber monofilaments, which is defined as the fiber orientation coeffi-
' ' '
cient k in this work (cos o = k ). a cos a = b cos b = f (15)
Daniel [34] has demonstrated that when n tends to be infinite, the
where, a and b is the offset angles of fibers a and b, respectively.
tensile strength of the unimpregnated carbon fiber bundle is subjected
According to the Hooke’s law, the axial displacement within the
to the following normal distribution:
fiber is ordered as u, then, tensile and shear stresses can also be ex-
1 (Xc X¯ c )2 pressed by:
f (X c ) = exp
S 2 2S 2 (7)
dua (x )
= Ef
where, the average tensile strength of unimpregnated carbon fiber
a
dx
bundle X̄c and the square error S can be expressed by: dub (x )
b = Ef
dx (16)
X¯ c = Xm [1 F(Xm )] (8)
G
Xm F (Xm )[1 F (Xm )] b = [ub (x )cos b ua (x )cos a]
S= h
n (9)
b cos b = a cos a (17)
In both equations, F (Xm ) is a probability distribution function of the
monofilament strength; Xm is the stress of the monofilament, which can where, Ef is the elastic modulus of the fiber, G is the shear modulus of
be determined by: the matrix, h is the spacing distance between fibers, and r is the fiber
radius.
d {X [1 F(X )]} By substituting Eqs. (16) and (17) into Eq. (14), the following
=0
dX X = Xm (10) equilibrium equation can be obtained:
Since it has been assumed that the strength of monofilament is cos a rEh d 2ua cos a
subjected to the Weibull distribution in Eq. (3), the average strength of ub + ua =0
cos 2 b G dx 2 cos b
monofilament can be obtained by substituting Eq. (3) into Eqs. 2
rEh d ub
(7)–(10): 2 + ubcos b ua cos a = 0
G dx 2 (18)
Xm = 0 (l /l 0) 1/
(11)
After simultaneously combining Eq. (18) with Eq. (15), the axial
After substituting Eq. (11) to Eq. (8), X̄c can be obtained as: tensile stresses of carbon fibers a and b can be obtained as:
X¯ c = 0 (l /l 0 ) 1/
(12) '
f 3cos b G
x
a = (1 e rEh )
Then, the tensile strength of the unimpregnated carbon fibers con- cos a
sidering the fiber orientation coefficient can be expressed by: '
f 1 3cos b G
x
b = (1 + e rEh )
¯c = k
f 1 = kX 0 (l e/ l 0) 1/
(13) cos b 2 (19)
According to Eq (19), when the deformation x of the fiber b turns
2.5. Tensile strength f2 of impregnated carbon fibers out to be 0, the fiber b is subjected to the maximum tensile stress b .
Moreover, by substituting Eq. (15) into Eq. (19), the maximum stress
For the C-CFRP sample, the ductility of the plastic matrix is larger concentration factor of the model can be acquired as follow:
than that of carbon fiber, so the impregnated carbon fiber will break
( b/ b' ) x = 0 = 3/2 (20)
first when the C-CFRP is subjected to the axial tensile load. The shear-
lag model [35–37] has been widely used to analyze the mechanism of Since the area of the fiber b adjacent to the fracture of the fiber a
load transmission in this condition based on the hypothesis that the experiences a larger load, this portion is more likely to get fractured.
fibers evenly and vertically distribute, as shown in Fig. 4. The tensile strength of the impregnated carbon fibers can be thus
However, the orientation of the fibers in the composite would not achieved when the impregnated fiber b is capable of bearing the load

4
F. Wang, et al. Additive Manufacturing 32 (2020) 101102

Fig. 4. Schematic of the elements within a traditional C-CFRP material for shear-lag analysis.

Table 1
Properties of carbon fiber monofilament.
Property Value

Diameter 7 μm
Density 1.76 g/cm3
Average tensile strength 0 3580 MPa
Elastic modulus Ef 230 GPa
Shape parameter 8.3
Reference length l0 8 mm

and SCF/PA (PA reinforced by 25 wt.% short carbon fibers with a

diameter of 3∼10 μm) filaments with 1.75 mm in diameter (isun3d
Tech Co., Shenzhen, China). In addition to their differences in me-
chanical properties, they exhibited varied values of viscosity coeffi-
cient, permeability, flow velocity, shear rate, etc., affecting the fiber-
Fig. 5. Schematic of the elements within FFF-fabricated C-CFRP for shear-lag matrix impregnation behavior, which could eventually lead to the dif-
analysis. ferent values of part strength and stiffness.

under such a stress concentration effect. Thus, 3.2. Experimental setup for C-CFRP fabrication
' 2
= = b cos Fig. 6 shows an FFF desktop printer built in house for the C-CFRP
f2 f
3
b
(21)
fabrication. Both matrix material and carbon fiber bundle were si-
As carbon fiber b is a specific fiber presented in Eq. (21), for any multaneously fed into the co-axial extrusion head from two individual
arbitrary impregnated carbon fiber, the general expression of its tensile inlets. Then, the nozzle extruded both matrix material and carbon fiber
strength can be obtained by: along the path on the printing platform, and meanwhile, the matrix
n n
cos i material was impregnated into carbon fiber mainly due to the nozzle
2 i=1 i i=1 2 2
f2 = = 0 cos 0 = k 0
(22) squeezing action, forming a single strand of C-CFRP.
3 n n 3 3
Rectangular C-CFRP bars were fabricated using an FFF desktop
As mentioned in Section 2.1, after measuring and obtaining other printer built in house. The most important FFF process parameters for
intermediate variables, the tensile strength and elastic modulus of C- controlling the amount of extruded materials include printing speed,
CFRP part can be finally achieved by substituting Eqs. (13) and (22) layer thickness, and raster width, which should be determined based on
into Eq. (2). the designed C-CFRP sample size. FFF process parameters for C-CFRP
part fabrication in this work are shown in Table 2. During the co-ex-
3. Experimental conditions trusion based FFF of C-CFRP parts, the printer employed a strategy of
continuous forming of carbon fiber to allow for a continuous deposition
3.1. Materials without breakpoint jumping process between each two consecutive
layers. The printing trajectory adopted in this work is shown in Fig. 7,
In this paper, the continuous carbon fiber bundle was Toray T300- where the C-CFRP samples were created in a concentric-infill pattern.
1000 (Liyang New Material Technology Co., Cangzhou, China) con- During the fabrication, the sum of the material volumes of the fibers
taining 1000 monofilaments. The specific parameters of carbon fiber and the matrix fed into the nozzle should be identical to the volume of
monofilament are shown in Table 1. The distribution parameters of T- the extruded material. Thus,
300 carbon fiber monofilament, such as average tensile strength, shape
S1 v1 + S2 v2 = hbv3 (23)
parameter, and reference length were obtained [39]. In order to verify
the theoretical model above, five common matrix materials were se- where, S1 and S2 are the cross-sectional area of fiber and matrix, re-
lected for the C-CFRP part fabrication, including PA, PC, PETG, PLA, spectively; v1 and v2 are the feed rate for fiber and matrix, respectively;

5
F. Wang, et al. Additive Manufacturing 32 (2020) 101102

Fig. 6. The FFF experimental set-up for C-CFRP fabrication with (a) an overall FFF equipment and (b) the enlarged co-axial extrusion head structure.

Table 2
FFF process parameters for C-CFRP part fabrication.
Parameters Values

Nozzle diameter 1 mm
Layer thickness 0.3 mm
Raster width 1 mm
Printing speed 270 mm/min
Nozzle temperature 200℃/PLA
240℃/PETG
250℃/PC
250℃/PA
250℃/SCF/PA

Fig. 8. Tensile testing of the FFF-built C-CFRP sample.

Fig. 7. Concentric infill pattern of FFF-built C-CFRP sample.
h is the layer thickness; b is the raster width; and v3 is the printing
speed.
As the continuity of the carbon fiber should be ensured during the
FFF process, the fiber feed rate v1 would have to be consistent with the
printing speed v3 (v1 = v3 ). Furthermore, the volumetric percent (Vf) of
reinforcing carbon fiber is equal to the proportion of fiber area in the
overall cross-sectional area of an extruded C-CFRP strand.
S1 d 2 250
Vf = = × 100%
hb hb
By Eq. (24), it can be calculated that all FFF-fabricated C-CFRP samples
contain an approximately identical Vf of 12.83 %.
3.3. Tensile test
In this work, the rectangular C-CFRP bars were fabricated referring
to the dimensions in the standard of ISO 527-4:1997 [40], which pos-
sessed a size of 150 × 15 × 2.4 mm for the tensile testing. As shown in
Fig. 8, a universal testing machine (WDW-100E, Jinan Wenteng Test
Instrument Co., Ltd, China) was utilized to measure the tensile
properties of the C-CFRP samples. For each test, three samples were
measured to obtain an average value of the tensile properties. A testing
speed of 2 mm/min and the clamping length l of 90 mm were applied
during the tensile test. In addition, tensile samples of matrix materials
including PA, PC, PETG, PLA, and SCF/PA were fabricated and mea-
sured to obtain the values of m* and Em . The tensile testing exactly
followed the standard of ASTM D638-14 [41] with the overall sample
dimensions of 165 × 19 × 3.2 mm.
3.4. Experimental measurements
3.4.1. Measurement of fiber orientation coefficient k
In order to characterize the fiber orientation coefficient k, a single
strand of C-CFRP was printed. The strand samples with each matrix
material were observed using an optical microscope with super-high
magnification (VHX-600, Keyence Co., Osaka, Japan). In order to ac-
(24)
curately measure k, each strand sample was cut into five segments for
robust statistical calculation.
Fig. 9 shows the measurement procedures for quantitatively char-
acterizing fiber orientation coefficient k using the image processing
technology. Specifically, a two-dimensional Fast Fourier Transform
(FFT) function in the ImageJ software was firstly employed to extract
the fiber orientation distribution pattern in the captured micrographs of
the strand samples, and then the “Oval_profile” tool in the software was
used to measure the fiber orientation direction [42]. For example, for
those carbon fiber monofilaments arranged along the horizontal di-
rection in Fig. 9(c), the gray value of the image slightly changed along

6
F. Wang, et al. Additive Manufacturing 32 (2020) 101102

Fig. 9. Analysis of carbon fiber orientation. (a) A single strand of FFF-fabricated C-CFRP, (b) Enlarged zone showing carbon fibers with various orientations, (c) An
originally captured image, (d) FFT-processed image.

the direction of the monofilament, causing a bright vertical line in the Table 3
spectrogram, as shown in Fig. 9(d). Such a phenomenon was ascribed to Normalization process to obtain fiber orientation coefficient k.
the generation of grayscale gradient during the rendering of the digital A B C D E F
image spectrogram. Taking the center of Fig. 9(d) as the origin, a radial
line would be drawn at an interval of 0.36°, thereby producing 1000 θ(°) Gray value Min B B-C D/sum(D) E × sinA
lines within the circle. Then, the total gray value on each radial segment 45 58215.531 57488.215 727.316 0.000861311 0.000609039
45.36 58121.586 57488.215 633.371 0.000750059 0.000533694
would be calculated. The statistical distribution of all gray values 45.72 58060.543 57488.215 572.328 0.00067777 0.00048524
containing fiber arrangement information at the angle range from 0° to …
360° could be thus generated, which would be further utilized to obtain 89.64 65555.164 57488.215 8066.949 0.009553145 0.009552957
the value of fiber orientation coefficient k. 90 66375.500 57488.215 8887.285 0.010524614 0.010524614
90.36 65847.125 57488.215 8358.910 0.009898895 0.009898700
Fig. 10 illustrates the distribution of all the gray values at degrees from
…
0°to 360°. The major peaks were found at 90° and 270°, while the minor 134.28 58875.035 57488.215 1386.820 0.001642318 0.001175795
ones showed up at 0° and 180°. In Fig. 10, Regions I and II represented the 134.64 58523.769 57488.215 1035.484 0.001226254 0.000872524
degrees from 45° to 135° and that from 135° to 225°, respectively, and 135 58549.449 57488.215 1061.234 0.001256748 0.000888655

Region I was selected to acquire the fiber orientation coefficient k due to

the positive orientation of carbon fiber. Table 3 shows the normalization
process to obtain k value. The minimum gray value (column C) in Region I
was considered as the reference value, and after further data processing in
columns D and E, the proportion of fiber orientation at each degree could
be obtained in column F. Finally, the sum of all the values in column F was
the value of fiber orientation coefficient k.

3.4.2. Measurement of volumetric variables

Fig. 10. Illustration on the distribution of all the gray value values at degrees
from 0°to 360°.
The as-built tensile test samples of C-CFRP were sectioned by a
diamond wire cutter (STX-202AQ, Kejing Auto-instrument Co.,
Shenyang, China) with a diameter of 0.25 mm to measure the volu-
metric variables including the gap ratio within the extruded strand Vg ,
the volume fraction of unimpregnated carbon fibers Vf 1, and volume
fraction of impregnated carbon fibers Vf 2 . The tensile samples with each

7
F. Wang, et al.
Fig. 11. Cross-sectional morphology of FFF-fabricated C-CFRP part with (a) an original SEM image, (b) impregnation phenomenon, and (c) image processing
procedures.
Fig. 12. Fiber orientation coefficient k of C-CFRP with different matrix mate-
rials.
matrix material were observed using a scanning electron microscopy
(SEM) (Q45, FEI Co., Hillsboro, OR, USA). In order to accurately
measure these variables, five different cross-sectional areas of the ten-
sile sample were selected for the statistical calculations. The specific
impregnation behavior within the FFF-fabricated C-CFRP sample is
shown in Fig. 11(a) and Fig. 11(b), where the physical gap existing
within the carbon fiber bundle as well as impregnated and unim-
pregnated carbon fiber monofilaments can be observed. Fig. 11(c) de-
picts the overall image processing procedures using the binarization
method with different thresholds to obtain the volumetric variables. It
8
Additive Manufacturing 32 (2020) 101102
Fig. 13. Experimental results of all the volumetric variables of C-CFRP with
different matrix materials.
can be seen that the boundary of the unimpregnated fiber zone was
firstly extracted in step 2 from the to-be-processed image in step 1.
Then, Vg can be obtained by calculating the ratio of black pixel amount
in step 3 to the total pixel number of the extruded C-CFRP strand. In
addition, the difference in the amount of black pixels between the last
two steps can be considered as the pixels for unimpregnated fibers,
thereby achieving the value of Vf 1 through calculating the ratio of the
pixel difference to the total pixel number of the extruded C-CFRP
strand. Then, Vf 2 can also be obtained with the known values of Vf 1 and
Vf .
F. Wang, et al. Additive Manufacturing 32 (2020) 101102

Fig. 14. Representative stress-strain curves of the tensile samples fabricated by matrix materials (a) without and (b) with continuous carbon fiber reinforcements.

Table 4
Tensile properties of FFF-fabricated matrix materials and C-CFRP with different matrix materials.
Materials C-CFRP Pure matrix

Ultimate tensile strength (MPa) Elastic modulus (GPa) Failure strain (%) Elastic modulus (GPa)
m (MPa)
*

PA 252.36 ± 3.21 26.68 ± 0.20 0.880 23.05 1.88 ± 0.07

PC 238.85 ± 3.82 26.28 ± 0.19 0.875 15.98 1.58 ± 0.09
PETG 256.04 ± 5.54 28.21 ± 0.22 0.908 18.80 1.75 ± 0.06
PLA 277.11 ± 4.76 29.12 ± 0.15 0.901 33.72 2.63 ± 0.06
SCF/PA 288.65 ± 5.33 28.97 ± 0.17 0.958 29.90 2.51 ± 0.05

4. Experimental results and model verification Vr n 1

4.1. Fiber orientation coefficient acquisition
All the fiber orientation coefficients in the C-CFRP with different
matrix materials are demonstrated in Fig. 12. It can be seen that both
CCF/PLA and CCF/SCF/PA exhibited a larger average fiber orientation
coefficient (94.4 %) than the other three types of samples, which in turn
would contribute to a better axial load-bearing performance of the part.
Such a phenomenon could be explained by the matrix viscosity. The
fibers impregnated in the matrix were stretched by the tension action of
the solidified C-CFRP while being subjected to the resistance of the
matrix materials. Due to the lower viscosity of SCF/PA and PLA, they
exhibited less resistance to the fibers causing more easily straightened
fibers. In addition, it was worth noting that CCF/PC showed the smal-
lest average fiber orientation coefficient of 92.2 %, however, the dif-
ferences of fiber orientation coefficient among all these five types of C-
CFRP were not significant, as the tension action dominated the
straightening effect of carbon fibers.
4.2. Obtaining values of volumetric variables
As aforementioned, different matrix materials possessed various
values of viscosity coefficient, permeability, flow velocity, shear rate,
etc. During the fiber-matrix impregnation process, the flow of the
molten resin follows Darcy’s law, as shown in Eq. (25).
Kr dp
Vr =
dr
where, Vr is the flow velocity of molten matrix along the radial direc-
tion of the fiber tow, Kr is the permeability along the radial direction of
the fiber tow, η is the viscosity coefficient of the molten matrix, and dp
dr
is the pressure drop in the radial direction of the fiber tow. When the
power-law fluid flows in a porous media, the value of viscosity affected
by shear rate can be described by:
n 1
=m
2R (26)
where, is the effective dimensionless shear rate in the fibrous
medium, n and m denote the power-law exponent and the fluid con-
sistency, respectively. Within an infinitesimal time period for the nozzle
squeezing action, Eq. (25) can be represented by:
Kr dp K p
Vr (t ) = = r
dr r (t ) (27)
where, Vr(t) is the instantaneous flow velocity of molten matrix along
the radial direction of the fiber tow, r(t) is the real-time impregnation
distance of the molten matrix to the fiber tow, and t is the squeezing
time of nozzle to the single composite strand.
Thus, it can be seen from Eqs. (25)–(27) that the rheological para-
meters of matrix materials significantly affect the fiber-matrix im-
pregnation behavior. Such a difference would be manifested by the
volumetric variables including Vg , Vf 1, and Vf 2 that represented the
impregnation degree in this work, which could eventually produce
different modeling results.
The measuring results of all volumetric variables are shown in
Fig. 13. It can be seen that CCF/PLA achieved the lowest mean Vg of
3.68 % and the highest mean Vf 2 of 8.39 %. PLA matrix turned out to
easily penetrate into the physical gaps within carbon fiber bundle as
such a polymer possessed lower viscosity and the binding of its mac-
romolecular chains could be attenuated at the heated state. This
property led to the reduction of physical gap and improvement of im-
pregnated fiber volume fraction in CCF/PLA. On the other hand, CCF/
(25) PC samples showed the highest mean Vg of 6.43 % and the lowest mean
Vf 2 of 4.66 %. It could be thus considered that the matrix materials
significantly affected the physical gap within the fiber bundle as well as
fiber-matrix impregnation behavior. In addition, the measuring results
revealed that the increase of Vg led to an increase in Vf 1 and, of course, a
decrease in Vf 2 due to the constant overall fiber content Vf . The gap was
enlarged by the absence of the flowing matrix materials so that fewer
fibers were impregnated with the matrix materials.

9
F. Wang, et al. Additive Manufacturing 32 (2020) 101102

Fig. 15. Fractured cross-section of (a) CCF/PA, (b) CCF/PC, (c) CCF/PETG, (d) CCF/PLA, and (e) CCF/SCF/PA after tensile testing.

Fig. 16. Comparison of (a) ultimate tensile strength and (b) elastic modulus between experimental results and theoretical results.

4.3. Tensile property of C-CFRP and matrix materials
Representative stress-strain curves of the tensile samples
fabricated by matrix materials without and with continuous carbon
fiber reinforcements are shown in Fig. 14(a) and Fig. 14(b),
respectively. Their corresponding mean values and standard
deviation of tensile strength and elastic modulus are presented in
Table 4.
Fig. 14(a) indicated that the PA matrix owned the largest ductility of
17.2 %, while PLA plastic exhibited the smallest one of only 1.93 %.

10
F. Wang, et al.
Table 5
Experimental results and theoretical results of FFF-fabricated C-CFRP.
Materials Ultimate tensile strength
Experimental results (MPa) Theoretical results (MPa)
CCF/PA 252.36 ± 3.21 259.83
CCF/PC 238.85 ± 3.82 247.61
CCF/PETG 256.04 ± 5.54 267.53
CCF/PLA 277.11 ± 4.76 285.99
CCF/SCF/PA 288.65 ± 5.33 279.25
Fig. 17. Carbon fiber status before and after the tension action.
The failure strain of all matrix materials was significantly larger than
that of the associated C-CFRP specimen (less than 1 %, as shown in
Fig. 14(b)), suggesting the correct assumption for the model develop-
ment that the fiber fractured first when the C-CFRP was subjected to the
axial tensile load. Experimental results showed that the largest tensile
strength (288.65 MPa) was achieved by CCF/SCF/PA, whereas the
smallest one was seen in the CCF/PC sample with an average value of
238.85 MPa. On the other hand, CCF/PLA possessed the largest average
elastic modulus of 29.12 GPa, and CCF/PC again was the specimen
containing the smallest elastic modulus of 26.28 GPa. It could be ob-
served that the type of matrix material exerted a significant effect on
the ultimate tensile strength and elastic modulus of C-CFRP. In addi-
tion, the matrix stress m* of each related material at the failure strain
(ductility) of the C-CFRP can be then calculated, as listed in Table 4. As
aforementioned, the measured matrix stress and elastic modulus of
matrix materials would be used to predict the theoretical values of
tensile strength and elastic modulus of FFF-fabricated C-CFRP.
4.4. Fractural analysis
Fractural analysis on the cross-section of all C-CFRP samples was
conducted using SEM observation, as shown in Fig. 15. It is notable
that the fibers in the CCF/PA were not well bonded with the matrix, as
indicated by the smooth surfaces of some fibers with barely attached
matrix materials. Additionally, fiber-matrix impregnation behavior in
CCF/PC was hardly seen, and a large number of unimpregnated fibers
were pulled out of the matrix with remarkable void formation. These
phenomena evidenced the results that CCF/PC showed the lowest UTS
and elastic modulus. CCF/PETG had a relatively larger amount of
impregnated fibers but still experienced significant unimpregnated
fiber pull-out. On the other hand, the fiber-matrix impregnation in
CCF/PLA and CCF/SCF/PA was relatively better with less im-
pregnated fiber pull-out, indicating that the continuous carbon fibers
in these two materials had a larger bonding strength with the matrix.
The fractography observation provided evidence for the experimental
findings that CCF/PLA and CCF/SCF/PA possessed the larger UTS and
elastic modulus.
Additive Manufacturing 32 (2020) 101102
Elastic modulus
Prediction error (%) Experimental results (GPa) Theoretical results (GPa) Prediction error (%)
2.87 ± 1.24 26.68 ± 0.40 28.88 8.23 ± 1.39
3.53 ± 1.54 26.28 ± 0.38 28.48 8.36 ± 1.33
4.29 ± 2.07 28.21 ± 0.45 28.95 2.63 ± 1.55
3.10 ± 1.66 29.12 ± 0.31 30.05 3.19 ± 1.03
−3.36 ± 1.91 28.97 ± 0.34 29.91 3.23 ± 1.14
4.5. Model verification
After obtaining the variables including k, Vg , Vf 1, Vf 2 , m* , and Em in
previous sections, the theoretical results of both ultimate tensile strength
(UTS) c and elastic modulus Ec of C-CFRP were finally achieved.
Comparisons on c and Ec between experimental results and theoretical
data are shown in Fig. 16(a) and Fig. 16(b), respectively. The specific
values and prediction errors are also listed in Table 5. The comparative
results on UTS indicated a good match between the experimental and
theoretical results, as evidenced by the absolute average value of pre-
diction errors ranging from 2.87 % to 4.29 % only. Moreover, all the C-
CFRP materials exhibited a larger theoretical UTS than the experimental
one, except for CCF/SCF/PA which produced an average theoretical UTS
result with a 3.36 % lower value. On the other hand, the predicted elastic
modulus values agreed well with the trend of experimental ones along
with different matrix material compositions. It can be seen that CCF/
PETG, CCF/PLA, and CCF/SCF/PA exhibited minor discrepancy with the
prediction error of only about 3 %, while CCF/PA and CCF/PC generated
an average prediction error of 8 %. In addition, all the theoretical results
of elastic modulus were larger than the experimental ones.
The larger theoretical results of UTS and elastic modulus could be
due to the low content of impregnated fibers in FFF-built C-CFRP.
Fig. 17 illustrates the carbon fiber status before and after the tension
action. Within the carbon fiber bundle, some portion of the unim-
pregnated fibers existed as a curved shape prior to the tensile loading.
When the tensile test was initiated, the tensile load was distributed on
both aligned and unaligned carbon fibers, but not all the fibers endured
the load at this time. The weak carbon fibers tended to firstly fracture,
and the curved fibers were then gradually straightened as the de-
formation and load continued to increase. However, the curved fibers
exhibited a “delay” in carrying the load, resulting in a decrease of the
overall load-bearing capacity of the fibers. Such a phenomenon could
cause smaller experimental results than the theoretical ones that were
predicted based on the assumptions.
5. Conclusions
In this study, a novel mechanistic model for predicting tensile
strength and elastic modulus of C-CFRP built by co-extrusion based FFF
process was developed. Fiber-matrix impregnation characteristics in-
cluding fiber orientation coefficient, physical gap ratio, as well as the
volume of impregnated and unimpregnated fibers were studied for the
first time. The validity of the established model was verified by com-
paring the theoretical values with the experimental results obtained
through the fabrication of C-CFRP parts with different matrix materials.
The main conclusions obtained in this work are drawn as follows:
(1) The theoretically predicted values of tensile strength and elastic
modulus agreed well with the experimentally measured results of C-
CFRP with different matrix materials, achieving an average pre-
diction error of 2.87∼4.29 % and 2.63∼8.36 %, respectively.
(2) The largest tensile strength (288.65 MPa) was achieved by CCF/
SCF/PA, whereas the smallest one was seen in the CCF/PC sample
with an average value of 238.85 MPa. On the other hand, CCF/PLA
11
F. Wang, et al.
possessed the largest average elastic modulus of 29.12 GPa, and
CCF/PC again was the specimen containing the smallest elastic
modulus of 26.28 GPa.
(3) CCF/PC specimens exhibited poor fiber-matrix impregnation in-
dicated by the serious unimpregnated fiber pull-out phenomenon,
whereas CCF/SCF/PA and CCF/PLA showed a better impregnation
behavior evidencing the larger UTS and elastic modulus obtained
experimentally.
The fraction of carbon fiber could affect the impregnation degree
(Vf1 and Vf2) by changing the space between neighboring fibers. In the
future work, the influence of carbon fiber fraction on the impregnation
behavior and the subsequent tensile strength/modulus would be in-
vestigated to improve the prediction accuracy of the mechanistic
model.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.
Acknowledgments
Fuda Ning gratefully acknowledges SUNY Binghamton for providing
support through his startup funds. Fuji Wang acknowledges the sup-
ports by the Science and Technology Innovation Foundation of Dalian
(Grant#: 2018J11CY001) and National Innovative Research Group
(Grant#: 51621064) in China.
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