Applied Food Research 2 (2022) 100150

Contents lists available at ScienceDirect

Applied Food Research

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

4D printing: a new approach for food printing; effect of various stimuli on

4D printed food properties. A comprehensive review
Muhammed Navaf a, Kappat Valiyapeediyekkal Sunooj a,∗, Basheer Aaliya a,
Plachikkattu Parambil Akhila a, Cherakkathodi Sudheesh a, Shabir Ahmad Mir b, Johnsy George c
a
Department of food science and technology, Pondicherry University, Puducherry,605014, India
b
Department of Food Science and Technology, Government College for Women, M.A. Road, Srinagar, Jammu, and Kashmir, India
c
Food engineering and packaging division, Defence food research laboratory, Mysore,570011, India

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

Keywords: 4D printing is an additive manufacturing technique and is an extension of 3D printing. 4D food printing is a newly
Shape memory polymers developed area in 4D printing, and it is in the stage of infancy. 4D food printing has gained much attention from
Model designing the academic and industrial sectors. Compared to other fields of 4D printing, the number of literature reviews
Food printing
available for 4D food printing is scanty. The current article gives an overview of 4D printing with an emphasis
Stimulus induced changes
on 4D food printing. This review address the effect of various stimuli on the properties such as color, flavor,
texture, and shape of 4D printed food samples. Besides, it also covers 4D design development, food printing ink,
and various methods used in 4D food printing. Most 4D food printing focuses on microwave treatment or the
influence of pH as a stimulating agent in printed food objects. The food properties like color, taste, aroma, texture
and the shape of 4D printed food changed under stimuli. Starch, soy protein isolate, potato purees, buckwheat
dough, etc., are food materials yet to be explored in 4D printing. The printing ink used in 4D printing consists
of a stimulus-responsive material, bringing spontaneous changes in 3D printed structure. Anthocyanine, vanillin
powder, and curcumin area few stimulus-responsive materials used in 4D food printing, which will change color
in response to pH. The use of multiple stimulus-responsive materials and different stimulating agents like light
can be explored.

1. Introduction
Four-dimensional (4D) printing is a newly developed field of print-
ing, which is an additive manufacturing technique. The 4D printing
technology is an extension of 3D printing, and it is a new concept that
changes the printed configuration over time (Choi et al., 2015). This
idea was first developed by a research team at the Massachusetts Insti-
tute of Technology (MIT) in 2013 (Tibbits, 2014). 4D printing is similar
to 3D printing in the printing process, like 3D design development and
printing the structure using a 3D printer (Choi et al., 2015). The ma-
jor distinctions between 4D and 3D printing are smart design and smart
materials, as 4D printed structures may change shape or function (Pei
& Loh, 2018).
Smart materials used in 4D printing have self-assembly, versatility,
and self-healing properties (He, Zhang, & Guo, 2020). Most 4D print-
ing materials are single or multilateral polymers (Kuang et al., 2019).
It includes shape memory polymers, liquid crystal elastomers, and com-
posite hydrogels (Sharma & Tabbits, 2020). Stimulus responsive shape
changes of 4D printing help to save space for transportation and stor-
age (Pei & Loh, 2018). Hence, 4D printing is explored in various fields
such as robotics, biomedical, tissue engineering, electronic device, etc.
(Ghazal et al., 2021). However, in the field of food, only a few pieces of
literature are available, and it’s in the stage of infancy. Material adapt-
ability is an advantage of 4D printing, allowing customized material
responsiveness configurations. The self-changing nature of 4D printed
things aids in material reduction (Chu et al., 2020). Consumer attitudes
and desire for unique food products have the potential to be addressed
by 4D printing (Phuhongsung, Zhang, & Bhandari, 2020). Furthermore,
the directed adjustable deformation of the structure may aid chefs in
determining the final point of cooking and make the food more visually
appealing and tasteful (Chen et al., 2021). In 4D printing, the desirable
properties of a product can be achieved in an appropriate time, and it
may decrease during the storage of printed products.
The research group first reported 4D food printing from MITdevel-
oped an edible 2D film with starch, cellulose, and protein that changes
to 3D in the presence of water (Wang et al., 2017). Unlike other fields of
4D printing, the food field uses various combinations of food materials
as printing ink instead of using smart materials (Jiang et al., 2019). It

∗
Corresponding author.
E-mail address: sunoojpufst786@gmail.com (K.V. Sunooj).

https://doi.org/10.1016/j.afres.2022.100150
Received 14 March 2022; Received in revised form 27 May 2022; Accepted 12 June 2022
Available online 14 June 2022
2772-5022/© 2022 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/)
M. Navaf, K.V. Sunooj, B. Aaliya et al.
depends on the structure and type of stimulating agent used. The use
of specific formula in the preparation of printing ink will bring pre-
dictable changes in the printed object’s properties (color, flavor, texture,
shape, etc.) under the presence of stimuli like temperature, pH, water,
etc. (Zhao et al., 2020). 4D food printing brings self-transformation of
color/ texture/ flavor and other properties of the printed object as a
function of time, which gives a unique character and visual enjoyment
during the meal (Ghazal et al., 2019).
The 4D printing in food is a fast-growing area in research. Hence
this review focuses on various stimulating agents, stimulus-responsive
materials, and stimulus-induced changes in different properties (color,
taste, aroma, texture, and shape change) of 4D printed food.
2. 4D printing
Additive manufacturing is gaining substantial attention due to the
development of 3D structures, and it has a history of 30 years (Choi et al.,
2015). 4D printing is an extended version of 3D printing, which pro-
vides a function of time. It helps to develop a dynamic structure, which
changes the shape, function, and properties under the influence of var-
ious stimuli (temperature, pH, ionic concentration, electric and mag-
netic field). In nature, there are many examples of 4D changes of ob-
jects with various stimuli like the hygroscopic unfolding of pinecones
and the heliotropic sun-tracking behavior of plants like sunflowers,
etc.(Mulakkal et al., 2018). The key components in the 4D printing
process are the additive manufacturing method, types of stimuli used,
type of stimulus-responsive material used, the interaction mechanism,
and mechanical modelling (Ali et al., 2019). Some of the technologies
utilized in 4D printing include micro extrusion-based printing, fused
deposition modelling, stereolithography, and digital light projection
(Lai et al., 2021). The micro-extrusion process is widely utilized among
diverse printing technologies due to its convenience and flexibility in
employing numerous inks.
2.1. 4D printing materials
The material used for 4D printing is known as smart materials. They
have the ability to change their properties during storage under the in-
fluence of a stimulus. These stimuli can be heat, pH, light, etc. Smart
materials can respond to external stimuli and possess behaviors like self-
assembly, self-healing, shape memory, and self-capability. In addition,
these materials may change color, flavor, etc. (Ahmed et al., 2021). The
smart materials used for 4D printing are either a single material like
shape memory polymers (SMP) or liquid crystal elastomers (LCE). It
can be a metamaterial composite like a hydrogel.
2.1.1. Shape memory polymer (SMP)
These polymeric materials can sustain a temporary change in shape
and structure and reform to their original shape under a stimulus. The
SMP has several advantages over other printing materials, such as higher
recovery, light weight, processability, better shape deformability, and
low cost. The SMPs exhibited a time-dependent dynamic change to a
preprogrammed shape or reverted to an initial design under certain
stimuli, known as 4D printing (Mehrpouya et al., 2021). Polylactic
acid is the most often used SMP in 4D printing, and other materials
such as bisphenol, poly cyclo-octene, etc., are also used (Ehrmann &
Ehrmann, 2021). Due to the high tunability of transition temperature,
optical and mechanical properties, and convenience of triggering shape
memory, thermo-responsive SMPs are widely investigated. In general,
these are printed in a deformed state. It is deformed by exposing at a
temperature higher than the transition temperature and then cooling to
a temperature below the transition temperature and finally unloaded.
Shape recovery is the induced or expected changes through external
factors after printing. The exposure to a temperature above transition
temperature results in a recovery step in which the SMPs regain their
pre-programmed shape due to entropic elasticity (Ahmed et al., 2021).
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Applied Food Research 2 (2022) 100150
2.1.2. Liquid crystal elastomers (LCE)
LCEs are another group of smart materials used in 4D printing that
reveal both the order of solid crystals and the fluidity of liquids. Gener-
ally, to generate the anisotropic properties of LCEs, mesogenic moieties
are incorporated into the polymer network, either in the chain backbone
or as side groups (Sun et al., 2021) .Poly (hydrosiloxane) polymers, acry-
lates, and methacrylates are the most commonly used precursors for syn-
thesising LCEs (Ula et al., 2018). LCEs are stimuli-responsive, reversible,
anisotropic shape-changing materials. LCEs may undergo shape change
by environmental stimuli like temperature, light, electric, and magnetic
fields. Under the influence of an external stimulus, the contraction of
LCEs containing liquid crystal molecules (or mesogens) can be substan-
tial in the direction of the mesogens (or nematic director). At a tempera-
ture above or below, it exhibits microscopic contraction and elongation,
respectively (Wan et al., 2020).
2.1.3. Composite hydrogel
Hydrogels are a kind of polymers like shape memory polymers and
liquid crystal elastomers, which are widely used in 4D printing. Hydro-
gels are a 3D network of hydrophilic materials that absorb moisture
without dissolving and gets wells. It also possesses a high printing ca-
pability as various structures were developed using hydrogels capable
of folding, bending, stretching, and geometrical expansion. However,
the slow reverse response of the hydrogels, to overcome this, hydrogels
are needed to be programmed so that anisotropy will be added to their
swelling (Ahmed et al., 2021). Many researchers exploited the proper-
ties of hydrogel to develop shape-changing materials. The 4D printing
of hydrogels is usually carried out by light-based printing and extrusion-
based printing. Light-based printing techniques use the photopolymer-
ization principle to convert monomers present in the printing ink to
hydrogels. Stereolithography and digital light processing are two vari-
ants used for radiating the printing ink. Stereolithography and digital
light processing use laser beams and a projector to promote gel forma-
tion. In extrusion printing, the preconditioned gel is forced through a
nozzle, and the deposition process can be aided either by forced air or
by mechanical means. The use of multiple extruders facilitates the si-
multaneous deposition of different compounds and the production of
multiple colored products. It is a faster process, which avoids the swap-
ping out of one filament to other. Post printing treatment of hydrogels
hastens the polymerization and cross-links development in printed hy-
drogels. One of the challenges faced by extrusion printing hydrogels is
their low polymerization kinetics, which may cause problems in keeping
the dimensions of the printed object. Based on the stimuli-responsive
mechanism, hydrogels are grouped into active and passive responsive
hydrogels. The active responsive hydrogels undergo volume or phase
change while exposed to a stimulus. It is mainly due to the molecular
changes and rearrangements of polymer chains and networks in hydro-
gels (Shen et al., 2020).
A 4D printed alginate and methylcellulose shape morphing hydrogel
was created by deliberately regulating the network density gradients
vertical to the orientation of the patterned strips. The 4D structure is
out of a succession of patterned 2D structures encoded with anisotropic
stiffness and swelling characteristics (Lai et al., 2021). The shape mor-
phing of the hydrogel is due to the development of non-uniform inter-
nal stress, which results in localized uneven swelling or shrinkage of
hydrogels (Lai et al., 2021). These shape morphing hydrogels can be
developed by using different compounds across the hydrogel thickness
(Kirillova et al., 2017), hydrogel plane, and in both hydrogel plane and
thickness (Du et al., 2019).
3. 4D Bioprinting
4D bioprinting refers to the printing of 3D biocompatible materi-
als or living biological structures that evolve over time (Kuang et al.,
2019). It includes a predetermined conformational change in the
printed object by comprising a stimulus-responsive biomaterial or cell
M. Navaf, K.V. Sunooj, B. Aaliya et al.
(Ashammakhi et al., 2018). The 4D bioprinting has potential application
in in-vivo experiments, where it needs to develop characteristic struc-
ture after printing due to environmental changes (Yang et al., 2019). It
is also explored in tissue engineering, drug delivery, and wound repair
(Yang et al., 2020).
4. 4D printing in food
In the food sector, 4D printing was first introduced by researchers
from MIT. They developed a starch, cellulose, and protein-based 2D film
and used water as a stimulating agent. The printed 2D film was changed
to 3D in the presence of water (Wang et al., 2017). 4D printing of food
will help customize the product and develop unique characteristic fla-
vors for the products. The stimulus-induced changes in the 4D printed
food samples can be achieved by using the printing ink in different com-
binations of food materials based on the structure and specific food for-
mula (Teng et al., 2021). Food may change its color, texture, aroma, and
shape under various stimuli like temperature and pH. A 4D change in 3D
printed buckwheat dough, and lotus root powder gel was observed when
microwave heating was used as a stimulating agent (Guo et al., 2021;
Chen, Zhang, Mujumdar, et al., 2021). Similarly, pH-induced changes
in the color of 3D printed soy protein isolate, pumpkin, and beetroot
mixture were reported (Phuhongsung, Zhang, & Devahastin, 2020a).
4.1. Inks in 4D food printing
In 4D food printing, the food ingredients used for printing are re-
ferred to as printing ink (Kewuyemi et al., 2021). The printability of food
printing ink is a combination of rheological characteristics for smooth
extrusion and mechanical strength to maintain mass and texture dur-
ing the printing process (Lee et al., 2019). The printability of the food
ink also influences the structure’s extrudability, flowability, and post-
printing stability (Kewuyemi et al., 2021). The food ink used for printing
must possess both liquid-like and solid-like structures before and after
printing (Gholamipour-Shirazi et al., 2019). The effect of particle size
on the printing performance of food inks was studied. The researchers
noticed that the larger particles (307 μm and 259 μm) are more porous
than small particles (up to 172 μm), showing a skeleton-like cellular
structure. And the particle size of printing ink will affect the physical
and functional properties (density, oil, water absorption capacity, etc.)
of the printed object (Lee et al., 2019).
In the recent past,a large number of food materials have been de-
veloped by using printing technology. Food materials used in food
ink production include chocolate (Rando & Ramaioli, 2021), soybean
(Phuhongsung, Zhang, & Devahastin, 2020b; Balla et al., 2020), meat
(Wilson et al., 2021; Wilson et al., 2021), starch (Zheng et al., 2021;
Zeng et al., 2021) fruit and vegetables (Chen et al., 2021; Chen et al.,
2021), food hydrocolloids (Pant et al., 2021), etc. The moisture con-
tent of the food material used as food ink has a significant role in their
printing performance. Hence, using a dried and powdered form of food
materials can maintain food materials’ nutritional value and functional
properties (Lee et al., 2019).
In addition, 4D printing food ink mixture consists of certain materials
which act as stimulus-response material. Under certain conditions or
stimuli, these compounds change their color, flavor, texture, etc.Hence
the sensitivity of the stimulus-response material in food printing ink
plays a significant role in 4D changes in printed objects. The pigments
present in printing ink cause 4D changes in the color of food under
different pH. Curcumin is one of the stimulus-responsive materials used
in 4D printing, which exhibits a red color in alkaline pH and yellow in
acidic or neutral pH (C. Chen, Zhang, Guo, et al., 2021).
Similarly, anthocyanin also acts as a stimulus-response material and
exhibits different colors under pH stimulus (He et al., 2021). Gelatin-
gum Arabic-flavor oil complex also proved its thermal response and is
used as a stimulus-response material in printing buckwheat dough with
yellow flesh peach. The research team observed a simultaneous change
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Applied Food Research 2 (2022) 100150
in color and flavor of the product under microwave stimuli (Guo et al.,
2021). The stimuli-induced changes of the 4D printed object should be
controllable, and the uncontrolled changes may result in undesired prod-
uct formation. The controlled changes in the properties of the 4D printed
object under various stimuli can be achieved by coding design and by
proper distribution like a uniform, gradient, or patterned distribution of
their components.
4.2. Model design and printing process
The 4D printing refers to the stimulus-induced changes in 3D printed
model. Hence the model design is critical in the 4D printing process.
The effective software solution is an essential factor in 4D printing as it
enables the manufacture of the desired product. The 4D model design
and printing process involved using a series of software solutions and a
management software solution. It includes one solution for each of five
stages, such as Simulation, Modeling, Slicer, Host/Firmware, Monitor-
ing, and one Printing Management software (Fig. 1).
Simulation is the method of studying the behavior of an object or
a system by mimicking it on a computer application. The simulation
software is generally applied before a product can be designed and gen-
erated, and it reduces the risk of failure prior to actual product develop-
ment. It is based on the process of real phenomena using mathematical
formulas. It helps the user to understand the entire operation without
performing. The simulation technology applied in 4D printing is divided
into two types: simulation using finite element analysis (FEA) software
and software to develop simulation functions (Chung et al., 2017). Mao
et al.,(2015) simulated a 4D printing using FEA simulations of unfolding
and folding conducted using the FEA software ABAQUS (Simulia, Prov-
idence, RI, USA) with a user-defined constitutive model implemented
in a UMAT subroutine, and a reduced-order model (ROM) developed to
simulate rigid body motions of the panels and to investigate the folding
pathways.
Upon completion of the simulation, the 3D design of the printing ob-
ject is developed by using modelling software. Modeling creates a model
of the object with all its properties, which may be similar to the real
object. It generates a 3D design of the object. A few common computer-
based graphics and Computer-aided design (CAD) software used for de-
sign development in food printing are Rhino 6 software and Rhinoceros
5.0. (Liu et al., 2021), SketchUp Pro2015 (Ghazal et al., 2021), etc. The
modelling software does not pass any information regarding the 3D de-
sign to the printer. As a result, the slicer software converts the model to
2D sections that consist of information required for the printer.
Slicer software is computer software used in the majority of 3D print-
ing processes for the conversion of a 3D object model to specific instruc-
tions for the printer. It consists of the editing tools like rotation, scaling,
import, and export to CAD files. In addition, it contains a subdivision
function as Stereo Lithography (STL) file. A low-resolution image can be
converted to a high-resolution image by increasing the degree of elabo-
ration and smoothness (Chung et al., 2017). Slicer software extracts the
plan for the printing (G code). It consists of all the information which
defines the entire printing process. Some of the common slicing software
used in food printing are Slic3r, Simplify 3D, etc.
Once the slicer software makes the G-code (slicer data) ready, it will
transmit it to the printer. The host/Firmware software creates the 3D ob-
ject after connecting a Personal Computer (PC) to the printer. In other
words, the host software controls the printer’s head and bed and analy-
ses the G- data received, and sends G-code to the printer.
In 4D printing, the synthesized 3D object gradually changes its prop-
erties over time. These changes occur when the object is in a suitable en-
vironment. Monitoring software facilitates observation of this stimulus-
induced self-transformation of 4D printed objects and brings necessary
actions if needed (Chung et al., 2017). This monitoring software can be
installed on user devices and can be continuously monitored.
The material used has a prime role in determining the 4D design.
The material must be responsive to the stimuli while being printed layer
M. Navaf, K.V. Sunooj, B. Aaliya et al.
Fig. 1. Flow diagram of software used in 4D printing
by layer. The type of material used will determine the stimuli needed
to trigger the self-transformative changes of printed objects. The expo-
sure of the printed object to the stimuli will not interact with all the
component of the product, only desired component will interact and
leads to the predetermined transformation in the product. The inter-
action mechanisms of the 4D printed object to the stimulating agent
include mechanical loading, or physical manipulation, which results in
a series of changes in the product. Mathematical modelling determines
the extent of exposure to stimuli to attain desired changes in a printed
object (Ahmed et al., 2021). The shape-shifting effect of a single ma-
terial can be achieved by manipulating the gradient distribution of the
material by strategically controlling the special position and morphol-
ogy of the lattice structure throughout the product (Pei & Loh, 2018).
The self changes in the shape of the material depend on the stimulus
responsiveness and physical design geometry of the material (Lendlein
& Kelch, 2002).
The 4D printing process consists of different steps and different soft-
ware. The outcome from one step maybe utilizes the input of the for-
warding steps. Hence the software in each step plays a particular role
and may influence the next step, and all the stages are interconnected
and act as a network. Hence, all the software in each processing stage is
monitored and controlled by the user.It is performed by using a print-
ing management system connected to each software in every stage and
designed to optimize the use of printers (Chung et al., 2017).
4.3. Food printing methods
4.3.1. Extrusion printing
Extrusion-based printing is one of the easiest ways of food print-
ing and has been widely used for food printing. It is generally used
for molten materials using a temperature control or semi-viscous sys-
tem (Mantihal et al., 2020). The first stage in extrusion printing is to
program a virtual 3D model and convert it to individual layer patterns
and unique codes for printing using slicing software. The printing of
food begins with uploading these codes to the printer and selecting the
appropriate recipe. Depending on the programming done, while gener-
ating the item, materials are extruded by moving the nozzle above a
fixed stage or by moving the stage under the nozzle to form a layer. The
extruded layers cling to one another, producing a 3D structure built on
layers (Sun et al., 2018).
The material’s rheological characteristics determine the appropriate-
ness of food for 3D printing. The ease of dispensing and stability in post-
deposition is also important. The material should be stable during post-
printing processing like baking. The smooth dispense of material from
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Applied Food Research 2 (2022) 100150
the extruder through the nozzle requires particular mechanical force.
This force depends on the rheological characteristics of the material and
the geometry of the nozzle (Sozer et al., 2018).
Many researchers used room temperature extrusion for the synthesis
of 4D food products. Chen, Zhang, Guo, et al. (2021) used an extruder
for the synthesis of a 4D printed lotus root powder gel, with a nozzle di-
ameters of 1.2mm and 1.5 mm, gives a rough surface. However, a nozzle
dimension of 0.8mm provides a surface with a smooth surface. Similarly,
a 1.2 mm nozzle diameter is also used in the 4D printing of potato puree
(He, Zhang, & Guo, 2020). Chen et al. (2021) used a nozzle diameter
and layer height of 0.8mm during the printing of purple sweet potato
paste. Similarly, an extrusion-based in-house fabricated delta-type 3D
food printer with a diameter of 0.84 and 1.28 mm was used for the print-
ing of the sago starch turmeric blend (Shanthamma et al., 2021). Print-
ing speed also plays a potential role in extrusion-based food printing.
Printing speeds like 25mm/sec (Ghazal et al., 2019; Ghazal et al., 2021),
20mm/sec (He et al., 2021; He, Zhang, & Devahastin, 2020),18mm/sec
(Shi et al., 2022), etc., are used for the synthesis of 4D printed foods.
4.3.1.1. Room temperature extrusion. It refers to the extrusion of print-
able material like dough and melted cheese at room temperature. Room
temperature extrusion is widely used to make high-repeatability con-
fections, which are not easily made by hand. Pasta printing also can be
done by using room temperature extrusion. The materials like carbohy-
drates (He, Zhang, & Devahastin, 2020), protein (Phuhongsung, Zhang,
& Bhandari, 2020), puree (Shi et al., 2022), etc., have been used as
printing material in room temperature extrusion. Different parameters
such as nozzle dimension, printing speed, extrusion rate, infill percent-
age, layer height, etc., need to be addressed (Gholamipour-Shirazi et al.,
2019).
4.3.1.2. Hot-melt extrusion. Hot-melt extrusion is the process of pro-
duction of new material by heating and melting the raw material. The
molten ink is then forced through a die under controlled conditions. It is
mainly used for the synthesis of polymeric materials. Food materials like
chocolate are extruded at a temperature of 28°C to 40 °C through a mov-
able extrusion printer nozzle (Fig 2), and higher temperatures can also
be attained (e.g., 90 °C). And it gets solidified instantly after extrusion
and sealed to the previous layer. The heat applied in hot melt extrusion
varies with the type of material, and a higher temperature should be
maintained to control the material’s viscosity and flowability through
the printing nozzle. The products synthesized through hot-melt extru-
sion exhibited uniform thickness and density(Tan et al., 2018). Hot-melt
M. Navaf, K.V. Sunooj, B. Aaliya et al.
Fig. 2. Schematic representation of the hot-melt extrusion
Fig. 3. Schematic representation of the hydroforming extrusion
extrusion is gaining much attention because of its ability to solidify and
weld with the adjacent layer immediately after extrusion.
4.3.1.3. Hydroforming extrusion. In the hydroforming extrusion
method, the hydrocolloid solution or dispersion is dispensed to gel
setting/ polymer/ hardening bath using a syringe pipette, jet cutter,
vibrating nozzle, and similar apparatus (Fig 3). In this method, the
viscoelastic characteristics of the materials have a primary role, and it
5
Applied Food Research 2 (2022) 100150
Fig. 4. Schematic representation of the binder jetting
depends on the gel-forming ability of the material (Le-bail et al., 2020).
In this technique, the hydrocolloid solution should exhibit a viscoelastic
characteristic first and then transform into self-supporting gels. A
temporal control mechanism is applied to prevent the pre-gelation of
material in the printer (Godoi et al., 2016). In general hydro gel-forming
involve three mechanisms (1) chemical cross-linking, (2) ionotropic
cross-linking, and (3) complex coacervates formation (Kirchmajer et al.,
2015). This method is widely used for the printing of fruit-based soft
foods.
4.3.2. Inkjet printing
Inkjet printing is also commonly used in 4D printing and is gener-
ally used in confectionery and decorations (Pallottino et al., 2016). It
consists of a series of pneumatic membrane nozzles-jets typically 20-50
μm, which dispense tiny droplets of printing food material to a moving
object. The single and multiple nozzles can work at the same time, and
the printing ink can be sprayed on the printing platform, forming a lay-
ered structure. The drops combine to form a digital image with surface
fillings and cavity depositions. Inkjet printing generally uses low viscous
materials. Hence, it is used to draw flat products than to print complex
structures. The temperature has a significant effect on inkjet printing. It
will affect the viscosity and surface energy of the material (Le-bail et al.,
2020).
Robert John Young describes a machine that contains a bubble-jet
printer head and a storage container for liquid food colorant and is used
to print a picture onto the surface of an edible substrate as previously es-
tablished. A technique of printing an image onto an edible substrate was
also incorporated into this innovation (Robert John Young, 2000). Sim-
ilarly, Pallottino et al. invented an instrument that enhances the print-
ing of low viscous substances on an edible surface by modifying the sur-
face with a high-polarity water-based glaze or polishing the gum surface
(Pallottino et al., 2016). Inkjet printing is generally used for low viscous
substances. Hence, inkjet printing is not suitable for the production of
complex food structures. It finds application in graphical decoration,
fillings, micro-encapsulation, and to some extent, in 3D nano printing
(Fernanda C. Godoi et al., 2018).
4.3.3. Binder jetting
Binder jet printing is an additive manufacturing process. The pow-
dered materials are spread over a fabrication platform. A binding agent,
usually liquid, is sprayed over the powder layer, allowing neighboring
powder layers to be bound together (Fig 4). Unlike inkjet printing, the
binder or ink is only released when required through pulse actuation.
Generally, a counter-rotating roller is used to apply a powder coating to
each layer of the component. To create the layer’s 2D design, the bind-
ing agent in the form of liquid is dispensed through the head of an inkjet
onto the powder bed (S Holland et al., 2018). This technique has the ad-
vantages of being low-cost and requiring less time to operate. However,
the surface finishing is less (Le-bail et al., 2020)
In binder jet printing of food, with the introduction of liquid binder
to the powder materials. Powdered materials will tend to agglomerate
themselves due to higher hygroscopicity and stickiness. The release of
M. Navaf, K.V. Sunooj, B. Aaliya et al.
Fig. 5. Schematic representation of the selective laser sintering
liquid binder to powder particles will enhance the adhesive force among
them. The material properties and its interaction with the binding agent
will affect the binder jetting process. Minimum quantities of a better-
suited material added to hydrophobic or water-insoluble materials can
offer enough interaction to bind; this should be considered at the mate-
rial scoping phase of the binder jetting process (Holland et al., 2019).
4.3.4. Selective sintering
Based on the type of sintering used, selective sintering is divided
into selective laser sintering, selective hot air sintering, and melting.
The basic principle of both sintering methods is similar, consisting of
a sintering agent for fusing powder and forming a solid structure. This
method has an advantage over other methods, developing food struc-
ture without any further treatment within a short period (Le-bail et al.,
2020). Sugar and sugar-rich powder may be sintered to produce a com-
plicated solid structure when done correctly. The sintering agent, either
laser or hot air, travels along the X and Y axes after spreading a layer
of powder to fuse the powder particles. This process is continued until
attaining desired structure (Sun et al., 2015).
Carl Deckard and Joe Beaman invented selective laser sintering in
early 1980. The infrared laser beam is guided to a scanner and reflected
to the printing materials (Godoi et al., 2016). By scanning in a cross-
section motion calculated by the 3D digital description encoded by the
3D software, the laser beam acts as a heat source and selectively sinters
the powder materials (Mantihal et al., 2020) (Fig 5). This is a solvent-
free, high-efficiency printing technique that does not require the poly-
merization of raw material monomers and further post-processing. The
solvent-free nature of this method is ideal for orienting solvent-sensitive
materials. The printed products are immediately available for consump-
tion without further processing, such as drying or curing, except by
harvesting printlets from the loose powder (Charoo et al., 2020). The
powder sintering is greatly influenced by the energy of the input laser
and the wavelength of the laser beam. It depends on the absorptivity.
Hence, laser selection is an important process in this printing technique
(Gu et al., 2012). The interaction between the laser beam and the par-
ticle in powder material is substantial in, explaining the laser sintering
process’s feasibility and quality (Mantihal et al., 2020). In the selective
hot air and melting method, hot air with low velocity is passed to a bed
of powder material, where the X-axis and Y-axis of the beam move in
interchanging motion. The hot air method can sinterize any material in
powder form (Mantihal et al., 2020; Godoi et al., 2016).
4.4. Stimulations in 4D printing
Stimulus is a the primary requirement for triggering changes in
the functionalities, properties, and shape in 4D printed materials. A
6
Applied Food Research 2 (2022) 100150
stimulus may occur through different means, such as physical, chemi-
cal, or biological. Physical stimuli include temperature, moisture, light,
magnetism, and electric energy. The chemical stimulus has pH, ionic
strength, and the presence of chemicals. Glucose and enzymes are
grouped under biological stimuli (Zafar & Zhao, 2020). The few stimu-
lating agents and their impact on 4D food printing are summarized in
Table 1.
4.4.1. Temperature
The most frequent stimulant used in 4D printing is temperature.
Polymers may change or lose their properties by exposure to tem-
perature. Glass transition temperature and ink composition’s melt-
ing temperature are two factors considered when exposed to thermal
stimuli (Pinho et al., 2020). In food hydrogel, the temperature will
cause dehydration and, subsequently, shrinkage or contraction of the
structure, and this temperature-induced transformation is reversible
(Champeau et al., 2020). Microwave heating is a non-contact method
that causes temperature-induced changes in 4D printed objects. Mi-
crowave heating has the advantage of fast heating, high energy effi-
ciency, easy control, and good sanitary conditions, and it has certain
advantages in post-printing processes (Guo et al., 2021). Microwave has
a significant impact on the shape-changing behavior of the 4D object.
The dehydration caused by microwave heating results in the bending
deformation or shrinkage of printed materials (He et al., 2021). It also
facilitates the flavor changes in 4D printed objects by destroying micro-
capsules (Guo et al., 2021).
4.4.2. pH
The impact of pH changes in 4D printed structure and surrounding
medium on the structural and functional properties are highly studied.
The pH-induced color changes in many plant-based food printed mate-
rials are broadly studied. Chlorophyll, carotenoids, and anthocyanin are
major pigments found in fruits and vegetables, and it has a beneficent
effect on human health. (Chandra et al., 2021). The pigment chlorophyll
responsible for the green color is highly sensitive to pH, and the color
degradation is high at lower pH. Similarly, a reduction in carotenoid
content at lower pH was also noticed. Anthocyanin exhibited a red color
at lower pH and yellow color at a higher pH (Ghazal et al., 2021)
4.4.3. Light
The use of light as a stimulating agent in 4D printing permits quick
action and noninvasive stimulation. Hence a specific region of the sam-
ple can be illuminated to cause localized changes in the printed ob-
ject (Kuksenok & Balazs, 2016). Light can penetrate into the printed
structure and generate heat energy in shape memory polymers (Leist
& Zhou, 2016). In the 4D printing process, light-stimulated shape
memory polymers are widely employed in self-assembly structures, so-
phisticated folding techniques, and transformational surface deforma-
tions(Ubukata et al., 2007).
4.4.4. Ionic strength
Ionic strength indicates the amount of dissociated ions in water. The
ionic strength and ionic concentrations will influence the changes in 3D
printed objects (Champeau et al., 2020). Depending on the chemical
nature of hydrogels, ionic concentration has a significant impact on hy-
drogel swelling. Ions help to develop physical interaction (ionic bond)
in charged hydrogels. Divalent or trivalent cations are broadly used to
develop ionic cross-linking in anionic polymers; alginate cross-linked
with divalent metal ion is a typical example of the development of ionic
polymer (Hu et al., 2019).
4.5. Stimuli induced changes in 4D printed food
4.5.1. Changes in color
Stimulus-induced changes in color are most studied in 4D printed
food. Color has become a visual attribute used by consumers to value
M. Navaf, K.V. Sunooj, B. Aaliya et al. Applied Food Research 2 (2022) 100150

Chen, Zhang, Guo, et al. (2021)

Chen, Zhang, Mujumdar, et al.

He, Zhang, & Guo (2020)
He, Zhang, & Devahastin
Phuhongsung, Zhang, &

Phuhongsung, Zhang, &

Ghazal et al. (2019)

Ghazal et al. (2021)

Devahastin (2020a)
Guo et al. (2021)

Bhandari (2020)

Liu et al. (2021)

Shi et al. (2022)
References

(2021)
(2020_
maltol, and eugenol). Increase in bitterness, astringency, umami, richness,

NaHCO3 sprayingchanged the color from reddish/ yellow to green. And a

color changed from red to green-yellow as a function of pH (pH 2 to 10
Shape changing and increase in bending angle with shrinkage ratio and
Increase in a∗ value, and Chroma value and the color changed from

Development of new flavor compounds (1-Octen-3-ol, Maltol, Ethyl

Color changed from red to green by a change in acidic pH to alkali

Transformation of 2D planar flowers and butterflies into 3D

Changes in color at a pH below 6.Lower pH gives a higher

Sample with lower pH shows significant color change

Increase a value, and cinnamaldehyde content

hardness.Changes in flavor at a pH 8 and 10

Spontaneous changes in the shape of puree

Fig. 6. Schematic representation of the impact of pH on the color of 4D printed

food containing anthocyanin
decrease in a∗ and b∗ values

a product before deciding on the purchase. It could help to describe

rate of dehydration

the quality, such as the freshness of the product. It can also set cus-
and saltiness.
yellow to red

tomers’ expectations towards the likely taste and flavor of the product
4D changes
∗

(Chandra et al., 2021). The color of food is due to the presence of dif-
ferent pigments. Some pigments may change their color with changes
in the environment, and the changes in pH may change the chemical
structure. In alkaline pH, curcumin and anthocyanin exhibited red and
green colors, respectively. However, under the acidic condition, it ex-
gelatin-gum Arabic-oil complex, buckwheat dough, yellow flesh peach

hibits yellow and red colors, respectively. This will be exploited in 4D

red cabbage juice, vanillin powder, potato starch and fruit juices

printed food to change color over a storage period by influencing a stim-

ulus like pH, temperature, etc.
soybean protein isolate, k-carrageenan and vanilla flavor

The impact of the microwave stimulation on 4D printed lotus root

powder gel was studied, in which curcumin was used as stimulus-
anthocyanin-potato starch gel and lemon juice gel

response material (Chen, Zhang, Guo, et al., 2021). The printing ink
Lootus root gel, anthocyanins and lemon yellow

was prepared by mixing lotus root powder and water with curcumin
soy protein isolate, pumpkin, and beetroot

mashed potato/purple sweet potato puree

emulsion and was printed by using an extruder printer with a nozzle

diameter of 1.2 mm and 1.5 mm for thick extrusion lines and 0.8 mm
curcumin and lotus root powder gel

diameter for smoother extrusion lines. The exposure of printed 3D struc-

Oleogel and purple potato puree

ture to microwave resulted in changes in color from yellow to red, and

Stimulus and stimulus-induced changes in 4D printed food.

it depends on curcumin concentration and microwave treatment time. A

Purple sweet potato puree

reduction in L∗ and b∗ value and an increase in a∗ value was noticed by

microwave treatment. It also changed the chroma value of the printed
food sample. The changes in color by the exposure to microwave are due
Printing ink

to the movement of the water molecule by microwave heat. It enhances

the alkalinity of the medium in which curcumin is present. The develop-
Starch

ment of higher temperatures will cause changes in emulsion structure.

It may break or aggregate and develop particles with increased size.
The breakdown of emulsion at higher temperatures results in releasing
Microwave, infrared and air

a higher amount of curcumin to the surrounding medium (Kharat et al.,

2017).
Microwave dehydration

Similarly, the impact of microwave stimulation is also studied in

Microwave heating
Microwave heating

Microwave heating

Microwave heating
Stimulating agent

4D printed buckwheat dough (Guo et al., 2021). Multi-material com-

pound with gelatin-gum Arabic-oil complex coacervates microcapsules
dehydration

was used as a stimulus-response material. Microwave treatment en-

Table 1

hanced the redness of the dough, and the lightness got decreased. This
pH

pH
pH
pH
pH

is due to the destruction of the capsule by the exposure of microwave

and with embedded oil released.
Anthocyanin is a water-soluble pigment, and it has pH-dependent
color-changing properties. As shown in Fig 6, It exhibits red color in

7
M. Navaf, K.V. Sunooj, B. Aaliya et al.
acidic pH, purple color under neutral pH, and green under alkaline pH,
and the color intensity increases with storage time (Ibrahim et al., 2011).
Purple sweet potatoes are rich in anthocyanin. He et al. (2020) printed
purple sweet potato puree with a mashed potato by using a dual ex-
trusion printer. Four different pH values of mashed potato are used for
printing, and the mashed potato is printed on the top layer to distin-
guish the color changes easily. The color intensity was increased with
increased storage time and increased amount of purple sweet potato
puree. The L∗ and b∗ values increased, and a∗ value decreased with
mashed potato concentration. This may be due to the reduced diffu-
sion amount of anthocyanin from purple sweet potatoes to mashed pota-
toes. Over the storage time, the mashed potato color changes from white
to red, and it exhibits a color difference between the upper and lower
sides. It is due to the difference in concertation of anthocyanin at dif-
ferent parts. Similarly, a combination of anthocyanin and lemon yellow
as stimulus-responsive material in lotus root gel was studied. The re-
searchers noticed a rapid color change (within 1 min) in a printed ob-
ject from reddish/ yellowish to green by external spraying of NaHCO3
solution (Chen, Zhang, Mujumdar, et al., 2021).
The effect of surface pH on the color change of 3D printed soy
protein isolate, pumpkin, and beetroot mixture rich in betalain was
studied. The researchers observed that at higher pH (above 6), the
printed material did not show any changes in color value after 1 hr
of storage. However, at lower pH, the color values changed signifi-
cantly (Phuhongsung, Zhang, & Devahastin, 2020a). Due to the oxida-
tive degradation of color pigments, the color values changed over an
extended storage period. The color value changes at lower pH are due
to the degradation of color pigments under high acidic conditions. A
significant change in color regarding internal and external pH stimulus
was noticed in 3D printed multi-smart material structure (Ghazal et al.,
2021). The formulation consists of red cabbage juice, vanillin powder,
potato starch (RC-V-P), and fruit juices used as stimulus material. The re-
searchers noticed a reduction in anthocyanin color intensity with potato
starch concentration. It is due to the complex formation of anthocyanin
with starch chains such as amylose and amylopectin (Di Marco et al.,
2020; Lay Ma et al., 2011). The application of different pH-controlled
solutions of pH 2, 3–4, 5–6, 7, 8–9, and 10 on the surface of 3D printed
RC-V-P structure changed the color from blue to red, purple, violet, blue,
blue-green, and green-yellow colors, respectively (Ghazal et al., 2021).
He also noticed the color changes over the storage period in a 3D printed
bilayer structure of RC-V-P and fruit juice gel (apple, orange, and lemon
juice). This color change is due to the internal pH stimulus (migration of
H+ or OH− ions) from the lower layer of fruit juices inside the product,
resulting in reversible structural change in anthocyanin molecules.
4.5.2. Changes in aroma
Food flavor is a vital food property and the most concerned property
from the consumer’s point of view. In 4D printing, the printing pro-
cess, such as ink preparation and alignment of printed layers, provides
a suitable environment for developing characteristic flavor in printed
objects. The preparation of printing ink enhances the chemical reaction
of the flavor compound and facilitates uniform distribution (Teng et al.,
2021). Electronic nose and GS-MS analysis can analyze the changes in
the flavor of constituents of 3D printed food structures.
Vanillin (4-hydroxy-3-methoxy benzaldehyde) is an important food
flavoring agent, and its flavor intensity is highly sensible to differ-
ent stimuli like temperature, pH, moisture, etc. (Frenkel & Havkin-
Frenkel, 2006). Many researchers used vanillin as stimulus-responsive
material in the 4D printing process (Phuhongsung, Zhang, & Bhandari,
2020; Ghazal et al., 2021). Phuhongsung et al. studied the post-printing
microwave exposure of 4D printed objects that contains vanilla flavor as
a compound in printing ink (Phuhongsung, Zhang, & Bhandari, 2020).
The effect of microwaving on flavor was estimated by a discrimination
Index value. The GC- MS noticed the appearance of four volatile com-
pounds (1-Octen-3-ol maltol, ethyl maltol, and eugenol) in a vanillin-
containing structure. However, many volatile compounds reported in
8
Applied Food Research 2 (2022) 100150
previous studies are not found because of the lower concentration of
vanillin (0.5%).
Changes in aroma compounds of microwave treated 3D printed struc-
ture containing gelatin-gum Arabic-oil complex coacervates microcap-
sules as a stimulus-response material is also reported (Guo et al., 2021).
The authors noticed an increase in the amount of volatile flavor con-
stituents such as 1-hexanol, hexanal, and benzaldehyde present in yel-
low peaches and (E)-cinnamaldehyde encapsulated in the microcapsule.
The (E)-cinnamaldehyde exhibits a two-fold increase by a 4 min expo-
sure of microwave. The enhanced aroma of microwave-treated objects
is due to the microwave-induced destruction of the microcapsule, and
the heating facilitates the diffusion of aroma compounds.
A clear difference in aroma of the 4D printed structure containing red
cabbage juice, vanillin powder, and potato starch at different pH was no-
ticed by using an E-nose (Ghazal et al., 2021). The samples treated with
higher pH (pH 9 and 10) showed a lower response, and those treated
with lower pH showed a higher response. The reduced odor strength at
high pH values might be due to the phenol group of vanillin, which has
a pKa of 7.38, being negatively charged and reducing volatility under
basic circumstances (Kan et al., 2017). The effect of different pH on 4D
printed soy protein complex with pumpkin and beetroot powders was
noticed. After 5 hr of spraying, the changes in flavor indicated the for-
mation of new aroma compounds under high pH stimuli (pH 8 and 10)
(Phuhongsung, Zhang, & Devahastin 2020a).
4.5.3. Changes in taste
Food printing technology plays a significant role in forming char-
acteristic tastes because it brings various compounds together to facili-
tate favorable reactions. The changes in taste properties of printed food
samples are examined by e- tongue analysis. Which uses characteristic
eight senses correspond to human tongue perceptions, including sour-
ness, bitterness, astringency, aftertaste-A, aftertaste-B, umami, richness,
and saltiness. The radar chart obtained from e- tongue analysis will de-
scribe the taste perception of the sample analyzed.
Similarly, pH-stimulated changes in taste properties of 4D printed
food multi- smart materials were reported (Ghazal et al., 2021). The
saltiness and umami taste decreased with a decrease in pH value (2-10).
However, the sourness increases with a decrease in pH value. Similarly,
a high saltiness value was reported at a pH of 10 in 3D printed soy
protein isolate, pumpkin, and beetroot mixture (Phuhongsung, Zhang,
& Devahastin, 2020a), and authors noticed higher astringency at lower
pH of 4.
The increased number of hydrogen ions at lower pH values decreases
the pH value of the sprayed solution (Phuhongsung, Zhang, & Deva-
hastin, 2020a). The enhanced saltiness under high pH is due to the
sodium protein interaction, leading to sodium release from printed ob-
jects (Kuo & Lee, 2014). The lower umami taste under acidic conditions
is by the suppression of umami taste under lower pH conditions. Acidic
conditions restrict the binding of phenolic compounds with protein, re-
sulting in a large number of free phenolic compounds at lower pH, which
results in enhanced astringency at a lower pH (Zdunić et al., 2016).
4.5.4. Changes in texture
In the point of consumer acceptance, along with the visual appear-
ance and taste, food texture plays a significant role. In 3D additive man-
ufacturing, the food is developed by layer by layer alignment of the food
inks. Raouf Fahmy et al.developed a 3D printed starch-based food tex-
ture using a dual extruder coupled with near-infrared heating for ther-
mal stabilization (Raouf Fahmy et al., 2021). The authors noticed that
the two factors would influence the textural property of the printed ob-
jects.1) the calculated offsets in the Cartesian coordinates between two
costume extruders. Textural characteristics in the elastic area are unaf-
fected by offsets and minor variations in layer height along the z-axis.
2) the impact of slicing parameters and printing settings on the textual
characteristics. A 4D structure of mashed potato with various internal
structures was created, and the researchers reported that the hardness
M. Navaf, K.V. Sunooj, B. Aaliya et al.
and gumminess of printed objects strongly depend on infill concentra-
tions and perimeters (Liu et al., 2018).
Likewise, a 4D deformation of the pumpkin/ paper double-layer
structure was also noticed. To achieve the goal of 4D directed deforma-
tion, the study concentrated primarily on the structure’s anisotropy and
the directionality of the plane layer. The authors noticed that the hard-
ness of the structure increased exponentially with time, and it shows
a negative correlation with time (F. Chen et al., 2021). The mechani-
cal property of many objects has a great dependence on their moisture
content. The hardness, gumminess, springiness, and cohesiveness of 4D
printed lotus root powder gel were significantly increased by microwave
stimulation (C. Chen, Zhang, Guo, et al., 2021). The sample became
harder after microwave exposure. The heat generated by microwaves
leads to moisture loss and results in a harder and more compact struc-
ture of 4D printed food. The increase in cohesiveness results in a more
strong internal force, and an increase in springiness results in the need
for a higher force to chew the food (Fan et al., 2020).
PH-induced changes in textural properties of a 3D printed soy
protein composite were observed by Phuhongsung, Zhang, & Deva-
hastin, (2020a). The spray of a solution with lower pH (pH 3) results
in an enhanced hardness and gumminess. In addition, the authors no-
ticed that the springiness and cohesiveness of the 3D printed sample
increased with the increased pH of the solution. The agglomeration of
protein molecules at higher pH results in increased springiness and cohe-
siveness of gel. In contrast, applying various pH solutions on 3D printed
red cabbage juice, vanillin powder, and potato starch mixture negatively
affected the texture properties (Ghazal et al., 2021). Among various pH
conditions (2-10), the authors noticed that pH 3 exhibited higher hard-
ness. It could be due to the leaching of starch molecules in a highly
acidic environment (Hirashima et al., 2005). The negative impact of
surface treatment of the 3D printed sample with pH solution is due to
moisture absorption. It may result in reduced hardness of the printed
object.
4.5.5. Changes in shape
The post-printing programmable changes in the structure of 3D
printed objects are referred to as 4D printing. Shape changing of the
printed object can be in any direction, such as from 1D to 1D, 1D to
2D, 2D to 2D, 1D to 3D, 2D to 3D, and 3D to 3D, among which the
switch from 2D to 3D is more common in the food field (Momeni et al.,
2017). For shape-changing, the printing process consists of develop-
ing a bilayer structure with two materials having different expansion
or shrinkage properties under different environments (W. Wang et al.,
2017). The shape-changing behavior of 4D printed materials is based
on three fundamental laws. First law: the relative expansion of active
and passive materials is the main cause of the 4D change of multi-
materials,including coiling, curling, twisting, bending, etc. Second law:
mass diffusion, thermal expansion, molecular transformation, and or-
ganic growth are the four key factors that lead to the 4D changing of 4D
printed multi-materials. Third law: the changes in the shape of all 4D
printed multi-materials are governed by two "types" of time constants.
This constant depends on the type of printing materials and the environ-
mental stimuli (Ahmed et al., 2021). Shape changing of 3D printed food
materials can be stimulated by water hydration processes like cooking
or by dehydration.
4.5.5.1. Changes by hydration. Food hydrogels are shape-shifting ma-
terials in food printing due to their anisotropic swelling capacity
(Stephen et al., 2021). Hydrogels have a cross-linked 3D network struc-
ture formed by either physical or chemical interaction (White et al.,
2013). It consists of an expandable hydrophilic material that facili-
tates shape-shifting under various stimuli (Tao et al., 2019). Hydration-
stimulated shape-shifting creates a unique mouthfeel, achieves pro-
grammable transformation, and easy shipping and storage.
A protein, cellulose, and starch composite film with a shape trans-
form concept were developed, and it changes the dimension from 2D to
9
Applied Food Research 2 (2022) 100150
Fig. 7. Schematic representation of shape-changing (bending) of 4D printed
food
3D by anisotropic swelling during cooking (W. Wang et al., 2017). The
authors developed food film by xPrint to deposit cellulose on gelatin
films by an adjustable dispenser mounted on a CNC platform. Similarly,
the shape-changing of kneaded and sheeted flour-based dough with an
integrated design strategy for morphing food during cooking was ob-
served (Tao et al., 2019).
4.5.5.2. Changes by dehydration. Dehydration is an important food pro-
cessing method, and drying causes various effects on food items, such
as shape and texture changes. Dehydration diffuses moisture from the
sample, which causes stress generation in food, and leads to shrinkage
and bending of the product (Sannino et al., 2005). Hence, dehydration-
induced shape change has excellent scope in 3D printing. Different dry-
ing methods like microwave, osmotic, hot air, etc., apply different mech-
anisms for drying. The moisture content and the shrinkage ratio have a
positive relation, and the dielectric constant loss factor has a negative
relation to the bending angle of a 3D printed object (Liu et al., 2021). A
4D change of pumpkin/paper by dehydration at 25°C was also studied
(F. Chen et al., 2021). The authors found a positive relationship between
the bending angle of a double layer and the drying time.
Similarly, the bending angle of 4D printed starch-based purple sweet
potato puree was increased with an extension in dehydration time
(Fig 7) at different microwave power levels (He, Zhang, & Devahastin,
2020). Shape changing of microwave treated purple potato puree and
oligo gel was reported (Shi et al., 2022). They concluded the existence of
a linear relationship between microwave power, time, and the bending
angle up to a certain extent. At the early stage of microwave treatment,
the bending angle has a great trend with the rise of moisture content
in the slurry (Shi et al., 2022). It is due to the dielectric character of
moisture, which absorbs more microwave and increases the rate of de-
hydration. However, a moisture content below 25% (He et al., 2021)
and a microwave power above 150 W (Shi et al., 2022) did not show
any significant deformation. It may be due to the formation of a rigid
structure at this moisture content, and the sample volume remains con-
stant (J. Wang et al., 2018).
The effect of different dehydration techniques (microwave, infrared
radiation, and air drying) on the shape-changing of 4D printed starch-
based edible structures was reported (Liu et al., 2021). The authors ob-
served a higher bending in the air-dried sample followed by infrared
treated and microwave treated samples. All the simulation shows a
higher rate of bending at the initial time of exposure. In infrared treated
samples, lower temperature treated samples show a higher final bending
angle than those treated at a higher temperature. Higher temperature
exposure results in the formation of a porous structure by accelerated
evaporation, which has a lower volume shrinkage (J. Wang et al., 2018)
The stimulus-induced shape changes of printed samples are influ-
enced by factors such as the interaction between layers and the adhe-
sive property of the printed objects on the surface. The presence of salt
and fructose syrup will also influence the dehydration-induced shape
changes (Liu et al., 2021; He, Zhang, & Devahastin, 2020).
4.5.6. Nutritional changes
Food printing can alter the nutritional content of food based on the
need of consumers. It can be achieved by the introduction of healthy
ingredients such as cellulose, plant chemicals, and high-quality proteins
M. Navaf, K.V. Sunooj, B. Aaliya et al.
and the reduction of adverse substances such as anti-nutritional factors
and allergens. The nutritional supply of printed food can be controlled
by the rational distribution of nutrients in printing ink or alternatives
during printing. The use of fruits and vegetables as a part of food ink
can supply micronutrients, cellulose, and other nutrients (Chen et al.,
2022). The use of tissue engineering in food printing has a potential
role in the nutritional aspects of 4D printing. The replacement of ink
and tissue with food-grade materials in 4D biotechnological printing
will improve the nutritional quality of printed food. Since the exposure
of material with appropriate conditions stimulate the growth of tissues.
The printing object contains plant or animal cells that have the capacity
to form tissue-like structures under suitable stimuli and produce nutri-
ents (Teng et al., 2021). Printing food with probiotics will also enhance
the printed object’s nutrition quality. The incorporation of microalgae
provides additional nutritional, functional components such as protein,
fatty acid, sterol, and vitamins (Uribe-Wandurraga et al., 2020).
UV-irradiation of 4D printed purple sweet potato pastes incorporated
with ergosterol resulted in significant improvement in vitamin D2 con-
tent (Chen et al., 2021), and an increase in vitamin D2 content has
been noticed in the irradiated area. Similarly, microwave stimulated
beeswax-based oleo gel- purple potato powder ink produced a low fat
printed product (Shi et al., 2022)
4.6. Challenges and future aspects in 4D food printing
4D food printing is in the stage of infancy. Hence it is open for great
exploration for research. In the present scenario, 4D printing is carried
out by using traditional 3D printing equipment; hence the development
of new printing conditions or equipment with improved functionality
will simulate the 4D printing. It will help to easily attain the required
changes like deformation and denaturation of different components of
food ink. At present, the researchers mainly focus on microwave heating
and changes in pH as a source of stimulus. However, the new stimulus
agents like light, changes in ionic concentration, etc., can be explored in
4D food printing. Similarly, the number of stimulus-response materials
studied in 4D food printing is limited. The new component like diacetyl,
vanillin, etc., could be studied. The use of multiple stimulus-responsive
materials to bring out target simultaneous changes in multiple proper-
ties of food will be a breakthrough in 4D food printing. Developing a
monitoring system to evaluate the degree of 4D changes could play a
potential role in obtaining controlled changes in 4D.
5. Conclusion
The 4D printing is an extension of prevailing additive manufactur-
ing like 3D printing, which has the ability to a spontaneous change in
printed configurations under stimuli. The 4D food printing is gaining
attention in the field of both academic and industrial sectors. The 4D
printed food may change color, flavor, texture, and shape. At present,
the exploration of 4D food printing is restricted to a few materials such
as starch hydrogel, soy protein, and potato puree. Most of the works fo-
cus on microwave heating or changes in pH as a source of stimulating
agents. Stimulus-induced changes in the color of 4D printed food are ex-
plored to a large extent. However, the changes in texture and shape can
be explored more. And the use of multiple stimulus-response materials
in food ink can be recommended, which may help to observe multiple
changes in the 4D printed object under stimuli.
Ethical statements
This study does not involve any animal /humans
Declaration of Competing Interest
The authors have no conflicts of interest
10
Applied Food Research 2 (2022) 100150
Acknowledgement
The authors are grateful to Dr. Shijin. A, Government of Kerala.
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