Materials Today Advances 5 (2020) 100045

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Materials Today Advances

journal homepage: www.journals.elsevier.com/materials-today-advances/

Additive manufacturing of multidirectional preforms and composites:

from three-dimensional to four-dimensional
Y. Liu a, T.-W. Chou b, *
a
College of Textiles, Donghua University, Shanghai, 201620, PR China
b
Department of Mechanical Engineering, University of Delaware, Newark, DE, 19716, USA

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

Article history: Multidirectional textile preforms, such as three-dimensional (3D) angle-interlock woven fabric,
Received 28 September 2019 orthogonal woven fabric and braided fabric, have been often used for developing lightweight and high-
Received in revised form strength composites. Although multidirectional preforms for composites have been fabricated using
1 December 2019
traditional textile-forming techniques, some basic technological barriers still exist. Recent advancements
Accepted 2 December 2019
Available online 8 January 2020
in additive manufacturing (also known as 3D printing) have opened up new opportunities for
manufacturing of multidirectional preforms and their composites. Furthermore, the functionalization of
3D preforms can greatly facilitate their application in the field of smart devices. The key step of the
Keywords:
Multidirectional preform
functionalization is to add the ‘time’ dimension to the 3D printed objects, with the resulting process
3D printing known as four-dimensional (4D) printing. In this review article, we first briefly summarize the recent
4D printing research work in the characterization of fabrication-induced defects when using a layer-by-layer
Mechanical property deposition process and discuss the effect of processing parameters. Then, the various approaches in
Shape memory property 4D printing for achieving shape morphing overtime are reviewed. Finally, some strategies for developing
4D printed multidirectional shape memory polymer-based preforms with high shape memory perfor-
mance are summarized. Potential challenges and opportunities in the development of 3D printing and
4D printing are outlined.
© 2020 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND
license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

1. Introduction
Additive manufacturing (AM), also known as three-dimensional
(3D) printing, is a versatile and powerful technology to fabricate
composites with complex microstructures [1,2]. Its history dates
back to 1984, when Charles Hull filed the patent on stereo-
lithography (SLA) [3]. AM is usually defined as the process of
building a 3D object from model data with the deposition of ma-
terials layer by layer, as opposed to subtractive manufacturing
methods [4]. Superior to other manufacturing techniques, 3D
printing enables the rapid fabrication of lattice and multidirectional
structures ranging from nanoscale [5] to microscale [6] to macro-
scale [7]. In recent years, researchers have devoted much attention
to four-dimensional (4D) printing technology, which combines 3D
printing with stimuli-responsive materials [8]. The concept of 4D
printing was first introduced by Skylar Tibbits at a 2013 TED talk [9].
Four-dimensional printing is generally defined as a 3D printing
* Corresponding author.
E-mail address: chou@udel.edu (T.-W. Chou).
process of which the shape and property of its product can change
overtime in response to a certain stimulus, such as heat [10e12],
light [13,14], solvent [15,16], electric field [17] or magnetic field [18].
It has been demonstrated that 4D printing technology has many
potential applications in the fields of soft robotics [19,20],
biomedical engineering [21], electronic devices [22], and functional
textiles [23,24].
Besides its application in apparel fabrication, modern textile
engineering has enabled the design and manufacture of advanced
lightweight composites based on high-performance fibers [25e27].
Two-dimensional and 3D textile preform reinforced polymer-,
metal-, and ceramic-matrix composites have demonstrated unique
in-plane and through-the-thickness strength as well as damage
tolerance [28e31]. Although these multidirectional preforms have
been fabricated using traditional textile-forming techniques [32],
some basic technological barriers still exist. For instance, the
microstructure of a textile preform may deviate from that of the
designed model [33], and the available textile topological struc-
tures are limited in many textile-forming machines [34]. Ad-
vancements in 3D printing technology have provided tremendous

https://doi.org/10.1016/j.mtadv.2019.100045
2590-0498/© 2020 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
2 Y. Liu, T.-W. Chou / Materials Today Advances 5 (2020) 100045
opportunities for manufacturing of multidirectional preforms and
their composites based on direct, layer-wise processes [35]. Thus,
the aim of this study is to review some of the recent research on 3D
and 4D printed multidirectional preforms and composites as well
as the results of their performance characterizations. Strategies for
improving the shape memory property of 4D printed multidirec-
tional preforms are also summarized.
2. Multidirectional textile preforms
Multidirectional textile preforms have been fabricated by
weaving, knitting, braiding, and stitching techniques with the
reinforcing yarns oriented in multiple directions [27,36e38]. Fig. 1
schematically shows the classification of typical structures of
multidirectional preforms based on the yarn spatial orientation.
Two-dimensional textile preforms, such as plain woven fabric,
triaxial woven fabric, knitting fabric inset with straight yarns, and
triaxial braid (Fig. 1aed) are often used individually or stacked to
form laminates. The term two-and-a-half-dimensional textile pre-
forms refers to a family of angle-interlock woven fabrics without
through-the-thickness yarns. Fig. 1e and f show layer-to-layer
angle-interlock woven fabrics without and with insetting straight
yarns, respectively. Three-dimensional textile preforms often
exhibit good dimensional stability [39] and outstanding out-of-
plane mechanical properties [40]. Fig. 1gej shows some typical
3D preforms, including through-the-thickness angle-interlock
woven fabric, orthogonal woven fabric, a braided structure, and a
stitched laminated preform. Although the textile preforms
described previously have been successfully applied to the fabri-
cation of advanced composites for over three decades, the
complexity in preform processing and the low level of automation
have hindered their further development.
Fig. 1. Classification of typical multidirectional textiles based on the dimension of
preform structures. Two-dimensional (2D) textile structures: (a) plain woven fabric, (b)
triaxial woven fabric, (c) knitting fabric inset with straight yarns, and (d) 2D triaxial
braid; 2.5D textile structures: layer-to-layer angle-interlock woven fabric (e) without,
and (f) with insetting straight yarns; 3D textile structures: (g) 3D through-the-
thickness angle-interlock woven fabric, (h) 3D orthogonal woven fabric, (i) 3D
braided structure and (j) 3D stitched laminated preform. 2.5D, two-and-a-half-
dimensional; 3D, three-dimensional; 2D, two-dimensional.
3. Three-dimensional printing of multidirectional preforms
and composites
3.1. Three-dimensional printing methods
There are currently more than 50 different AM techniques in
accordance with the American Society for Testing and Materials
(ISO/ASTM 52900:2015). Extrusion-based and photo-assisted
methods have been used most often for 3D printing of polymers
[41]. Typical extrusion-based methods are fused deposition
modeling (FDM) and direct ink writing (DIW). Frequently used
photo-assisted methods include SLA (using a laser beam), digital
light processing (using a projector) and inkjet 3D printing (using
multinozzles). All of these 3D printing methods have been adopted
for manufacturing reinforced composites [42,43]. The methods,
materials, and distinctive attributes of 3D printing (AM) techniques
have been well summarized in [1,44]. Recent advancements in AM
technology have enabled rapid, support-free fabrication with low
energy consumption and high resolution. For example, support-
free fabrication of spring-like structures has been realized using a
DIW frontal polymerization technique, in which an exothermic
reaction wave can self-propagate to cure liquid monomers within
seconds [45]. It has been demonstrated that a 900 cm2 carbon fiber
(CF)ereinforced polymer composite panel with 51% fiber volume
fraction can be prepared in 5 min with energy consumption around
750 J. Another example can be found in computed axial lithography
(CAL), a modified version of SLA, which is capable of printing all
points in a 3D model using a dynamically evolving light pattern for
curing a rotating volume of photosensitive material [46]. The CAL
technique can not only process objects with smooth surfaces in a
support-free condition, but also realize one-step 3D integrated
manufacturing without relying on conventional layer-based
printing.
3.2. Microstructure of 3D printed preforms
Compared with the traditional injection molding of polymers,
there are more interfaces and voids in 3D printed products owing to
the layer-by-layer process. Optical microscopy [47] and scanning
electron microscopy (SEM) [48], for example, have been used to
examine the morphologies of 3D printed objects. However, these
microscopic techniques are often effective for characterizing
external morphologies and provide little information about the
internal microstructures. X-ray micro-computed tomography (m-
CT), a nondestructive and high-resolution imaging technique, has
been used to analyze the internal morphology of 3D printed parts
[49e51]. For example, [52] demonstrated the use of m-CT to identify
fabrication-induced defects in multidirectional preforms; they
included interline gaps within a printed layer, interline gaps be-
tween adjacent layers, and voids on the boundary of a printed layer
(Fig. 2a and b). Furthermore, the horizontal cross-sectional m-CT
image of a 3D printed braided preform showed that it had internal
gaps in the printed yarns (Fig. 2c), which resulted from the lack of
line overlapping [52]. The 3D reconstructed model from m-CT im-
ages (Fig. 2d) showed a good fidelity to the designed model of the
preform. The printing parameters and fillers also have significant
influences on the void content of 3D printed objects [53] demon-
strated the printing direction dependence of the anisotropic me-
chanical properties of printed parts. In addition, higher printing
speed tended to give rise to higher void content (Fig. 2e) [54].
Compared with a carbon nanotube (CNT)/acrylonitrile-butadiene-
styrene (ABS) specimen, the short CF/ABS composite showed
higher void content because of the relatively poor polymer melt
mobility (Fig. 2f). The morphologies of the various components,
namely the fiber, matrix, and voids, of a 3D printed basalt fiber-
 Y. Liu, T.-W. Chou / Materials Today Advances 5 (2020) 100045 3

Fig. 2. Microstructure characterizations of 3D printed objects using the X-ray m-CT imaging technique. (a) Cross-sectional m-CT image, and (b) 3D reconstructed m-CT image of a 3D
printed cube [52]. (c) Designed model, cross-sectional m-CT image, and (d) 3D reconstructed microstructure of the ABS-printed braided preform [52]. (e) m-CT images of 3D printed
specimens with printing speeds of 40 mm/s, 60 mm/s, and 80 mm/s [54]. (f) m-CT images of 3D printed specimens using ABS, CNT/ABS, and carbon fiber/ABS filaments [54]. (g) m-CT
images of a 3D printed basalt fiber-reinforced PLA composite and its individual components [55]. m-CT, micro-computed tomography; CNT, carbon nanotube; ABS, acrylonitrile-
butadiene-styrene; 3D, three dimensional; PLA, polylactic acid.

reinforced polylactic acid (PLA) composite were clearly identified

using m-CT imaging as demonstrated in Fig. 2g [55]. The micro-
structural knowledge of 3D printed preforms and composites
gained from using m-CT imaging is beneficial in improving their
mechanical properties.

3.3. Fabrication and characterization of 3D preforms and

composites

Some of the recent developments in the research of 3D printed

multidirectional preforms and their reinforced composites are
reviewed in the following paragraph. Quan et al. [56] first fabri-
cated an array of complex multidirectional preforms using FDM
with a pure ABS filament. They also identified all the topologically
independent 3D orthogonal preforms in terms of the Cartesian,
cylindrical, and spherical coordinate systems [57]. Then, using the
FDM method, all the topologically independent 3D preforms were
printed. For example, Fig. 3 presents the designed and fabricated
preforms based on the cylindrical coordinate system. It is inter-
esting to note that 3D printing enables the fabrication of preforms
developed based on the cylindrical coordinate system, which is not
possible to use textile-forming techniques. The results of the study
by Quan et al. [53] also showed that the mechanical properties of
3D printed preforms using short CF-reinforced ABS filament were
Fig. 3. Four topological designs and additive manufacturing of 3D orthogonal preforms
inferior to those of the ABS counterpart, which was attributed to are in terms of the cylindrical coordinate system. The corresponding yarn alignments,
the higher void content in the CF/ABS-printed preform. It should be designed models, and manufactured preforms are given from left to right [57]. 3D,
noted that the mechanical properties of printed multidirectional three dimensional.
preform/resin composites could be lower than those of the pure
resin if there was a poor interface bonding between the printed
preform and the infused resin [58]. have investigated 3D printed continuous fiber-reinforced polymer
To achieve mechanical properties comparable with those of composites. For example, continuous carbon fiber (CCF) and ther-
traditional fiber-reinforced polymer composites, many researchers moplastic ABS filament were simultaneously extruded through the
4 Y. Liu, T.-W. Chou / Materials Today Advances 5 (2020) 100045

nozzle to fabricate laminates, which showed comparable me-
chanical properties to those of the injection-molded CCF/ABS
specimen [59]. The laminate fracture mode of Yang et al. [59] was
fiber pullout, and the SEM image showed poor polymer matrix
impregnation in the carbon yarns. In an attempt to improve poly-
mer impregnation (i.e. low void percentage) in continuous fibers,
Eichenhofer et al. [60] adopted the approach of preparing small
diameter CF-reinforced polyamide filament first, and then coex-
truding seven individual filaments through four conical dies with
cyclic softening (Fig. 4a). Eichenhofer et al. [61] successfully fabri-
cated a multidirectional fiber-reinforced polyamide composite as
the core of an ultralightweight load-bearing sandwich (Fig. 4b).
Owing to the limited yarn systems available, the interlacing of
continuous fiber-reinforced polymer filament was difficult to
realize in a 3D printer. Dickson et al. [62] presented a method to
print woven composites by controlling the fiber path using modi-
fied G-code (a programming language to control the nozzle
movement) (Fig. 4c). Unlike the aforementioned fiber-reinforced
thermoplastic polymer composites, Hao et al.[63] reports the
fabrication of a lightweight multidirectional fiber reinforced ther-
moset polymer tube by printing continuous CF-reinforced epoxy
prepreg on a rotating cylindrical platform (Fig. 4d). The results
showed that the mechanical properties of the 3D printed contin-
uous fiber-reinforced thermoset composite were superior to those
of their 3D printed thermoplastic counterparts and 3D printed
short fiberereinforced counterparts.
4. Four-dimensional printing of multidirectional preforms
and composites
The functionalization of 3D printed multidirectional preforms
greatly facilitates their application in the field of smart devices. The
key step of the functionalization is to add the ‘time’ dimension to
3D printed objects, advancing to 4D printing. Various approaches
have been developed in 4D printing to achieve shape morphing
overtime, and these methods are summarized in Table 1. One of the
simplest methods for realizing shape morphing overtime is to print
an object using stimulus-responsive materials, such as shape
memory polymers (SMPs), liquid crystal elastomers and hydrogels.
For example, Liu et al. [64] demonstrated the recovery behavior of
large shape transformation of Miura-origami structures printed
using the FDM method and shape memory PLA filament. Choong
et al. [65] used the SLA method to print a 3D fullerene-like struc-
ture, which maintained high shape memory performance with
more than 20 shape recovery cycles. In addition, the release of re-
sidual stress, thermal stress-induced shrinkage, and mismatching
properties can be used to obtain shape morphing overtime
(Table 1).
The convergence of 3D printing technology and SMPs has
motivated numerous research efforts in 4D printing of multidirec-
tional preforms and their functional composites. A few examples
are cited in the following paragraphs. Zhang et al. [86] examined
the shape recovery behavior of printed circular braided tube pre-
forms using the FDM method with the SMP filament (Fig. 5a). A
typical shape memory cycle is shown in Fig. 5b. The circular braided
preform with a 30 braiding angle and three braiding layers almost
recovered to its original shape at 180 s (Fig. 5c). The results also
demonstrated that higher recovery temperature, larger braiding
angle, and smaller braiding layers resulted in shorter recovery time.
The final recovery ratio of the circular braided preform was 84.6%,
which did not reach full recovery because of the influence of the
self-weight. Furthermore, composites fabricated by infusing sili-
cone elastomer matrix into the printed preform significantly
enhance the recovery force. Liu et al. [67] printed the rectangular
braided preform and showed its high model-to-part fidelity using
m-CT imaging (Fig. 5d). A PLA specimen that was bent to a 90 angle
recovered its original shape at 124 s (Fig. 5e). Compared with the
PLA braided preform, the CNT/PLA braided preform had a smaller
final recovery ratio, resulting from the CNT slippage in the polymer
matrix (Fig. 5f). The infusion of silicone elastomer matrix improved
the final recovery ratio of the CNT/PLA braided preform because of
the elasticity of the silicone matrix (Fig. 5g). Furthermore, the
addition of either CNTs or a silicone matrix could improve the re-
covery force of the resulting preform or composite.
The shape recovery properties of the printed thermoplastic
SMPs were often less than desirable. Some strategies for future

Fig. 4. Three-dimensional printed continuous carbon fiberereinforced polymer composites. (a) Schematic of the coextrusion and the cross-sectional optical images of the filaments
after 1 time softening process and 4 times softening process [60]. (b) Ultralightweight sandwich structure with multidirectional long fiber-reinforced polymer composite core [61].
(c) Three-dimensional printed woven carbon fiber laminate through control of the fiber path and illustration of the cross-sectional structure [62]. (d) Modified FDM platform (left)
and continuous carbon fiberereinforced thermoset tubular composite (right) [63]. FDM, fused deposition modeling.
 Y. Liu, T.-W. Chou / Materials Today Advances 5 (2020) 100045 5

Table 1
Summary of methods of 4D printing.

Mechanism of shape morphing Printing method Material type Stimulus Applications

Shape memory effect FDM [24,64,66e69] Shape memory polymers Heat Actuators, smart textiles
Shape memory effect SLA [65,70,71] Shape memory polymers Heat Actuators, stents
Shape memory effect DIW [72,73] Shape memory composites Magnetic field, heat Biomedical and electrical devices
Switch between nematic state DIW [74,75] Liquid crystal elastomers Heat Actuators, hinges
and isotropic state
Swelling DIW [76e78] Hydrogels, fibrils-filled hydrogels Heat and water Hinges, biomimetic devices
Release of residual stress FDM [79] Shape memory polyurethane Heat Self-tightening sutures and stents
Thermal stress-induced shrinkage FDM [80,81] Polylactic acid Heat Self-morphing structures
Mismatching swelling ratios Polymer jetting [82] Rigid plastic base and hydrophilic polymer Water Self-morphing structures
Mismatching coefficients of FDM [83] Continuous carbon fiber/polyamide Heat Self-morphing structures
thermal expansion 66 and pure polyamide 66
Mismatching modulus Polymer jetting [84,85] Tangoblack (a rubbery material) and Verowhite Heat Hinges
(a rigid plastic)

4D, four-dimensional; FDM, fused deposition modeling; DIW, direct ink writing; SLA, stereolithography.

development of 4D printed multidirectional SMP preforms with
high shape memory performance are summarized as follows: (a)
Melt-blending. SMP and elastic polymer (e.g. PLA and poly-
urethane): were melt blended to obtain good shape memory effect
[87e90]. (b) Filling. Nanomaterials and fibers, such as (CNTs)
[91,92], graphite oxide [93], SiC [94], and short and long carbon
fibers [95,96], could be added in the SMP matrix as printing ma-
terials for manufacturing multidirectional preforms. (c) Hybridiz-
ing SMP with polymeric elastomer. A printed SMP preform
hybridizing with the additionally printed elastomer component

Fig. 5. Four dimensional printed multidirectional preforms. Four-dimensional printed circular braided preform: (a) optical image (left), enlarged optical image (middle), and its
silicone elastomer matrix composites (right); (b) typical shape memory cycle based on a compressive load; (c) snapshots of shape recovery process at 70  C [86]. Four-dimensional
printed rectangular braided preform: (d) optical image and its local m-CT image; snapshots of shape recovery process at 90  C of the preform printed with (e) PLA, and (f) CNT/PLA
filaments, as well as (g) the CNT/PLA braided preform/silicone matrix composite [67]. m-CT, micro-computed tomography; CNT, carbon nanotube; PLA, polylactic acid.
6 Y. Liu, T.-W. Chou / Materials Today Advances 5 (2020) 100045
[97], and compositing with silicone elastomer matrix [67,86] have
been adopted for improving the shape recovery capacity. Ge et al.
[84] fabricated active laminated composites by jet printing SMP
fibers in an elastomeric matrix using a multimaterial 3D printer. (d)
Hybridizing SMP with metallic spring. Wang and Wang [98], Kim
and Park [99] and Liu et al. [69] demonstrated enhanced shape
memory of a hybrid laminate composed of an SMP specimen and a
spring steel strip. Here, the hybrid effect is attributed to the release
of the elastic strain energy of the spring strip in facilitating shape
recovery of the SMP specimen.
5. Concluding remarks
In this review, typical multidirectional textile structures were
first summarized. 3D printing has provided the unique capability to
manufacture certain topological structures that were not feasible
using traditional textile-forming techniques. m-CT imaging is a
versatile technique for characterizing the microstructures of 3D
printed multidirectional preforms and composites as well as their
fabrication- and deformation-induced defects. Three-dimensional
printed continuous fiber-reinforced polymer composites have the
potential to manufacture multidirectional composites with high
mechanical performance. Strategies in advancing 3D printing to 4D
printing are reviewed, and recent research work on 4D printed
multidirectional preforms and composites is discussed. In addition,
recent approaches for enhancing the shape recovery properties of
4D printed composites are summarized. Finally, some interesting
opportunities and challenges in manufacturing multidirectional
preforms and composites are given in the following points.
(1) A one-step 3D integrated manufacturing technique without
relying on layer-based printing, such as CAL, may be prom-
ising in reducing fabrication-induced defects for
manufacturing multidirectional preforms and composites.
(2) An interesting and challenging pursuit in 3D printing using
continuous fiber is to create multidirectional preforms where
yarn interlacing is preserved.
(3) It is desirable to further develop 4D printing of multidirec-
tional preforms using short or continuous fiber-reinforced
thermoset SMP for high shape memory performance. Their
interfacial bonding strength also requires in-depth studies.
Conflict of interest
The authors declare that they have no known competing
financial interests or personal relationships that could have
appeared to influence the work reported in this paper.
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