Food Hydrocolloids 131 (2022) 107760

Contents lists available at ScienceDirect

Food Hydrocolloids
journal homepage: www.elsevier.com/locate/foodhyd

Bioaerogels as food materials: A state-of-the-art on production and

application in micronutrient fortification and active packaging of foods
Pavidharshini Selvasekaran , Ramalingam Chidambaram *
Instrumental and Food Analysis Laboratory, School of Biosciences and Technology, Vellore Institute of Technology, Vellore, Tamil Nadu, 632014, India

A R T I C L E I N F O A B S T R A C T

Keywords: Bioaerogels labeled as “solid smoke” are third-generation advanced food materials. Due to their unique prop­
Bio-polymers erties such as high surface area, low density, highly porous structure, and biodegradability, studies on bio­
Food-grade aerogels aerogels have drawn widespread attention among researchers worldwide. The success of bioaerogels in the
Micronutrient fortification
pharmaceutical industry has encouraged their potential as advanced materials suitable for food-related appli­
Food packaging
cations. Bioaerogels are being used as carrier matrices of various compounds and possess a huge potential in the
micronutrient fortification of foods. The high mechanical stability, high thermal stability, and water holding
capacity of bioaerogels are desired for the production of food packaging materials. However, bioaerogels as food
materials are not commercialized and research on their direct application into food products should gain a
foothold among the scientific community. In this review, state-of-art on the production of bioaerogels as food
materials are discussed. The literature on various carbohydrate polymers that are used as precursors for the
production of bioaerogels was emphasized. Further, their benevolent effects on micronutrient fortification and
active packaging of foods are comprehended.

1. Introduction
The rapidly emerging focus on bioaerogels is evident with the
increased number of scientific publications available in the literature
over the past two decades. The keyword search of “Bio-aerogels” in one
of the utmost approached scientific databases (https://www.sciencedi
rect.com/) displayed over 2262 research dating from 2001 to
February 2022. About 80% of research articles have been published
dating from 2011 which specifies the increasing interest in bioaerogels
among the scientific community. The journals that have published high
number of research articles on bioaerogels include Carbohydrate Poly­
mers, Food Hydrocolloids, International Journal of Biological Macromole­
cules, The Journal of Supercritical Fluids, Chemical Engineering Journal,
Polymer Contents, Journal of Colloid and Interface Science, Carbon, Ad­
vances in Colloid and Interface Science, Journal of Hazardous Materials, and
European Polymer Journal. In terms of this subject area, most of the
publications in the above-mentioned journals were on pharmaceutical
applications, drug delivery, wound healing, and environmental sciences.
However, literature focusing on the application of bioaerogels in food is
still limited.
Bioaerogels in common are synthetic porous lightweight materials
derived from hydrogels by replacing the liquid present in the gel
structure with gas. They have lower density, higher mechanical
strength, high pore volume, and larger surface area. Bioaerogels are
fabricated into different shapes and sizes and are commonly used as
carriers, catalysts, and supporting materials (García-González, Jin,
Gerth, Alvarez-Lorenzo, & Smirnova, 2015a). Using polysaccharides,
proteins, and seed mucilages as aerogel matrix has additional advan­
tages as they are biobased, biodegradable, and recognized as safe for
food-related applications. The commonly used biopolymers for the
production of bioaerogels include starch, cellulose, alginate, pectin,
carrageenan, konjac glucomannan, whey protein, egg white protein,
seed mucilages, etc., (Selvasekaran & Chidambaram, 2021b). These
biopolymers are approved for use in food products as gelling agents,
carrier matrices, emulsifiers, thickeners, and stabilizers. They possess
excellent gelation ability and form a hydrogel upon interaction with
water or a suitable solvent, di-cations, presence of co-polymers, and
crosslinking agents (Mikkonen, Parikka, Ghafar, & Tenkanen, 2013).
Further, the bioaerogels are fabricated from hydrogel by employing an
appropriate drying method which is generally supercritical CO2 drying.
The dried bioaerogels in various shapes and sizes hold ultra-low density,
higher porosity, and higher specific surface area which specifies its

* Corresponding author.
E-mail addresses: pavidharshiniselva58@gmail.com (P. Selvasekaran), cramalingam@vit.ac.in (R. Chidambaram).

https://doi.org/10.1016/j.foodhyd.2022.107760
Received 17 February 2022; Received in revised form 5 April 2022; Accepted 25 April 2022
Available online 28 April 2022
0268-005X/© 2022 Elsevier Ltd. All rights reserved.
P. Selvasekaran and R. Chidambaram
widespread possibilities for application as novel food materials (Gar­
cía-González, Alnaief, & Smirnova, 2011).
Concurrently, food researchers and industries are constantly facing
novel technological challenges in terms of micronutrient fortification
and food packaging materials. Micronutrient fortification plays a sig­
nificant role in the enhancement of bioactive functionalities and the
nutritional profile of packaged foods and beverages. Despite a large
extent of research being undertaken, still there are technological de­
mands to protect sensitive micronutrients (Ephrem, Najjar, Charcosset,
& Greige-Gerges, 2018). One such emerging technological advancement
is the hypothesis of manufacturing bioaerogels and loading them with
sensitive micronutrients. Moreover, bioaerogels are considered as an
upcoming environmental-friendly and economical approach to occupy
the food packaging sector. In relevance to this, the current work was
categorized into five major sections-the state of art on fabrication pro­
cesses of bioaerogels focusing on hydrogel formation, alcogel formation,
and drying methods (section 2), evaluation of the commonly used pre­
cursors of bioaerogels (section 3), methods to characterize important
physicochemical properties of bioaerogels suitable for food applications
(section 4). Nevertheless, its potential application in micronutrient
fortification and active packaging of food products is emphasized (sec­
tions 5 and 6).
2. Production of bioaerogels
The key parameter in the production of bioaerogels is to obtain a
three-dimensional (3D) structure with lower density, higher porosity,
exceptional mechanical and thermal stability, and higher specific sur­
face area (Selvasekaran & Chidambaram, 2021b). The production of
bioaerogels is initiated by the dissolution of bio-polymer in water or a
suitable aqueous solution leading to the formation of hydrogel (de Oli­
veira et al., 2020). The gelation of biopolymers is induced by the use of
physical or chemical crosslinking promotors such as pH and temperature
or crosslinking agents, respectively. The aqueous phase held in the
wet-gel structure is eliminated and replaced with a suitable solvent
leading to the formation of alcogel (Dogenski, Navarro-Díaz, de Oliveira,
& Ferreira, 2020). Later, bioaerogels are obtained by entirely removing
the solvent from alcogel through an appropriate drying method (Soor­
baghi et al., 2019). Fig. 1 represents various stages of bioaerogel
production.
2.1. Gelation of precursors
Gelation is the preliminary process that involves the addition of
biopolymers such as polysaccharides, proteins, and seed mucilages
Fig. 1. Schematic representation of bioaerogel formation.
2
Food Hydrocolloids 131 (2022) 107760
either in water or an appropriate solvent (usually ethanol or ionic liq­
uids), which upon interaction causes the dissolution of biopolymers
(Soorbaghi et al., 2019). The hydrogel formation is facilitated by the use
of crosslinking promotors which can be either physical or chemical in
nature. Depending on the type of cross-linking during the gelation
mechanism, the hydrogel can be denoted as either physical or chemical
hydrogel. Moreover, the nature of crosslinkers and their mode of
incorporation into the biopolymer solution determines the kinetics
involved in the gelation and processing approaches to produce bio­
aerogels with various morphology and size (García-González, Jin, Gerth,
Alvarez-Lorenzo, & Smirnova, 2015a). Zhu et al. (2019) reported that in
the physical hydrogel, biopolymers form a gel in an aqueous solution
without any additive or additional gelling treatment. E.g., under
appropriate conditions (temperature or pH), the gelation mechanism of
polysaccharides occurs due to the formation of weak and reversible
chemical interactions between polymeric chains such as hydrogen
bonding and electrostatic interactions. Alnaief and Smirnova (2011a)
used inorganic salts such as calcium chloride, calcium carbonate, cal­
cium sulfate, sodium chloride, and potassium chloride to promote the
weak interactions in the physical gelling process. The use of chemical
crosslinking agents provides better control over the pore structure, ho­
mogeneity, and swelling kinetics of resulting bioaerogels (Camponeschi
et al. 2015). An increase in hardness and decrease in adhesiveness was
reported in starch bioaerogels which were produced by using trisodium
citrate as the chemical crosslinker. The uniform pore distribution and
high crystallinity index (38%) were obtained in chemically crosslinked
starch bioaerogels than those without trisodium citrate (23%) (Abhari,
Madadlou, & Dini, 2017). Likewise, a homogenous structure with
fibrillated network and high chemical stability was reported in wheat
starch bioaerogels that were chemically crosslinked with sodium
metaphosphate. However, at human body temperature, bonds in bio­
aerogels formed by the use of chemical crosslinkers are reported to be
irreversible which subsequently delays their biodegradation (Ubeyito­
gullari, Brahma, Rose, & Ciftci, 2018). Internal setting and diffusion
method are the two commonly approached chemical crosslinking
methods. The former offers controlled and slow crosslinking providing
sufficient time for biopolymer and crosslinker interaction whereas the
latter involves a longer duration of crosslinking. Bioaerogel monoliths
obtained from pectin hydrogels crosslinked with CaCl2 through the in­
ternal setting method revealed uniform crosslinking due to a slow
crosslinking pattern. Bioaerogels obtained through crosslinking by the
diffusion method presented uniformly crosslinked dense structure due to
the longer duration of crosslinking (Veronovski, Tkalec, Knez, & Novak,
2014).
Bioaerogels with high performance can be obtained by choosing an
P. Selvasekaran and R. Chidambaram Food Hydrocolloids 131 (2022) 107760

appropriate hydrogel formulation such as the concentration of bio-
polymer, pH, the functional group of the biopolymer, and the cross-
linking agent (Maleki et al., 2016). De Marco, Baldino, Cardea, and
Reverchon (2015) proved that the source and concentration of the
biopolymer significantly influence the morphology and porosity of the
resulting bioaerogels. Potato starch aerogels obtained by varying the
concentration of starch dissolved in water (5–15% w/w) exhibited
closed pores at 10% w/w. Wheat starch aerogels at 5% w/w and higher
concentration up to 15% w/w exhibited nanoporous structure with
microparticles and lenticular structure with closed pores, respectively.
Irrespective of the biopolymer concentration, aerogels obtained from
maize starch (5–15% w/w) presented a nanoporous structure with
microparticles.
The density of hydrogel which subsequently influences the end
structural characteristics of bioaerogels can be modified by mixing,
reinforcing, or blending the precursor with co-polymer. Ahmadi,
Madadlou, and Saboury (2016) blended whey proteins with micro­
crystalline (MCC) and nanocrystalline (NCC) cellulose particles. The
obtained hydrogels exhibited densities in the range of 1.09–1.2 g/cm3.
Blending the whey protein with MCC had no influence on the density
whereas blending with NCC decreased the density of hydrogel. This
effect was attributed to the surface charge dissimilarity between the
NCC and MCC particles. Upon increasing the concentration of the pre­
cursor κ-carrageenan, Manzocco et al. (2017) documented declined
network density, whereas Alnaief, Obaidat, and Mashaqbeh (2018)
documented improved textural properties and large particle size in
bioaerogels.
Ionic strength and pH of the hydrogel are significant parameters that
influence the end characteristics of protein-based bioaerogels (Selmer,
Kleemann, Kulozik, Heinrich, & Smirnova, 2015). reported high surface
area (380 m2/g) and a well-structured network in bioaerogels obtained
from egg white hydrogels with low (especially at pH 2) and high pH than
bioaerogels (16 m2/g) derived from hydrogels with pH 4.6 nearer to the
isoelectric point of the egg white protein (Kleemann, Selmer, Smirnova,
& Kulozik, 2018). documented that egg white hydrogels with pH 11.5, 9,
3.5, and 2 produced bioaerogels with homogeneous and dense structure
whereas at pH 4.6 bioaerogels with coarser network and heterogenous
structure were achieved. The former was attributed to the delayed ag­
gregation process during gelation as a strong repulsive force was formed
between egg white protein molecules. Contrary, rapid aggregation
occurred in the latter as a consequence of insufficient repulsive force
between egg white protein molecules. Moreover, strong attraction be­
tween the partly negative and partly positive egg white protein subunits
at pH 4.6 created numerous aggregates leading to a heterogenous and
coarser network (Selmer et al., 2015). Similarly (Betz, García-gonzález,
Subrahmanyam, Smirnova, & Kulozik, 2012), observed that at neutral or
basic pH, whey protein hydrogels yielded bioaerogels with 310–388
m2/g of high surface area and high mechanical stability.
2.1.1. Emulsion gelation
Selmer et al. (2019a) indicated that for direct application into food,
bioaerogels in the form of microspheres are highly preferred. Emulsion
gelation is the commonly used gelation method to obtain bioaerogels in
the form of microspheres. Therefore, this review was mainly focused on
elaborating the production of hydrogel through the emulsion gelation
method. Table 1 enlists the structural characteristics of bioaerogels
obtained through emulsion gelation.
Emulsion gelation (in situ production) technology facilitates the
production of hydrogel microspheres with predefined size and
morphology. Integrating the sol-gel process with solvent exchange and
supercritical drying of gel-oil dispersion is a versatile and robust method
for the industrial production of biodegradable aerogel microspheres
(Alnaief, Alzaitoun, & Smirnova, 2011). Fig. 2 represents the emulsion
gelation method that involves- 1) preparation of dispersed phase
through the process of sol-gel; 2) immersion and emulsification of
dispersed phase in a continuous phase (generally vegetable oil immis­
cible with the dispersed phase); 3) formation of stable gel microspheres
through crosslinking or gelation within the dispersed phase (Alnaief &
Smirnova, 2011b; García-González, Camino-Rey, Alnaief, Zetzl, &
Smirnova, 2012). The commonly utilized oils to prepare the continuous
oil phase include rapeseed oil (Athamneh et al., 2019), paraffin oil
(Mohammad Alnaief et al., 2018), and sunflower oil (Kleemann et al.,
2018). Alnaief et al. (2011) for the first time presented the emulsion
gelation method to fabricate biodegradable alginate hydrogel and sub­
sequent bioaerogel microspheres. Water-in-oil emulsion (1:5 ratio) was
obtained by incorporating sodium alginate solution (dispersed phase)
into vegetable oil (continuous phase) containing Tween® 80 (0.2 wt %)
as the surfactant. The emulsification was performed in a beaker under a
certain stirring speed using a marine propeller for 15 min followed by
the addition of 0.05 M CaCl2/paraffin oil + glacial acetic acid as the

Table 1
Structural characteristics of various bioaerogel microspheres produced through emulsion gelation.
Bioaerogel source Chemical Surfactants Specific Pore Bulk density Pore Mean particle Total Reference
crosslinkers Surface volume (g/cm3) diameter size (μm) porosity
area (m2/ (cm3/g) (nm) (%)
g)

Corn starch (52.6% – Polyglycerol 93 0.69 – 24–25 1.2 87.7 Goimil et al. (2017)
amylose content) polyricinoleate
(PGPR)
Corn starch – Glyceryl 34–120 0.12–0.36 – – 215–1226 – García-González,
(Amylose monostearate Camino-Rey, et al.
content- 52.6%) (2012)
Alginate/ Calcium Span® 80 446–611 – 0.035–0.063 – 33.0–40.0 97.6–98.7 Athamneh et al.
hyaluronic acid carbonate (2019)
κ-carrageenan, Potassium Span® 80, 34–174 0.10–0.54 0.06–0.50 7.4–16.5 06.67–189.91 – Alnaief et al.
Carrageenan chloride, Span® 85 (2018)
suitable for gel Potassium
preparation, carbonate,
Carrageenan type Aluminum
I chloride,
Potassium Iodide
Whey protein – – 354 1.55 241 14.0 66.6 – Selmer et al.
isolate (2019a)
Egg white protein – – 232 2.28 179 41.7 32.7 – Selmer et al.
(2019a)
Sodium Caseinate – – 48 0.28 443 13.4 40.9 – Selmer et al.
(2019a)

-: Not mentioned.

3
P. Selvasekaran and R. Chidambaram
Fig. 2. Steps involved in the emulsion gelation process.
crosslinking agent through diffusion method/internal setting method,
respectively.
García-González and Smirnova (2013a) reported that emulsion
gelation does not influence the textural properties of bioaerogel mi­
crospheres whereas the particle morphology including particle size
distribution, mean particle size, and roundness is determined by various
factors including aqueous phase-oil ratio, rotator/stator design, agita­
tion speed, and surfactant concentration, etc. Alnaief and Smirnova
(2011b) established an emulsion gelation method to fabricate bio­
aerogel microspheres with controlled particle size distribution. The
study reported that the particle shape and size distribution of bio­
aerogels was influenced by the sol: oil volume ratio. Among the various
sol: oil ratios (2:1, 1:1, 1:2, and 1:3), no microspheres were obtained
from 2:1 due to the larger sol phase than the continuous oil phase. This
condition did not facilitate the formation of sol droplets in the contin­
uous phase instead during the process of gelation the dispersed sol phase
was moved to a separate continuous gel phase. The mean particle size of
the bioaerogel increased (in the order 1:1 < 1:2 < 1:3) upon a simul­
taneous increase in the continuous oil phase volume. This is due to the
decrease in the volume of the dispersed phase, particle coalescence, and
frequency of collisions during agitation which results in the formation of
spherical microspheres with less particle aggregation (García-González,
Uy, et al., 2012). Similarly, Jeffery, Davis, and O’Hagan (1991) observed
the influence of sol: gel ratio on the mean particle size which decreased
upon simultaneous reduction in the volume of the continuous phase.
Contrarily, Gabor, Ertl, Wirth, and Mallinger (1999) reported that the
volume of the continuous phase did not exhibit a significant effect on the
mean particle size distribution. In a study conducted, increasing the
aqueous solution: oil ratio (1:1, 1:2, 1:3) resulted in round particles with
a narrow particle size distribution, however, it did not influence the
mean particle size (García-González, Uy, et al., 2012). It is important to
highlight that influence of volume ratio between sol (dispersed phase)
and oil (continuous phase) on the particle size distribution of bioaerogel
microspheres is not completely understood.
The shape and stirring rate of the agitator during emulsion gelation
have a significant effect on the particle shape and size distribution of
bioaerogels (García-González & Smirnova, 2013a). For instance, parti­
cles that are not uniform in shape and containing breakages were ob­
tained using a four-bladed radial stirrer with a high stirring rate ranging
between 1000 and 1800 rpm. The same agitator upon lowering the
stirring rate to 800 rpm produced gel particles that are spherical with a
diameter ranging between 100 and 200 μm. However, it is not possible
to produce gel particles <100 μm using four-bladed radial stirrers as the
tip of the blade applies high shear stress on gel particles during the
process of mixing (Alnaief & Smirnova, 2011b). Moreover, high collision
energy amplified by the irregular flow profile causes destruction and
abrasion of the microspherical gel particles as they collide with vessel
4
Food Hydrocolloids 131 (2022) 107760
walls. To overcome these issues, a two-bladed axial stirrer with a smooth
flow pattern and high input energy was used to obtain microspherical
gel particles at a higher stirring rate (>1800 rpm) (Alnaief & Smirnova,
2011b). In another study, a marine propeller stirrer with a diameter of 5
cm was used to emulsify the alginate: oil phase in the ratio of 1:2 by
differing the revolution speed between 200 and 1400 rpm. Increasing
the revolutionary speed subsequently resulted in very high energy input
allowing the formation of a large interfacial surface area. As an outcome,
the dispersed sol droplets in the continuous oil phase became smaller in
size which subsequently produced microspherical bioaerogels with
smaller particle size distribution (Alnaief et al., 2011). García-González,
Camino-Rey, Alnaief, Zetzl, and Smirnova (2012) concluded that higher
the stirring rate lower is the particle size distribution of spherical gel
particles. A decrease in the mean particle diameter from 40.0 to 33.0 μm
and 51.4–22.5 μm was observed for alginate-hyaluronic acid and algi­
nate bioaerogel microspheres, respectively upon increasing the stirring
rate from 850 to 1200 rpm. This was attributed to the higher energy
input and higher shear-thinning behavior of both the polymeric
solutions.
Generally, surfactant (stabilizer) is incorporated into the continuous
oil phase to prevent droplet coalescence. A decrease in the mean particle
size can be achieved by elevating the surfactant concentration as it de­
creases the interfacial surface tension between the two phases of the
emulsion (Alnaief & Smirnova, 2011b). As an example, the substantial
increase in the concentration of Span® 80 (0–3 vol %) declined the mean
particle diameter of alginate bioaerogel microspheres from 259 to 115
μm. Emulsion gelation coupled with diffusion method of crosslinking
and containing 0.2 wt % Tween® 80 as a surfactant in the oil phase
resulted in less aggregated spherical alginate aerogel particles. In the
case of emulsion gelation involving the internal setting method of
crosslinking, higher surfactant concentration (5 vol% Span® 80) was
required to obtain uniform spherical gel particles (Alnaief et al., 2011).
The major advantage of emulsion gelation includes eliminating the need
for chemical crosslinkers. García-González, Camino-Rey, et al. (2012)
formed biodegradable corn starch bioaerogels excluding the usage of
chemical crosslinkers by adapting the process of emulsion gelation along
with the use of a lipophilic surfactant (3% (w/w) of glyceryl mono­
stearate). The sphericity of gel particles was largely improved by the
surfactant as it decreased the size of dispersed phase droplets and
enhanced the stability of the water-in-oil emulsion. However, the low
specific surface area (34–120 m2/g) of resulting bioaerogels was indi­
cated as the major drawback. Although bioaerogels with particle size
ranging between 10 and 100 μm were obtained through emulsion
gelation, Goimil et al. (2017) for the first time produced
one-micron-sized bioaerogel microspheres by immersing the starch
aqueous solution into paraffin oil (1:2 ratio) containing polyglycerol
polyricinoleate (PGPR) (3% w/w) as an emulsifier and using ultrasound
P. Selvasekaran and R. Chidambaram
probe as the vigorous agitation method. Due to PGPR presence, the
surface of starch-based bioaerogels seemed wrinkled and porous
partially coated with fused particles. However, the removal of PGPR
resulted in a one-fold increase in the surface area (93–188 m2/g) and
pore volume (0.69–1.25 cm3/g).
Apart from other parameters, the viscosity of the dispersed and
continuous phase holds a key role in controlling the particle size dis­
tribution of bioaerogels. A decrease in the inner phase viscosity leads to
a reduction in the coalescence resistance capacity of the droplets and
results in broadening of the particle size distribution (Athamneh et al.,
2019). Broadening of the particle size distribution was detected due to a
continuous increase in viscosity of the sol phase over time with constant
viscosity of the continuous phase (1000 cP) (Alnaief et al., 2011). This
was in agreement with the results of Alnaief and Smirnova (2011b) in
which broadening of the particle size distribution was reported as the
viscosity of the dispersed phase continuously increased over time while
maintaining constant viscosity of the continuous phase (50.8 cP) (Gar­
cía-González, Uy, et al., 2012). suggested that broadening of the particle
size can be avoided by evenly distributing the energy throughout the
entire volume of the emulsion.
Amid the process of sol-gel, the dissolution of biopolymer in ethanol
produced bioaerogels with lower surface area ranging between
100–300 m2/g and higher density ranging between 0.3 and 0.4 g/cm3.
This was due to the dissolution of ethanol (15 wt % at 25 ◦ C and 25 wt%
at 40 ◦ C) into the continuous oil phase during emulsion gelation which
led to the shrinkage of gel particles. This issue was answered by satu­
ration of the oil phase with ethanol before the emulsification process
(Alnaief & Smirnova, 2011b). Interestingly, Alnaief et al. (2018) proved
that the temperature maintained throughout the emulsification in­
fluences textural properties as well as particle size. Increasing the tem­
perature during the emulsification process decreased the viscosity of the
aqueous and oil phase which reduced the interfacial tension between the
two phases. The aqueous carrageenan solution and paraffin oil were kept
in the water bath at various constant temperatures viz., 90 ◦ C, 75 ◦ C, and
65 ◦ C. The particle size of the gel particles produced at 90 ◦ C and 75 ◦ C
was slightly lower than those prepared at 65 ◦ C. The surface area and
pore volume decreased from 160 to 65 m2/g and 0.43–0.17 m3/g
respectively with an increase in the temperature from 65◦ C to 90 ◦ C.
Moreover, a slight influence of temperature on surface charge and pore
diameters was also observed.
2.1.2. Dissolution of precursors into other solvents
The use of ionic liquids is the rapidly emerging green technology for
the gelation of biopolymers which eliminates the use of toxic and vol­
atile organic solvents. The resulting gels significantly differ in physical
characteristics from those obtained by dissolution into water (hydro­
gels) and are scientifically termed ionogels (Agostinho et al., 2020).
Ionic liquids are reported to have a stronger affinity for polysaccharides
and their ionic character is particularly effective for the dissolution and
extraction process. The use of ionic liquids in the pharmaceutical in­
dustry continues to be controversial due to their biodegradability and
toxicity. However, low toxicity ionic liquids can be prepared by opting
for biocompatible and non-toxic anions and cations (Kadokawa, 2011).
Agostinho et al. (2020) used imidazolium ion-based ionic liquids for the
dissolution of κ-carrageenan and analyzed the resulting bioaerogels in
comparison to bioaerogels derived by the dissolution of κ-carrageenan
into the water in the presence of potassium salt as a crosslinking agent.
The stabilization effect of imidazolium ion on the double helix network
of κ-carrageenan gel allowed less volume shrinkage of resulting bio­
aerogels. The larger dimension and asymmetry of the imidazolium ion
led to numerous macropores in aerogels. On the contrary, high volume
shrinkage of 90% and homogeneous distribution of mesopores were
detected in bioaerogels obtained by dissolution into the water and
containing potassium salt as a crosslinking agent. Lopes et al. (2017a)
used high and low melting ionic liquids derived from alkylmethylimi­
dazolium as a dissolution media for the gelation of micro-crystalline
5
Food Hydrocolloids 131 (2022) 107760
cellulose. The resulting bioaerogels revealed less volume shrinkage
with pore volume, pore diameter, and specific surface ranging between
0.3 and 2.4 cm3/g, 7.9–34 nm, and 154–434 m2/g, respectively.
κ-Carrageenan bioaerogels with 90% of pores (100 μm) and good ho­
mogeneous structure were obtained by using lettuce homogenate as a
dissolution media for biopolymer gelation. Due to the reduction in
volume contraction, they presented lower firmness and low network
density with only a 4% decrease in total porosity than those bioaerogels
prepared by dissolution into water (Plazzotta, Calligaris, & Manzocco,
2019).
2.2. Alcogel formation
Alcogel formation is the second step which is generally obtained
through the solvent exchange method. Owing to the lower affinity of
water molecules to the supercritical CO2 drying process, it is crucial to
replace the water with a suitable solvent in the pores of the hydrogel
structure (Şahin, Özbakır, İnönü, Ulker, & Erkey, 2017). The existence of
slight droplets of water in micropores of the hydrogel could lead to
substantial modifications in the pore structure of bioaerogels upon su­
percritical drying. The common approach in the formation of alcogel is
the replacement of water and Stievano and Elvassore (2005) suggested
the use of alcohol or acetone as they are highly soluble in supercritical
CO2 fluid. Solvent exchange is commonly done in a one-step or
multi-step process. Wang and Zhao (2009) performed one-step solvent
exchange by directly soaking the hydrogel in the new solvent, whereas
the multi-step solvent exchange process involves sequential soaking of
hydrogel in a solution containing varying concentrations of water and
new solvent (generally ethanol). The latter is frequently employed in
which the concentration of the new solvent is gradually increased in
each subsequent soaking procedure (Subrahmanyam, Gurikov, Dier­
inger, Sun, & Smirnova, 2015). Considering the applications in food, the
chosen solvent to replace water should satisfy the requirements such as
a) should be accepted for manufacturing of food products, b) should not
dissolve the gel structure, c) should be completely soluble in water
(Alnaief & Smirnova, 2011a). De Marco et al. (2015) demonstrated that
the time taken during the process of solvent exchange influences the
porosity and morphology of bioaerogels. The solvent exchange time was
varied from 2 h to 24 h. Potato starch aerogels (10% w/w) at 2 h and 24
h of solvent exchange time exhibited closed pores and fibrous nano­
structures, respectively. The former was attributed to the insufficient
time required for the formation of alcogel. On the contrary variation in
the solvent exchange time did not influence the morphology of wheat
starch (5–15% w/w) and maize starch bioaerogels (5–15% w/w). In
both cases, 2 h of solvent exchange time was sufficient for the formation
of alcogel.
2.3. Drying
Drying is a significant process that involves the elimination of sol­
vent held in pores of alcogel without altering the shape and dimensions
while retaining the highly porous structure of the dissolved phase (De
Marco et al., 2015). The commonly employed methods to remove the
aqueous phase of alcogel include freeze-drying and supercritical drying.
Table 2 enlists structural characteristics of bioaerogels obtained through
freeze-drying or supercritical CO2 drying.
Freeze-drying is a cost-efficient, environmentally friendly, easily
applicable, and favorable technique for the fabrication of bioaerogels
with extremely ordered and controlled porous structures (El-Naggar,
Othman, Allam, & Morsy, 2020). Freeze-drying can also be performed
by excluding the solvent exchange process (Giannouli & Morris, 2003).
Kumar, Mishra, Reinwald, and Bhat (2010) performed freeze-drying of
wet-gel by lowering the temperature of the fluid contained in the pore
below its triple point followed by vacuum application and controlled
sublimation at the isobaric condition. The sublimation of water
decreased the specific surface area and led to the formation of
P. Selvasekaran and R. Chidambaram Food Hydrocolloids 131 (2022) 107760

Table 2
The end structural characteristics of bioaerogels obtained by supercritical CO2 drying or freeze-drying.
Bioaerogel source Drying Specific Pore volume (cm3/g) Bulk density (g/ Pore Mean Total Reference
method surface area cm3) diameter particle porosity (%)
(m2/g) (nm) size (μm)

Wheat starch SC-CO2 52.6–59.7 0.09–0.27 0.05–0.29 20 – – Ubeyitogullari and

drying Ciftci (2016)
Corn starch (70% SC-CO2 313–362 0.17–0.63 0.120–0.185 – – – Kenar et al. (2014)
apparent amylose)- drying
sodium palmitate
Wheat starch (25% SC-CO2 48.9 0.19 0.13 16.5 – 91.7 Ubeyitogullari et al.
amylose and 75% drying (2018)
amylopectin)
Alginate 4% (w/v) Freeze- – – 0.6158 expressed 1081 – 65.60 Chen and Zhang
drying in (g/mL) (2019)
Alginate/Pectin (1:1)- Freeze- – – 0.2970 expressed 215 – 66.70 Chen and Zhang
4% (w/v) drying in (g/mL) (2019)
Apple fruit pectin (2% SC-CO2 213 0.339 – 7.5 – – Veronovski et al.
w/w) drying (2014)
Citrus fruit pectin (2% SC-CO2 248 0.39 – 7.4 – – Veronovski et al.
w/w) drying (2014)
Citrus fruit pectin (1% SC-CO2 143 0.214 – 7.2 – – Veronovski et al.
w/w) drying (2014)
Apple fruit pectin (1% SC-CO2 515 0.95 – 8.7 – – Veronovski et al.
w/w) drying (2014)
κ-carrageenan SC-CO2 – 0.308 – – – 94.3 Plazzotta et al.
drying (2019)
κ-carrageenan Freeze- – 0.004 – – – 95.9 Plazzotta et al.
drying (2019)
κ-carrageenan SC-CO2 123–221 0.32–0.52 – – – – Agostinho et al.
drying (2020)
Microcrystalline SC-CO2 154–434 0.3–2.4 – 7.9–34 – – Lopes et al. (2017a)
cellulose drying
Nanofibrillated cellulose Spray- 80–100 – 0.012–0.033 10–100 – 98–99% Jiménez-Saelices
aerogels freeze et al. (2017)
drying
Konjac glucomannan/ Freeze- – – 0.0201–0.0524 – – 92.49–97.17 Wang et al. (2018)
potato starch/gelatin drying
Nanocrystalline Freeze- 1.72 0.0025 – – – – Ahmadi et al. (2016)
cellulose/whey drying
protein blend
Microcrystalline Freeze- 3.04 0.0078 – – – – Ahmadi et al. (2016)
cellulose/whey drying
protein blend
Whey protein isolate SC-CO2 390–422 1.27–1.69 – 9.2–14.0 – – Kleemann et al.
drying (2020)
Egg white protein SC-CO2 220–378 1.56–2.79 – 13.8–17.4 – – Kleemann et al.
drying (2020)
Sodium Caseinate SC-CO2 42 0.24 – 9.2 – – Kleemann et al.
drying (2020)
Silk fibroin SC-CO2 424 – 0.058 5–130 – – Marin et al. (2014)
drying
Soy protein SC-CO2 384–478 0.12–0.15 (micropore); 0.19–0.25 – 4–50 – Amaral-Labat et al.
drying 1.72–2.29 (mesopore); (2012)
1.41–2.72 (macropore)
Flax mucilage (10% w/ SC-CO2 201.1 0.82 0.16 – – – Comin et al. (2015)
w) drying
Balangu seed mucilage SC-CO2 95.74 0.368 – 1.29 – – Falahati and
(0.04 gr/ml) drying Ghoreishi (2019)
Camelina seed mucilage SC-CO2 228.7 0.28 0.05 5.6 – 94.3 Ubeyitogullari and
concentrate (10% w/ drying Ciftci (2020)
w)
Camelina seed mucilage SC-CO2 239.5 0.32 0.08 6.0 – 91.0 Ubeyitogullari and
powder (10% w/w) drying Ciftci (2020)

-: Not mentioned.

macropores in the resulting bioaerogels. The drawback of freeze-drying
includes the formation of microcrystals, structural shrinkage, high en­
ergy consumption, and prolonged processing time (Ni et al., 2016).
Structural imperfections occurred in whey protein aerogels as the ten­
dency to trap air bubbles increased during freeze-drying (Chen, Wang, &
Schiraldi, 2013). The pre-freezing temperature set during freeze-drying
influences the properties of bioaerogels. For instance, smaller pores in
konjac bioaerogels were formed by reducing the pre-freezing tempera­
ture (− 40 ◦ C to − 15 ◦ C). At 25 ◦ C uniform pore size distribution and
regular structure were obtained (Ni et al., 2016). Moreover, the reduc­
tion in thermal degradation and volume shrinkage in konjac bioaerogels
were reported upon lowering the pre-freezing temperature (Li, Ye, Zhou,
& Li, 2014). Recently, Jiménez-Saelices, Seantier, Cathala, and Grohens
(2017) adapted a novel approach called spray-freeze drying to produce
bioaerogels with a reduced pore size (nanometric scale). The
nano-crystalline cellulose wet-gel was first sprayed into the mold that
was earlier cooled down to − 80 ◦ C followed by freeze-drying. The ob­
tained bioaerogel monoliths exhibited homogeneous structures with

6
P. Selvasekaran and R. Chidambaram
reduced pore size. The advantages of spray-freeze drying over typical
freeze-drying are rapid freezing and prevention of structural deforma­
tion of bioaerogels.
Supercritical drying is an alternate drying method employed to
overcome complications associated with traditional and freeze-drying.
Large surface <3000 m2/g, densities <0.004 g/cm3, and high porosity
(85–99%) are inherent by definition to bioaerogels fabricated through
the process of supercritical drying (García-González & Smirnova,
2013a). Kleemann et al. (2020) reported that supercritical CO2 drying
protects the nanoporous structure of alcogels by avoiding pore collapse.
The supercritical CO2 drying is generally conducted with various sol­
vents such as scCO2 (supercritical carbon dioxide), Xe, and N2O. How­
ever, the most advisable fluid for the process of hydrogel/alcogel drying
is scCO2 due to its moderate critical point conditions (304 K, 7.4 MPa)
and Generally Recognized As Safe (GRAS) status (García-González et al.,
2015a). Based on the contact zone between the gel structure and scCO2
fluid, supercritical CO2 drying is distinguished into three types-dynamic
supercritical drying, static supercritical drying, and direct supercritical
drying. The commonly used dynamic supercritical drying process in­
volves exposing the alcogel to scCO2 fluid in a continuous flow pattern
(Miβfeldt et al., 2020) whereas static supercritical drying subjects the
alcogel to the batch flow of scCO2. In direct supercritical drying, the
wet-gel is dried by operating above the critical point of the solvent
contained in the gel (Mujumdar, Benali, & Boumghar, 2014). García-­
González et al. (2015a) mentioned that the phenomenon of pore
collapse and structural shrinkage was avoided by direct supercritical
drying due to the availability of scCO2 fluid in pores with no other liquid
phase. However, it resulted in the loss of surface tension of resulting
bioaerogels. Supercritical drying prevented volume shrinkage and only
2–3% was observed in κ-carrageenan aerogels due to the good chemical
interaction between supercritical CO2 and the ionic groups of κ-carra­
geenan (Ganesan & Ratke, 2014). Similarly (Lee, Kang, Jeong, Potthast,
& Liebner, 2017), reported that supercritically dried cellulose aerogels
exhibited a volume shrinkage of 9.5% which was lower than those ob­
tained from freeze-drying (11.7%). The solvents utilized during alcogel
production and their miscibility with scCO2 fluid play a key function in
influencing the properties of bioaerogels. For instance, pectin aerogels
produced by using acetone during solvent exchange presented <630
m2/g of high specific surface area and <0.065 g/cm3 of low density
whereas the use of ethanol presented comparatively low specific surface
area of <570 m2/g of and high density of <0.11 g/cm3. This was
attributed to the lower miscibility of ethanol with supercritical CO2 than
acetone (Groult & Budtova, 2018a). Whey protein aerogels produced
through supercritical drying presented a low density of 0.021 g/cm3
than the freeze-dried aerogels (0.070 g/cm3). Moreover, the former
presented less particle aggregation and a highly porous surface (Plaz­
zotta, Calligaris, & Manzocco, 2020). The optimization of the depres­
surization rate of supercritical drying is important to obtain desirable
properties of bioaerogels. The depressurization rate was found to be
negatively correlated with the specific surface area and total volume of
starch aerogels. The internal morphology of starch aerogels was highly
disrupted by a faster rate of depressurization than the slow rate of
depressurization (Kenar, Eller, Felker, Jackson, & Fanta, 2014). The
overvaluation of the supercritical CO2 drying period is the general
routine to ensure the overall elimination of remanent solvents used
during the alcogel formation. Nevertheless, García-González and Smir­
nova (2013a) found that prolonged supercritical drying time deforms
the morphology and textural properties of bioaerogels. In a study, a
supercritical drying period of 30 min yielded 102 m2/g of lower surface
area in starch aerogels. Upon increasing the drying time to 1-h, 91.8% of
solvent elimination with 274 m2/g of specific surface area was attained.
Although 99.1% of solvent elimination was attained after 1 h of drying,
textural properties and the mechanical stability of starch bioaerogels
were unfavorable (García-González, Camino-Rey, et al., 2012). The
drawbacks of supercritical drying include the use of large volume of
solvent during long solvent exchange step and use of high pressure and
7
Food Hydrocolloids 131 (2022) 107760
temperature during drying. This highly curtails the chance of scaling up
bioaerogels into industrial or pilot scale. This is also associated with high
energy and time consumption which elevates the overall production cost
of bioaerogels (El-Naggar et al., 2020).
Rarely used drying techniques include traditional drying, ambient
pressure drying, microwave drying, and vacuum drying. Traditional/air
drying alters the gel structure of alcogel and results in the formation of
xerogel. Xerogel is defined as a gel in which the liquid phase is elimi­
nated using air drying in an open atmosphere (Nayak & Das, 2018). Air
drying develops liquid-vapor menisci in alcogel pores which subsides
upon draining the gel pore. The surface tension of the liquid present in
nanopores of alcogel produces a capillary pressure gradient in pore walls
leading to major disadvantages including pore collapse, structural
shrinkage, and formation of macropores (García-González et al., 2011).
Ambient pressure drying is based on passivation of the pore surface of
wet gels which hinders the formation of new chemical bonds during the
drying process. After solvent evaporation, the obtained bioaerogels
present large volume shrinkage and insufficient porosity (Zuo et al.,
2015). Ambient pressure drying is applicable for the bulk manufacturing
of bioaerogels at an industrial scale, however, the evaporation of sol­
vents during drying emits pollution that is harmful to humans, animals,
and the environment (El-Naggar et al., 2020). Vacuum drying is a highly
energy-conserving technique as the wet-gel is dried under low pressure
and requires less heat for rapid drying. Microwave drying produces
three-dimensional bioaerogels with mesopores and micropores. The
bioaerogels obtained by microwave drying are similar to those aerogels
fabricated by freeze-drying but the former presents small-sized macro­
pores. However, microwave drying and vacuum drying are industrially
unfavorable as they form large pores, reduce the surface area and
collapse the end structure of bioaerogels (Zuo et al., 2015).
3. Biopolymers used for the production of bioaerogels as food
materials
3.1. Starch
Starch, the plenteous polysaccharide obtained from plants consists of
amylose and amylopectin as the two major components with multifar­
ious applications in the food industry. Amylopectin is a (1 → 4)-α-D-
glucan containing higher-density branches whereas, amylose is a rela­
tively linear (1 → 4)-α-D-glucan containing few counts of lengthy
branches, and both are connected to the backbone by α-(1 → 6) bonds
(Mikkonen et al., 2013). The branched structure of starch forms a
three-dimensional network upon interaction with water. The gelation of
starch is done in three steps, a-swelling by absorption of water molecules
in the hydrophilic region of starch granules; b-gelatinization through
heating of the dissolved starch which results in the gradual release of
amylose, permanent physical changes, and destruction of starch granule
structure; c-retrogradation which involves the formation of hydrogel
structure upon cooling, aging, particle reorganization, and fractional
recrystallization (García-González et al., 2011). However, increasing the
retrogradation time during the fabrication of starch aerogels decreases
the specific surface area. This can be avoided by decreasing the retro­
gradation time or completely excluding the process of retrogradation
(Druel, Bardl, Vorwerg, & Budtova, 2017). Villegas, Oliveira, Bazito,
and Vidinha (2019) reported that hydrogel formation is influenced by
the amylose content and gelatinization temperature of starch. Amylose
provides amorphous character to the formed gel structure and addi­
tionally contributes to the mesoporous structure. Starch containing a
higher content of amylose rapids the rate of retrogradation, increases the
resistance rate to volume shrinkage, and increases the specific surface
area while decreasing the density of the aerogels. However,
starch-containing pure amylose with a heterogenous structure does not
form aerogels as they do not sustain the drying pressure (Druel et al.,
2017). It was proved that the higher gelatinization temperature pro­
motes the amylose release from the starch granule structure which
P. Selvasekaran and R. Chidambaram
increases the crystallinity, rigidity, and density of aerogels (García-­
González et al., 2011). Despite the advantages of starch as the raw
material for bioaerogel production, the low hardness of the resulting
aerogel is a major drawback. Zhu (2019) indicated that the mechanical
property of starch aerogels could be enhanced during the preparation
process through the modification of raw starch. Abhari et al. (2017)
modified starch by crosslinking with trisodium citrate which decreased
the adhesiveness and improved the hardness of aerogels.
3.2. Cellulose
Cellulose has a relatively linear structure composed of β-(1 → 4)
linked D-glucopyranosyl units and represents the largest class of bio­
aerogels obtained from polysaccharides. The properties of cellulose are
mostly dependent on the degree of polymerization and length of the
polymer chain (Lopes et al., 2017a). Cellulose aerogels are generally
prepared through the classic aerogel preparation method. The gelation
of cellulose can be induced by two main gelation methods, a-gel for­
mation by dissolving the cellulose in a suitable solvent such as ionic
liquids or water solution containing NaOH (Gupta, Singh, Agrawal, &
Maji, 2018); b-utilizing cellulose nanofibers prepared from either micro
fibrillated cellulose or bacterial cellulose. Further, the cellulose hydrogel
undergoes supercritical drying after the multistep solvent exchange
process (Blanco et al., 2018). Wang, Su, et al. (2019) improved the
mechanical property of cellulose bioaerogels through the use of cellulose
nanocrystals as biopolymers and the obtained bioaerogels were termed
cellulose nanowhiskers. The source of cellulose is a major parameter
determining the morphology of aerogels. de Oliveira, Bruni, Fabra, et al.
(2019) produced composite bioaerogels from polyvinyl alcohol and
cellulose nanocrystals obtained from three different sources-eucalyptus,
oat, and rice. Better interconnected pores and well-organized three-di­
mensional structure was observed in rice cellulose aerogels than oat
cellulose aerogels whereas the eucalyptus cellulose aerogels exhibited
well-organized structures with smaller pores. Hemicellulose is closely
associated with cellulose whereas it is structurally different and exists in
the plant cell wall. Among the hemicellulose xylans, xyloglucan, and
β-glucan have been extensively investigated as bioaerogels (Comin,
Temelli, & Saldaña, 2012; Long, Shen, Wang, Tian, & Hu, 2019). The
backbone of the xylan is composed of β-(1 → 4) linked D-xylopyranosyl
units. The potential substitute for xylans includes α-L- arabinofuranosyl
groups, acetyl, feruloyl, and α-D-glucopyranosyl uronic acid. Oat and
tamarind galactoxyloglucan is another captivating glucan with the po­
tential for the production of bioaerogels as food materials (Mikkonen
et al., 2013). However, it is important to mention that the pure cellulose
aerogels devoid of hemicellulose fractions offered greater density and
compacted structure than those containing hemicellulose (Farhat, Lees,
Macdonald-Clarke, & Amirabdollahian, 2019).
3.3. Alginate
Alginate consists of 1,4-linked-β-D-mannuronic acid (M) and α-L-
guluronic acid (G) which is a polydisperse polysaccharide with a linear
structure. Gelation of alginate occurs through crosslinking with divalent
cations (commonly calcium) and forms a novel egg box structure (Gar­
cía-González et al., 2011). Crosslinking is accomplished either by
diffusion method which involves the stepwise dropping of the solution
containing alginate into the cationic source solution (Escudero, Robit­
zer, Renzo, & Quignard, 2009), or internal setting method involving the
controlled release of cross-linking ions into the alginate solution (Alnaief
et al., 2011). Alginate has a high potential to attract cations due to the
presence of G-blocks as well as hydroxyl and carboxyl groups in its linear
structure (Dekamin et al., 2018). reported that the cationic content,
sequence, and ratio of G-to-M influence the gelling properties of the
alginate which correlates with hydrogel structure and the pore size of
resulting bioaerogels. Alginate exists in different forms such as free
carboxylic acid, alginate, and alginic acid which extensively function as
8
Food Hydrocolloids 131 (2022) 107760
gelling agents, thickening agents, and stabilizing agents in food in­
dustries. Sodium alginate is soluble at pH < 4, and between pH 6–9 it
possesses stable and viscous characteristics (Wang, Su, et al., 2019). The
shrinkage of alginate aerogels occurs during the conversion of hydrogel
to alcogel. The increased concentration of ethanol in the hydrogel dur­
ing solvent exchange rapids the water release and declines the surface
tension, thus decreasing the capillary pressure as well as gel volume
(Mehling, Smirnova, Guenther, & Neubert, 2009). The shrinkage of
aerogels was reduced by increasing the concentration of alginate and
employing a multistep low-frequency solvent exchange process. Later,
the supercritical drying fabricated alginate aerogels in various forms
such as monoliths, beads (<1000 μm), and microspheres (Wang, Su,
et al., 2019). High alginate concentration alters the morphology of
aerogels from nanofibrous to nanoporous (Antonyuk, Heinrich, Gurikov,
Raman, & Smirnova, 2015). proved that Eudragit® (pharmaceutical
polymer) based coating improved the mechanical property and pre­
vented structural deformation of alginate bioaerogels (<50%) against
the relative humidity. The mechanical property can also be improved
through covalent or ionic crosslinking (e.g., CaCO3, CaCl2, and ZnCO3
salts that release divalent metal cations Ca2+ and Zn2+). Double catalytic
performance can be achieved in alginate aerogels by integrating cova­
lent and ionic crosslinking (Selvasekaran & Chidambaram, 2021b).
3.4. Pectin
Pectin is termed as a linear polysaccharide composed of galacturonic
acid with different degree of esterification (DE). Based on the DE, pectin
can be distinguished as high-methoxy pectin (DE >50%) and low-
methoxy pectin (DE <50%) (Groult & Budtova, 2018b). The hydrogels
are formed by thermal or acidic and cationic treatment for high methoxy
and low methoxy pectin, respectively. In thermal-induced gelation, the
heat applied increases the pectin dissolution in water through the
establishment of hydrogen bond interactions between the free carbox­
ylic groups present in pectin and hydroxyl groups on the adjacent
molecules (Gawkowska, Cybulska, & Zdunek, 2018). Moreover, the
addition of cosolute such as acids and sugars (usually sucrose >55%) is
required to form a gel structure with high stability which induces the
partial dehydration of high-methoxy pectin. This is evident as Kastner,
Einhorn-Stoll, and Senge (2012) revealed that the sucrose present in
pectin improved the gel firmness and significantly decreased the
shrinkage rate during the solvent exchange and drying. Instead of su­
crose, ethanol, t-butanol, or dioxane can also be used as cosolute. A
small concentration of t-butanol or ethanol strengthens the hydrophobic
interactions whereas the inclusion of dioxane weakens the hydrophobic
interactions. Thermal/acidic treatment is time-consuming and as a so­
lution, ethanol-induced gelation can be adapted which involves the
dissolution of pectin only into ethanol to obtain a stable gel structure.
Tkalec, Knez, and Novak (2015a) employed ethanol-induced gelation by
adding 10% v/v absolute ethanol into pectin solution for the rapid
preparation (<12 h) of high-methoxy pectin bioaerogels. The advan­
tages of ethanol-induced gelation include the elimination of supple­
mentary substances such as acids or sugars, no temperature elevation,
rapid gelation, and low requirement of organic solvent as this method
does not require solvent exchange before supercritical drying. However,
ethanol-induced gelation for the formation of bioaerogels remains a
topic of interest. In cationic treatment, the low methyl esterified pectin
interacts with divalent cations (usually Ca2+) to form pectin hydrogel
through the renowned egg-box gelation. De Cicco et al. (2016) produced
low methoxy pectin bioaerogels that are devoid of crosslinkers through
amidation of the galacturonic acid content of pectin. Apart from the
gelation mechanism, the pectin source significantly influenced the aer­
ogel structure. The higher pectin content provided a dense and uniform
structure. The aerogels obtained from 2% amidated low methoxy apple
fruit pectin (AF) exhibited a uniformly crosslinked dense structure than
those obtained from 1% AF (Veronovski et al., 2014).
P. Selvasekaran and R. Chidambaram
3.5. Carrageenan
Carrageenan is a high molecular weight polysaccharide commonly
used as a thermally reversible gelling agent in food industries. The
chemical structure is comprised of repeating units of galactose and 3,6-
anhydrogalactose, both sulfated and nonsulfated linked by alternating
α-1,3 and β-1,4- glycosidic linkages. The sulfated functional group reacts
with the solvent utilized during the solvent exchange process and causes
extensive volume shrinkage of aerogels. E.g., the use of acetone or
ethanol as a solvent declined the water molecules that are present sur­
rounding the sulfate ions and repulsive forces between the carrageenan
molecules resulting in 33% of volume shrinkage (Ganesan & Ratke,
2014). Based upon the anhydrogalactose content as well as the location
and number of sulfate groups, carrageenan can be categorized into three
types: κ-carrageenan (kappa), ι-carrageenan (iota), and λ-carrageenan
(lambda). Monovalent cations such as potassium, rubidium, and
caesium are used as crosslinking agents for κ-carrageenan, whereas for
ι-carrageenan divalent cations (usually calcium) are used. However
(Selvasekaran & Chidambaram, 2021b), described that the trivalent
(Al+3) cation and divalent (Ca+2) cation are least effective in comparison
to monovalent cation (K+). The shape and size of bioaerogels obtained
from κ-carrageenan were retained with dual pore structure upon the
incorporation of 0.6 M potassium thiocyanate (KSCN) as a crosslinker
(Ganesan & Ratke, 2014). Similarly, bioaerogels formed by adding 0.6 M
potassium chloride (KCl) and 1 wt % KCl exhibited 200–230 m2/g of
surface area with overall pore volume ranging between 0.9 and 1.4
cm3/g and a round structure with fewer aggregates, respectively
(Robitzer, Di Renzo, & Quignard, 2011). Regardless, the use of cross­
linkers λ-carrageenan cannot form a stable gel and is considered not
suitable for bioaerogel production. The chemical modification of
carrageenan is being studied as an efficient method for remodeling its
mechanical properties for aerogel production (Wang, Su, et al., 2019).
Till today, κ-carrageenan above 4 wt% has not been studied for aerogel
production as the precursor dispersion is extremely viscous and prob­
lematic to handle. The fabrication of carrageenan bioaerogels in the
form of microspheres by adapting the emulsion gelation technique re­
mains unexplored (Alnaief et al., 2018).
3.6. Agar
Agar is composed of galactose and 3,6-anhydrogalactose units which
is structurally similar to carrageenan except it contains lower content of
sulfate. Agar consists of a combination of agarose and agaropectin, the
components that dissolve in the water around 85 ◦ C (Mikkonen et al.,
2013). The agar fractions with the potential to form gel have a molecular
weight above 100 kg/mol, whereas the non-gelling fractions of agar
consist of agaropectin. It has been reported that agarose, at a tempera­
ture exceeding 359 K existed as a disordered random coil and formed a
stable gel structure when cooled to room temperature (Alnaief &
Smirnova, 2011a). Robitzer, Di Renzo, et al. (2011) produced agar
hydrogel bead structure by rapidly boiling the agarose solution (2%
w/w) in a microwave oven at 85 ◦ C. The solution upon cooling was
added dropwise into the cooling water bath using a syringe. The ob­
tained bead hydrogel was subjected to solvent exchange with ethanol
and supercritically dried. The drying method strongly influenced the
aerogels as freeze-drying resulted in lower density and air drying
resulted in extensive shrinkage (Alnaief & Smirnova, 2011a).
3.7. Konjac glucomannan
Konjac glucomannan is a straight-chain high molecular weight
polymer containing D-mannose and D-glucose linked by β-1,4 glycosidic
bonds. The skeleton unit consists of free carboxylic and hydroxylic
groups in abundance, which contributes to the formation of a desirable
cross-linked structure and possesses the property to attract multivalent
cations (Selvasekaran & Chidambaram, 2021b). At present, appropriate
9
Food Hydrocolloids 131 (2022) 107760
physical or chemical strategies are being explored to obtain modified
glucomannan with astonishing properties suitable for the formation of
bioaerogels as food materials (Xin et al., 2017). The thermal insulation
properties of bioaerogels rely upon reduced pore size and high thermal
conductivity. Wang et al. (2018) improved the thermal insulation
property of konjac glucomannan bioaerogels by forming a closed pore
structure, thickening the pore wall, and decreasing the pore size through
the addition of starch and gelatin as co-polymer. The molecular chain of
glucomannan compounded with starch and gelatin induced the forma­
tion of closed and opened pores, respectively. The pore structure of the
konjac aerogels can be controlled by the use of a stabilizer and initial
konjac glucomannan concentration. Uniform pore structure was ob­
tained through the addition of a suitable stabilizer (0.10% glyceryl
monostearate) during the gelation and a reduction in the pore size was
attained with increasing concentration of konjac glucomannan
(0.1–0.5% w/v) (Ni et al., 2016).
3.8. Xanthan gum and guar gum
Xanthan gum and guar gum are other polysaccharides rarely
explored for the production of bioaerogels as food materials. Tkalec,
Knez, and Novak (2015b) produced pure xanthan gum and guar gum
aerogels with a specific surface area of 370 m2/g and 110 m2/g,
respectively. The use of crosslinkers was avoided by performing
ethanol-induced gelation. Also, this method eliminated the need for
solvent exchange before supercritical drying and reduced the overall
production time. Aerogels obtained from xanthan gum were mechani­
cally stable due to the denser crosslinking by ethanol-induced hydro­
phobic interactions and presented dual pores, whereas the guar gum
aerogels were highly brittle with the presence of macropores. However,
both the aerogels eventually degraded after immersion into the solution
containing phosphate buffer, water, or simulated gastric fluid (Tkalec
et al., 2015b).
3.9. Gum tragacanth
Gum tragacanth produces high viscosity solutions but requires 24 h
of hydration to reach the maximum viscosity and form a hydrogel.
Highly porous hybrid aerogels were fabricated from the blend of gum
tragacanth (GT) and polyvinyl alcohol (PVA). The blending ratio
significantly influenced the end properties of bioaerogels. Increasing the
concentration of GT (1:1–3:1) decreased the bulk density, reduced the
stiffness, and the volume of micropores and mesopores fell from 11.29 to
7.62 cm3/g. Also, larger pores with less branched microstructure were
noted. The highest surface area of 1029.20 m2/g was obtained at a 1:1
ratio of GT: PVA which was attributed to the presence of numerous small
pores in their fine structure (Niknia, Kadkhodaee, & Eshtiaghi, 2020).
3.10. β-glucan
β-glucan has a strong gel-forming capacity as they are highly viscous
and are used as edible film-forming material, dietary fibres, gelling
agent, water holder, etc. (Selvasekaran, MahalakshmiRoshini, Angalene,
ChandiniSunil, & Chidambaram, 2021). The gelation mechanism of
β-glucan is one of the important parameters involved in the production
of β-glucan aerogels. For instance, barley β-glucan is soluble in water,
whereas yeast β-glucan is not water-soluble. Therefore, the gelation
mechanism differed between both, where the cold set gelation was
employed for the former and the heat set gelation for the latter. Even
though the morphological and structural characteristics of β-glucan
aerogels obtained from both sources were similar, the yeast β-glucan
aerogels presented high density, high mechanical strength, and
high-water holding capacity (Salgado et al., 2017).
P. Selvasekaran and R. Chidambaram
3.11. Egg white
Egg white has a high tendency to undergo gelation upon thermal
denaturation. Swelling experiments revealed that egg white protein
aerogels remain stable and do not undergo structural collapse upon
contact with aqueous media. Emulsion gelation and supercritical drying
are predominantly employed for the production of egg white aerogels
(Selmer et al., 2015). Selmer et al. (2019a) produced egg white protein
aerogel microparticles with 41.7 nm, 32.7 μm, 2.28 cm3/g, 179 kg/m3,
and 232 m2/g of mean pore diameter, mean particle size, pore-volume,
bulk density, and specific surface area, respectively, for food applica­
tions (Selmer et al., 2015). reported that the source of egg white and its
protein concentration influences the structure of aerogels. The aerogels
obtained from spray-dried egg white with 10 wt % or 15 wt % of protein
contents were pH-independent, better connected, and denser in com­
parison to pasteurized egg white (10 wt% of protein content) aerogels.
The former aerogels presented high surface area, mesopores, and small
macropores. This was due to high degree of denaturation of the dried
egg white than the pasteurized which induced stronger interactions of
egg white protein molecules. The addition of sodium chloride during the
gelation of egg white increased the total porosity and decreased the
surface area of aerogels. The charges present on protein molecules were
covered by salt ions due to insufficient repulsive forces and faster ag­
gregation. As a result, the end aerogels exhibited a coarser and visible
structure. The mechanically stable egg white aerogels can be obtained
by increasing the pH above the isoelectric point (Selmer et al., 2015).
3.12. Silk fibroin
Silk fibroin, obtained from the cocoon of a Bombyx mori silkworm, is
a natural protein used for various food applications, especially in the
edible coating of fruits and vegetables. Marin, Mallepally, and McHugh
(2014) produced silk fibroin aerogels that exhibited density and surface
area of about 0.058 g/mL and 424 m2/g, respectively. It presented
mesopores with pore size distribution ranging between 5 and 130 nm.
Also, the textural properties of silk fibroin aerogels were observed to be
similar to that of whey protein aerogels as reported by Betz et al. (2012).
The combined phenomenon of macropore collapse by capillary force
and ionic interaction between the protonated amino and de-protonated
carboxylic groups of the protein molecules resulted in ~ 46% of volume
shrinkage in aerogels.
3.13. Sodium caseinate
Sodium caseinate aerogels were first produced by Kleemann et al.
(2018) in the form of monoliths from enzymatically crosslinked sodium
caseinate hydrogels. Gelation was induced by the enzyme trans­
glutaminase in a concentration of 10 U/g sodium caseinate. However,
the slow gelation process caused shape deformation and during emul­
sion gelation, this was compensated by the addition of fat with a melting
point of 44 ◦ C. As the casein molecules were covalently crosslinked, the
enzymatic gelation inhibited the disintegration of aerogels into swelling
solution (pH 6.8). However, the major drawback of enzymatically
crosslinked sodium caseinate aerogels is their low surface area (42
m2/g) in comparison to heat-denatured egg white (220–378 m2/g) and
whey protein aerogels (384–422 m2/g). This was attributed to the faster
aggregation and random crosslinking of casein protein molecules
(Kleemann et al., 2020). (Kleemann et al., 2018) reported that higher
substrate concentrate (15.0% (w/w)) is required to induce covalent
bonds between casein molecules, increase the stiffness, and enhance the
mechanical stability of sodium caseinate bioaerogels. Selmer et al.
(2019a) produced sodium caseinate bioaerogels with 40.9 μm, 13.4 nm,
443 kg/m3, 0.28 cm3/g, and 48 m2/g of mean particle size, mean pore
diameter, bulk density, pore-volume, and specific surface area,
respectively.
10
Food Hydrocolloids 131 (2022) 107760
3.14. Soy proteins
Soy proteins are derived as a by-product of the soybean oil industry
and they are highly demanded as food supplements. Soy protein aerogels
were fabricated by Amaral-Labat et al. (2012) using tannins as the
crosslinking agent and employing heat-induced gelation followed by
supercritical drying. The pH values set during the gelation significantly
influenced the end properties. Gelation of the initial dispersion occurred
at a pH ranging between 5.5 and 9, whereas pH outside this range did
not induce gelation. Several mesopores with a diameter ranging be­
tween 4 and 50 μm were observed and these pores appeared extremely
smaller in aerogels obtained at higher pH values. The volume shrinkage
of ~ 25% and ~ 31% was reported at pH 5.5 and pH 9, respectively.
Following this study, soy protein + nano fibrillated cellulose composite
aerogels were fabricated with increased mechanical property in acidic
pH however, volume shrinkage of ~27% was recorded upon
freeze-drying (Arboleda et al., 2013).
3.15. Whey proteins
Whey proteins possess a high tendency for irreversible aggregation
to develop a well-crosslinked gel network appropriate for the fabrication
of bioaerogels for food applications. Whey proteins are advantageous as
they aid the fabrication of water-insoluble and dry aerogels. During the
thermal gelation, covalent disulfide bonds form between the whey
proteins and avoid the structural collapse of aerogels in the aqueous
environment (Betz et al., 2012). Poor mechanical strength is the main
downside of whey protein bioaerogels. A ten-fold upsurge in the me­
chanical stability of whey protein aerogels was achieved through Na+
ion crosslinking during the thermal gelation (Chen et al., 2013). re­
ported that the blending of whey proteins with copolymers increased the
initial viscosity of the precursor solution and the mechanical properties
of aerogels. For instance, the techno-functional and textural character­
istics of whey protein aerogels were controlled by microcrystalline and
nanocrystalline cellulose particles as copolymers. Lower elasticity was
observed in whey protein bioaerogels containing microcrystalline cel­
lulose particles which were incompatible with whey protein molecules
due to their less surface charge and micron size. The higher orientation
of nanocrystalline cellulose towards the positively charged whey protein
domains was favorable and served as cross connectors to enhance the
elasticity of whey protein bioaerogels (Ahmadi et al., 2016).
3.16. Potato protein
Potato protein isolate as a precursor for bio-aerogel production was
first reported by Andlinger et al. (2020). One of the significant
gel-forming proteins present in potato tuber is patatin. Alike other
protein aerogels, the pH of the hydrogel was found to be the decisive
factor influencing the characteristics of aerogels. At low pH values, the
aerogels were brittle with high specific surface area, whereas at pH close
to the isoelectric point of patatin (pH 5) aerogels were brittle with low
specific surface area. The highly stable aerogels with an intermediate
specific surface area were produced from hydrogels at alkaline pH
(Andlinger et al., 2020). Analyzing the publication year of the
above-mentioned studies, it is evident that research on protein-based
bioaerogels has begun a few years back. However, recent studies
exploring the significance of various proteins in bioaerogel production is
still low. Meanwhile, we anticipate that similar to potato protein isolate,
other edible plant proteins with good gelation ability obtained from
various sources such as nuts, vegetables, grains, and legumes could be
studied for the production of bioaerogels for food applications. Never­
theless, food-grade bioaerogels from various animal-derived edible
proteins could also be expected in the upcoming years.
P. Selvasekaran and R. Chidambaram Food Hydrocolloids 131 (2022) 107760

3.17. Camelina, flax, and balangu seed mucilages Table 3

Structural and physicochemical characterization methods of bioaerogels.
Seed mucilages are soluble fibers present in the mucous epidermis Characterization Purpose Reference
(outermost layer) of various seeds and composed of mixtures of techniques/methods
numerous proteins and polysaccharides. Due to the excellent physico­ X-ray diffraction Determination of the relative Abhari et al. (2017)
chemical and functional properties, mucilages are being incorporated crystallinity of bio-aerogels
into various food formulations and are safe for consumption. Recently, Thermogravimetric Determination of thermal Alnaief et al. (2018)
the fabrication of novel bioaerogels from seed mucilages for food ap­ analysis stability of the bio-aerogels
Scanning electron Determination of the bio- García-González,
plications is considered an emerging trend (Selvasekaran & Chi­ microscopy aerogel morphology. Camino-Rey, et al.
dambaram, 2021b). Camelina seed mucilage with excellent swelling (2012)
kinetics and water absorption capacity was used to fabricate cylindrical Zeta potential Determination of the de Oliveira, Bruni, el
aerogels with minimum shrinkage, nanoporous structure, and high suspension stability of bio- Halal, et al. (2019)
aerogels
surface area. The pore volume of 0.32 & 0.28 cm3/g, porosity of 91 &
Powder densitometer Determines the bulk density Ganesan et al. (2018)
94%, pore size of 6.0 & 5.6 nm, density of 0.08 & 0.05 g/cm3, specific of bio-aerogels that are
surface area of 240 & 229 m2/g were observed for aerogels obtained complex in shape
from camelina seed mucilage concentrate and powder, respectively Helium pycnometer Determination of the skeletal Ganesan et al. (2018)
(Ubeyitogullari & Ciftci, 2020). Similarly, Comin, Temelli, and Saldaña density of open pores present
in bio-aerogels
(2015) produced flaxseed mucilage aerogels with 25.2 Å, 0.82 cm3/g,
Nitrogen adsorption- Analyzation of surface area, Nešić et al. (2018)
201.1 m2/g, and 0.16 g/cm3 of average pore diameter, pore volume, desorption pore volume and pore
specific surface area, and low density, respectively. However, difficulty diameter of bio-aerogels
in shape retention of the hydrogel at a concentration of seed mucilage Differential scanning Determination of the thermal Nešić et al. (2018)
calorimetry conductivity of bio-aerogels
<10% w/v (Ubeyitogullari & Ciftci, 2020) and <10% w/w (Comin et al.,
Texture Analyzer Analysis of texture profile of da Silva et al. (2020)
2015) was indicated as a major drawback that led to the deformed bio-aerogels
morphology of aerogels. A significant structural deformation during the Analytical balance Weight measurement of bio- Farhat et al. (2019)
solvent exchange and afterward supercritical CO2 drying was reported aerogels
as another major drawback during the production of balangu seed Digital caliper Volume or dimension Farhat et al. (2019)
measurement of bio-aerogels
mucilage aerogels with 0.368 cm3/g of pore volume and 95.74 m2/g of
UV spectrometry Quantification of Pantić, Knez, and
specific surface area (Falahati & Ghoreishi, 2019). micronutrient loading of bio- Novak (2016)
aerogels
Laser particle size Determination of particle Alnaief et al. (2018)
4. Characterization of bioaerogels
analyzer size distribution of bio-
aerogels
The desired properties of bioaerogels such as bulk density, specific Fourier transform- Determination of bonding Pantić, Kotnik, et al.
surface area, volumetric shrinkage, mechanical property, moisture ab­ infrared spectroscopy type and its interaction (2016)
sorption isotherm, surface morphology, and thermal behavior must be within bio-aerogel

evaluated before its application in micronutrient fortification and food

packaging. Following are the methods available to characterize the Renzo, et al., 2011).
structural and physicochemical properties of bioaerogels intended for
use in food. Nevertheless, it is important to mention that these tech­ Vpores =
1
−
1
(2)
niques are also applicable to other aerogels in general. Table 3 enlists ρbulk ρskeletal
characterization techniques to determine various properties of The total volumetric shrinkage (VSt) of bioaerogel monoliths can be
bioaerogels. determined by employing the following equation (3) (Ganesan et al.,
The bulk density(ρ) of bioaerogels can be determined by directly 2018).
measuring the weight (mass) and volume (dimensions). An alternative ( )
method to determine the bulk density is the use of a powder densi­ Vhydrogel − Vaerogel
VSt = × 100% (3)
tometer which measures the volume of bioaerogels that are geometri­ Vhydrogel
cally complex in shape. The skeletal density of open pores can be
determined by using a helium pycnometer (Ganesan et al., 2018). where Vhydrogel and Vaerogel are the volume of hydrogel and aerogel,
Further, the total porosity of bioaerogels can be calculated from the bulk respectively.
density and skeletal density according to the following equation (1) The mechanical property of bioaerogels can be evaluated by per­
(Dogenski et al., 2020). forming uniaxial compression tests using a texture analyzer (Abhari
et al., 2017). The stability of the aerogel in an aqueous solution can be
ρbulk
Porosity (%) = 1 − × 100 (1) determined by immersing them in excess water and maintaining them at
ρskeletal
room temperature for 7–8 days or as per the study, assisted with occa­
The specific surface area (Sa) can be measured by employing the sional stirring. Further, bioaerogels should be dried to obtain a constant
Brunauer–Emmett–Teller (BET) method and nitrogen adsorption tech­ weight. Later, their stability in the aqueous media can be calculated
nique (Robitzer, Tourrette, et al., 2011). Bioaerogels hold numerous according to equation (4) (Dogenski et al., 2020) and expressed as
mesopores and macropores ranging from hundreds of nanometres to aerogel mass loss in percentage.
several microns. Therefore, in addition to the specific surface area, pore
(W0 − Wi )
size and pore volume are the significant factors determining the end Aerogel mass loss (%) = × 100% (4)
W0
texture of bioaerogels (Ganesan et al., 2018). The pore volume and pore
size distribution are measured by applying standard methods which where Wo and Wi are the initial and final weight of the bioaerogels,
include the Barrett-Joyner-Halenda (BJH) approach or mercury poros­ respectively.
imetry (Rudaz et al., 2014). BJH is an effective approach to characterize The angle measurement of water content in bioaerogels can be done
the mesopores and smaller macropores however, it is not applicable to by using a contact angle analyzer equipped with a CCD camera and
determine the size of larger macropores (Kayser et al., 2012). The pore software to analyze the obtained image (Wang, Su, et al., 2019).
volume can be calculated by the following equation (2) (Robitzer, Di

11
P. Selvasekaran and R. Chidambaram
Moisture absorption isotherm of bioaerogels can be analyzed by using
the dynamic vapor absorption apparatus (Jin, Han, Li, & Sun, 2015). The
water/oil absorption capacity of bioaerogels can be studied by
immersing them in excess water/oil and periodically weighing them
after the removal of water/oil. Further, the water and oil absorption
capacity can be determined according to the following equation (5)
(Farhat et al., 2019).
( )
Wswollen,t − Wdry
Water or oil absorption capacity = × 100% (5)
Wdry
where Wswollen,t, and Wdry are the weight of the bioaerogel at a particular
time t and weight of the dried aerogel, respectively.
The surface morphology of bioaerogels can be visualized by using the
images obtained from the Scanning Electron Microscopy (SEM) (Groult
& Budtova, 2018b). 3D tomography is also a significant tool to char­
acterize the surface morphology of the bioaerogels (Budtova, 2019).
However, it cannot be used to analyze the pore size distribution ranging
below a few hundred nanometres (Ganesan et al., 2018). The crystal­
linity pattern can be obtained by irradiating bioaerogels with X-ray
using a diffractometer (XRD) (Abhari et al., 2017). Further from the
obtained pattern, the crystallinity index can be calculated according to
the following equation (6) (Chen & Zhang, 2019).
( ′)
I− I
Crl (%) = × 100% (6)
I
Where I is the crystalline region and I is the amorphous region on the X-
′
ray diffractograms.
The thermal behavior of bioaerogel microspheres can be character­
ized using differential scanning calorimetry (DSC) under a constant ni­
trogen flow whereas the thermal stability of the bioaerogel microspheres
can be investigated using a thermogravimetric analyzer (TGA) (Wang
et al., 2018). The type of bonding interaction within bioaerogel micro­
spheres can be analyzed from the Fourier transform-infrared (FT-IR)
spectra (Budtova, 2019).
5. Application of bioaerogels in micronutrient fortification of
foods
Micronutrient fortification is determined as one of the significant
methods applied to address the micronutrient deficiency of all age
groups and has occupied a niche in the food industry. The process of
micronutrient fortification involves the incorporation of micronutrients
(vitamins and minerals) in a particular product to enhance the nutri­
tional profile and quality of the food (Chadare et al., 2019). The common
challenges being faced by food technologists during micronutrient
fortification are bioavailability, dispersibility, homogeneity, and sta­
bility of the added micronutrients (Maurya, Bashir, & Aggarwal, 2020).
These challenges are the driving force that has led to the development of
various technologies for micronutrient fortification of foods and one
such technological advancement is the encapsulation of micronutrients
(Mehling et al., 2009). The advantages of encapsulation include pro­
tection of micronutrients from physicochemical stress such as pH, tem­
perature, moisture, and oxidation; acts as a solubility barrier between
micronutrients and food matrix; controlled and targeted release of
micronutrients; do not modify the appearance, taste, and quality of the
food matrix and sustains customer acceptance (Ribeiro et al., 2015). The
commonly used encapsulation technique in the micronutrient fortifica­
tion of foods is coacervation, spray drying, molecular inclusion,
co-crystallization, interfacial polymerization, fluidized bed,
freeze-drying, and nanoencapsulation (Levi et al., 2011).
An alternative and rapidly emerging approach is the concept of
loading micronutrients in bioaerogels as they possess specialized char­
acteristics such as high porosity, higher surface area, ultra-low density,
outstanding acoustic, thermal insulation, and stable mechanical
12
Food Hydrocolloids 131 (2022) 107760
properties. Besides, bioaerogels derived from seed mucilages, proteins,
and polysaccharides are safe, sustainable, renewable, and edible for
consumption (Selvasekaran & Chidambaram, 2021b). Bioaerogel mi­
crospheres have been explored in numerous research as potential carrier
matrices of valuable compounds for food applications (Ahmadi et al.,
2016; De Cicco et al., 2016; De Marco & Reverchon, 2017; García-­
González et al., 2015a; Gonçalves et al., 2016; Mustapa & Al., 2018;
Obaidat, Alnaief, & Mashaqbeh, 2018). Zheng, Tian, Ye, Zhou, and Zhao
(2020) indicated that polysaccharide based bioaerogels hold the ten­
dency to lower the calorific value of various food products as they
possess high porosity along with ultralow density and such bioaerogels
are suitable for loading micronutrients. The high inner surface area of
bioaerogels is accessible for the adsorption of various micronutrients,
while the higher internal porosity is well-structured for the capillary
condensation of delicate micronutrients (Chen & Zhang, 2019). The
occupied inner pores shield the micronutrients from adverse environ­
mental factors viz. light, moisture, temperature, and oxygen. Addition­
ally, this technique offers the feasibility to mask unfavorable odor and
taste of micronutrients (Selmer et al., 2019a fortification of foods, bio­
aerogels in the form of microspheres with closed pores are promising as
they do not modify the physicochemical and sensory properties of foods
(Mikkonen et al., 2013). However, it is highly challenging to produce
bioaerogels with dual and controlled pore size distribution which con­
fines them from occupying a niche in micronutrient fortification of food
products as the macroporosity of bioaerogels is of major concern. In such
a case pressurized CO2 gelation and its rapid depressurization rate are
documented as a novel approach. At a slow depressurization rate (0.02
MPa/min) no macropores were detected whereas at a fast depressur­
ization rate (3 MPa/min) macroporosity (31.3%) with good inter­
connectivity (33.2%) was detected in alginate aerogels (Quraishi et al.,
2015). Dual pores in alginate-starch hybrid aerogels were gained by
increasing the depressurization rate (0.1–30 bar/min) i.e., mesoporosity
(183–544 m2/g and 2.0–6.8 cm3/g of specific surface area & pore vol­
ume, respectively) and macroporosity (2–25%) with excellent inter­
connectivity (Martins et al., 2015).
Selmer et al. (2019a) reported that the consumer acquiescence of
micronutrients impregnated in bioaerogel microspheres is considered to
be surpassing in comparison to bioaerogel monoliths. The incorporation
of micronutrients into the bioaerogels is done amid various steps of
aerogel formation such as a)-prior to gelation; b)- amid the alcogel
formation; c)- amid the process of drying (generally supercritical CO2
drying); d)- succeeding the drying. However, it depends on the affinity
of micronutrients to the utilized solvent such as water, alcohol, and
supercritical CO2 (Zheng et al., 2020; Dogenski et al., 2020). Fat-soluble
vitamins (Vitamin A, D, E, and K) are proved as highly soluble in su­
percritical CO2 fluid (Pantić, Knez, & Novak, 2016). Fig. 3 illustrates the
loading of micronutrients into bioaerogels amid the various steps of
production. Table 4 enlists micronutrients loaded into various bio­
aerogels for food applications. The effective methods that are used to
impregnate bioaerogel matrix include supercritical impregnation, wet
impregnation, subcritical liquid impregnation, and oil absorption or oil
dispersion. In the case of the food industry, supercritical solvent
impregnation is a highly promising technique to load micronutrients as
the loaded aerogel will be devoid of contamination with residual sol­
vents (Milovanovic, Jankovic-Castvan, Ivanovic, & Zizovic, 2015). Be­
sides, supercritical CO2 loading of bioaerogels is gaining interest as the
green practice for the entrapment of poorly water-soluble micro­
nutrients (Pantić, Knez, & Novak, 2016). In supercritical impregna­
tion/supercritical CO2 adsorption, the saturated solution containing
supercritical CO2 fluid and micronutrients diffuses into the pores of
bioaerogels. Further, loading starts with the chemical adsorption of
micronutrients on the surface of bioaerogels. As an example, De Marco
and Reverchon (2017) dissolved micronutrients in the supercritical CO2
fluid and brought in contact with bioaerogels to be impregnated. At
supercritical conditions, the unique characteristics of CO2 such as high
diffusivity and low viscosity enhanced the micropore penetration and
P. Selvasekaran and R. Chidambaram Food Hydrocolloids 131 (2022) 107760

Fig. 3. Micronutrient loading of bioaerogels: (A) during the sol-gel process; (B) during the solvent exchange; (C) during supercritical drying; (D) after supercriti­
cal drying.

Table 4
Summary on the impregnation of micronutrients into various bioaerogels.
Aerogel Loaded Substance Loading technique Loading Loading Reference
Source time efficiency

Maize starch α-tocopherol (Vitamin E) Supercritical CO2 adsorption 24 h 19.99% De Marco and Reverchon
(2017)
Maize starch Menadione (vitamin K3) Supercritical CO2 adsorption 24 h 8.76% De Marco and Reverchon
(2017)
Corn starch Vitamin E (α-tocopherol, TOC) Supercritical impregnation 24 h – De Marco et al. (2019)
Alginate 2-methyl-1, 4-naphthquinone Supercritical impregnation 24 h – Pantić, Kotnik, et al.
(vitamin K3) (2016)
Alginate Cholecalciferol (vitamin D3) Supercritical impregnation 24 h – Pantić, Kotnik, et al.
(2016)
Alginate Cholecalciferol (vitamin D3) High pressure impregnation employing both supercritical 24 h – Pantić, Kotnik, et al.
and liquid carbon dioxide. (2016)
Cellulose L-ascorbic acid (vitamin C) Antisolvent Precipitation with Supercritical Carbon Dioxide 24 h – Haimer et al. (2010)
Apple fruit Nicotinic acid (Vitamin B3) During the sol-gel process – 25% Veronovski et al. (2014)
pectin
Citrus fruit Nicotinic acid (Vitamin B3) During the sol-gel process – 37% Veronovski et al. (2014)
pectin

-: Not mentioned.

rapid equilibration of the fluid phase within the highly porous aerogel
matrix. Further, micronutrient-loaded bioaerogels free of solvent were
obtained by removing the supercritical CO2 fluid at a slow depressur­
ization rate. The use of liquid CO2 over supercritical CO2 is advanta­
geous for the impregnation of temperature-sensitive micronutrients into
bioaerogels. Pantić, Kotnik, Knez, and Novak (2016) for the first time
reported the subcritical liquid impregnation of temperature-sensitive
vitamin D3 into bioaerogels derived from alginate. During storage
(2–8 ◦ C) the shelf life and stability of vitamin D3 were improved. This
method involved the utilization of liquid CO2 below the critical point of
supercritical CO2 (31.1 ◦ C). The liquid CO2 was reported to be an
appropriate solvent which allowed the prospect of operating at lower
temperature ranges, prevented the degradation of vitamin D3, and pro­
vided higher loading within the short period of impregnation. Both su­
percritical and subcritical impregnation method does not destroy or
damage the structure of bioaerogels (Pantić, Kotnik, et al., 2016).
The impregnation step succeeding the supercritical drying can be
avoided by employing wet impregnation which integrates liquid

13
P. Selvasekaran and R. Chidambaram
adsorption with supercritical CO2 drying of aerogels. In wet impregna­
tion, alcogels were allowed to interact with an organic solvent consisting
of micronutrients of interest for a certain time period. Later, loading
arises amid the process of drying through the removal of the solvent by
supercritical CO2 fluid and antisolvent precipitation of micronutrients
(Selvasekaran & Chidambaram, 2021b). However, residual levels of
toxic organic solvent, degradation of micronutrients, and undesired re­
actions in the resulting aerogels that may cause low processing effi­
ciency must be taken into account (Mustapa, Martin, Sanz-Moral, Rueda,
& Cocero, 2016). Oil absorption or oil dispersion also holds a huge po­
tential to impregnate bioaerogels with fat-soluble vitamins. In this
method, bioaerogels with good oil absorption capacity can be directly
immersed into the oil dispersion containing fat-soluble vitamins (Plaz­
zotta et al., 2020). Although wet impregnation and oil absorption
method was used to impregnate other functional ingredients into bio­
aerogels, no studies were reported on the loading of micronutrients.
Alginate and Starch bioaerogels are frequently used as carrier
matrices to impregnate micronutrients. Maize starch bioaerogels in the
form of microspheres were investigated for their prospect as carrier
matrices of poorly water-soluble vitamins – menadione (Vitamin K3) and
tocopherol (Vitamin E) through the supercritical CO2 adsorption for 24 h
(De Marco & Reverchon, 2017). The study described that bioaerogel
microspheres obtained from starch revealed 95–98% of vitamin loading
capacity. The recommended dietary allowance (RDA) of vitamin K3 and
vitamin E for adults is 100 μg and 15 mg, respectively. The maximum
release profile of loaded vitamin E was 145 μg/mg of aerogel and in the
case of vitamin K3, the maximum release profile was 100 μg/mg of
aerogel. Therefore, the authors concluded that 1 mg of maize starch
aerogel could satisfy the RDA of vitamin E and K3 and could be poten­
tially used for the micronutrient fortification of foods.
Micronutrient fortification of foods with vitamin D3 represents a
challenging task as it is insoluble in water and sensitive to high tem­
perature, light, and air. Thus, Pantić, Kotnik, et al. (2016) supercritically
impregnated cholecalciferol (vitamin D3) and vitamin K3 into alginate
aerogel microspheres. The highest loading capacity was achieved after 1
h of supercritical impregnation which was attributed to the higher sol­
ubility of vitamin D3 and K3 in the supercritical CO2 fluid. Compara­
tively, the solubility of Vitamin K3 in supercritical CO2 fluid was higher,
thus the amount of impregnated vitamin K3 was higher than vitamin D3.
The controlled release of both vitamins was achieved over a time period
of 6 h. The RDA value of vitamin D3 is 25 μg/day, whereas the maximum
release concentration of 1 mg alginate aerogels microspheres was 41.64
μg. Thus, 0.60 mg alginate aerogel microspheres loaded with 25 μg of
vitamin D3 could be potentially incorporated into foods for effective
vitamin D3 fortification (Pantić, Knez, & Novak, 2016).
De Marco, Riemma, and Iannone (2019) loaded starch aerogel with
α-tocopherol (vitamin E) using supercritical CO2 impregnation. The
study reported that 120 mg of starch aerogel could deliver 15 mg of
vitamin E, which was in accordance with the RDA of Vitamin E for adults
(15mg/day). Similarly, pectin/sodium alginate hybrid aerogel micro­
spheres were loaded with vitamin E, and the maximum loading capacity
of 81% was attained (Dhat, Naik, Amruta, & Parimal, 2009). Veronovski
et al. (2014) loaded nicotinic acid (Vitamin B3) into bioaerogels ob­
tained from citrus fruit pectin and apple fruit pectin during the sol-gel
process. The study elucidated that the impregnation efficiency
strongly depends on the specific surface area and pores of the aerogels.
The apple fruit pectin aerogels with comparatively low surface area
(213.5 m2/g) and pore volume (0.339 cm3/g) exhibited a maximum
loading efficiency of 25% whereas the citrus fruit pectin with a high
surface area (248.9 m2/g) and high pore volume (0.39 cm3/g) presented
the maximum loading efficiency of 37%. Haimer et al. (2010) impreg­
nated L-ascorbic acid (vitamin C) into bioaerogels obtained from bac­
terial cellulose during the process of supercritical CO2 drying. In general,
the amount of micronutrients impregnated into the bioaerogel matrices
determines its release profile. Contrarily the findings of this study re­
ported that the release profile was independent of the amount of loaded
14
Food Hydrocolloids 131 (2022) 107760
vitamin C, instead, dependent on the thickness of the cellulose aerogel
matrix.
After loading the micronutrients, a supplementary layer of coating
can be applied for the enhanced protection of the bioaerogel matrix
(Goslinska et al., 2019). However, Alnaief et al. (2012) strongly sug­
gested reducing the contact time of bioaerogels with coating solutions as
long contact time destroys the end morphology of aerogels. The loading
capacity of the bioaerogels is associated with their internal structure and
type of reaction with micronutrients. The micronutrient loading ca­
pacity can be elevated by decreasing the pore size and increasing the
specific surface area as that increases the capillary force contributing to
the high loading capacity (Mehling et al., 2009). In addition, Ubeyito­
gullari and Ciftci (2016b) reported that decreasing the size of micro­
nutrients increased their bioavailability. The encapsulation efficiency of
loaded micronutrients in bioaerogel microspheres can be calculated as
per equation (7).
Actual micronutrient amount
EE (%) = × 100 (7)
Theoretical micronutrient amount
Similar to the above-mentioned studies, the frequently used vita­
mins, and minerals as fortificants such as vitamin A, D, C, iron, folic acid,
iodine, calcium, magnesium, and zinc can be loaded into the suitable
bioaerogel matrices (Fig. 4) (Cardoso, Fernandes, Gonzaléz-Paramás,
Barros, & Ferreira, 2019). To the best of our knowledge, literature on
direct impregnation of various minerals into bioaerogel matrix has not
been reported yet and holds huge prospects for investigation. Selvase­
karan and Chidambaram (2021b) and Zheng et al. (2020) specified that
consumable bioaerogels obtained from seed mucilages, proteins, and
polysaccharides could be integrated into the food system as an aspiring
matrix to load the desired compounds. However, the lack of precise
technology facilitating precise micronization of bioaerogels hinders the
scope of this material to reach the food market of micronutrient delivery
systems (García-González & Smirnova, 2013a). However, it is important
to highlight that to date only (Ubeyitogullari & Ciftci, 2019) explored
the incorporation of bioaerogels (starch bioaerogels) into the real food
matrix-low-fat, non-fat, and regular granola bars. Further studies on the
incorporation of micronutrient-loaded aerogels into real food products
such as milk and dairy products, cereal-based products, soy sauce, and
various other processed products including fruit beverages are encour­
aged. Thus, fortified products could reach the target population and
ensure the daily dietary requirement of micronutrients (Chadare et al.,
2019).
Bioaerogels should be stable during the storage period and leakage of
impregnated micronutrients must be avoided. Therefore, the storage
and shelf life of impregnated and unimpregnated bioaerogels should be
explored in-depth (Zheng et al., 2020). Another major challenge is that
the loaded vitamins should be delivered at the interested site where their
physiological function is essential (Veronovski et al., 2014). Due to the
hydrophilic nature of polysaccharide aerogels, the impregnated vita­
mins undergo faster release as the aerogel matrix disintegrates upon
contact with water. Thus, the hydrophilic nature of polysaccharide
aerogels will be a major setback for incorporation in liquid foods. In such
a case, coating or chemical modification of aerogel surface could be
opted to change the hydrophilic bioaerogels into hydrophobic. Also, the
incorporation of micronutrient-loaded aerogels should not weaken the
rheological properties and deteriorate the sensorial aspects of the for­
tified food products (Selvasekaran & Chidambaram, 2021b). Ubeyito­
gullari et al. (2018) reported that different structure of aerogels
undergoes different digestion process and the use of chemical cross­
linkers decreases the digestibility of the aerogels. Therefore, in-vitro
digestibility experiments of various bioaerogels and food products
containing them should be investigated, as the literature available is still
limited. The micronutrient-loaded or unloaded bioaerogels should be
assessed for any possible allergic or intolerant reactions before their
incorporation into food products, especially in foods products that are
already proven to be associated with adverse food reactions
P. Selvasekaran and R. Chidambaram
Fig. 4. Illustration of micronutrients loaded in pores of the bioaerogel matrix.
(Muthukumar, Selvasekaran, Lokanadham, & Chidambaram, 2020). For
instance, whey which is a milk protein was reported to cause allergic
reactions upon consumption (Logeshwaran, Selvasekaran, & Chi­
dambaram, 2020; Sekar et al., 2020) and therefore aerogels prepared
from whey proteins could lead to adverse allergic reactions. The absence
of hazardous chemicals during the production of bioaerogels is indicated
as a major advantage, attention must be laid to the use of ethanol during
the solvent exchange step. This may cause consumption restrictions for
certain individuals such as children and consumers with strict religious
dietary restrictions (Manzocco, Mikkonen, & García-González, 2021).
As quoted by Mikkonen et al. (2013) and Zhu (2019) the food
products containing aerogels impregnated with micronutrients are not
commercialized in the market, but the scope for such products is
considered significant. In addition to micronutrients, bioaerogels favor
the incorporation of various aroma, biologically active compounds, and
healthy oils (Selvasekaran & Chidambaram, 2021b). Besides, the in­
clusion of bioaerogels in various food products is not indicated in the
current regulation. These novel food-grade bioaerogels should be eval­
uated under the current Novel Foods Regulation (EU Regulation
2015/2283, 2015). Accurate information is mandatorily required to
differentiate bioaerogels that could be included in the diet from those
requiring certain authorization (Manzocco et al., 2021). Above all, if
fortified products containing bioaerogels are commercialized, their cost
is expected to be higher than the regular fortified products. This is
anticipated due to the higher production cost of bioaerogels which in­
volves the cost of raw materials, multi-step production process and use
of sophisticated equipments.
6. Application of bioaerogels in active packaging of foods
Extended storage or long-distance transportation can expose fresh
produce or packed foods to various hazards including microbial
spoilage, softening, and ripening. Food packages are essential materials
that provide physical and barrier protection and serve as mere storage
containers to ensure food safety and quality (Lehtonen et al., 2020).
Novel approaches for the production of active or intelligent food pack­
aging materials with good oil and water absorption capacity, thermal
stability, and controlled release of active ingredients from the packaging
materials into food products are highly studied in recent years. In this
regard, the ultra-low density, high liquid absorption capacity, excellent
thermal properties, high surface-volume relationship, and high internal
surface area of bioaerogels are highly desired for the development of
biodegradable and non-toxic food packaging materials (de Oliveira,
Bruni, el Halal et al., 2019). A novel bioaerogel based active packaging
could reduce food waste and lift the sustainability and economy of the
food supply chain. Polysaccharide aerogels are represented as progres­
sive materials in food packaging industries in various forms such as
oxygen/humidity sachet scavengers, internal food packaging layers, and
wraps (Nešić et al., 2018). Hexanol is a volatile compound that prevents
the growth of spoilage microorganisms. Recently, Lehtonen et al. (2020)
incorporated food-grade sunflower oil into an active bioaerogel based
packaging material eliminating the use of organic solvent for the
15
Food Hydrocolloids 131 (2022) 107760
controlled long-term release of hexanal. During the preparation of bio­
aerogel material, the hydrogel was obtained from 2 wt % gal­
actoglucomannans and anionic cellulose nanofibril in the ratio of 70:30,
w/w using 2.5–12.5 wt % of ammonium zirconium carbonate as the
crosslinker. Later, an emulsion containing sunflower oil and hexane
(1–100 mg/g) was added to the prepared hydrogel which was followed
by freeze-drying. For at least 3 weeks, 7–23 μmol of hexanol per gram of
aerogel was produced and released. Blueberries stored along with
hexanal releasing bioaerogel matrix did not show any visual alteration
for 5 days at room temperature and cherry tomatoes maintained their
firmness for a longer period.
Bioaerogels obtained from cellulose nanocrystals exhibited water
absorption capacity ranging between 264.2% and 402.8% and therefore,
de Oliveira, Bruni, Fabra, et al. (2019) proved that aerogels obtained
from food-grade materials could be used as potential water absorbers in
food packaging. The functional groups occurring in the polysaccharides
easily interact with the medium due to the large surface area of aerogels.
This property facilitates the sorption of various surfactants, dissolved
polar molecules, saline solutions, water, and water vapor on the surface
of aerogels. Moreover, the crosslinked network of polysaccharides
maintains the physical structure of the aerogels during water absorption
(Quignard, Valentin, & Di Renzo, 2008). de Oliveira, Bruni, Fabra, et al.
(2019) and Oliveira et al. (2017) reported that bioaerogels obtained
from single polymer cellulose nanocrystals or polyvinyl alcohol (PVA)
disintegrated upon contact with water. As a solution, cellulose nano­
crystals were combined with polyvinyl alcohol (PVA) which augmented
the water absorption capacity. This proved that the combination of
various polymers could improve the water absorption capacity of bio­
aerogels. However, the high mechanical strength and chemical stability
of synthetic polymers such as PVA could slow the rate of degradation.
The distribution and size of the bioaerogel pores is also a key factor
determining their use as absorbers in food packaging applications as
they influence the capacity and mechanism of water absorption. de
Oliveira, Bruni, Fabra, et al. (2019) indicated that bioaerogels with
compacted structure and small pores exhibit a low level of
water-absorbing capacity or completely disintegrate upon contact with
water. The addition of appropriate co-polymers could increase the pore
size. Spagnol et al. (2012) documented that the presence of cellulose
nanocrystals as a co-polymer along with starch increased the pore size
and facilitated the easier and faster diffusion of the liquid into the aer­
ogel matrix.
The relative crystallinity of precursors also influences the water-
absorbing capacity of the bioaerogels. Bioaerogels obtained from euca­
lyptus and rice cellulose nanocrystals with relative crystallinity values of
86.4% and 75.5% presented a water-absorbing capacity of 264.2% and
357.5%, respectively. Evidently, a higher relative crystallinity value of
the precursor decreases the water-absorbing capacity of resulting aero­
gels (de Oliveira, Bruni, el Halal et al., 2019). This was due to the barrier
effect caused by higher relative crystallinity in the resulting matrix
which led to low diffusion of water molecules between the polymeric
chains. However, this phenomenon increases the degradation resistance
of the matrix in hydrolytic environments (Luiz De Paula, Mano, &
P. Selvasekaran and R. Chidambaram
Pereira, 2011). da Silva et al. (2020) produced bioaerogels suitable as
water-absorbing food packaging materials from wheat starch (non-­
germinated or germinated type) either including or excluding the use of
polyethylene oxide. After 24 h of immersion in water, the obtained
bioaerogels presented higher degradation temperature, enhanced
physical integrity, and excellent water absorption capacity. Irrespective
of the type of wheat starch, bioaerogels obtained excluding polyethylene
oxide showed water absorption capacity ranging between 946.5% and
957.0%. The inclusion of polyethylene oxide increased the water ab­
sorption capacity of wheat starch aerogels which ranged between
1143.6% and 1279.1%. This was attributed to the highly hydrophilic
nature of polyethylene oxide as it contains a high number of hydroxyl
groups that have a higher affinity to bind with water molecules.
Bioaerogels as moisture absorbers could be used to prevent
condensation of water as a consequence, water activity and microbial
growth rate will be reduced in packaged foods, especially in meat
packaging (de Oliveira, Bruni, el Halal et al., 2019). Lehtonen et al.
(2020) concluded that in upcoming years <1 g of bioaerogels could
preserve the plant-based food products against mold growth and soft­
ening in the 1-L package. de Oliveira, Bruni, Fabra, et al. (2019) also
indicated that composite aerogels obtained from food-grade materials
with biodegradable and renewable properties could be used as absor­
bent pads in fish trays or meat due to their ability to absorb high water
content released by fresh food products. In fresh meat packaging,
compression resilience and sufficient strength of bioaerogels that sustain
the meat weight without undergoing deformation can be used as an
alternative to expanded polystyrene which is commonly preferred in
meat packages (da Silva et al., 2020).
In recent years, several approaches are being explored on the
controlled release of functional components from the active food pack­
aging materials towards the food products. One such approach is the
impregnation of bioactive compounds into bioaerogel packaging mate­
rials. de Oliveira, Bruni, Fabra, et al. (2019) added agar-derived extracts
into various selected formulations consisting of PVA + cellulose/nano­
cellulose, PVA + cellulose, and pure PVA and assessed their controlled
release into the food simulants. Bioaerogels formed with pure PVA
spontaneously released the agar extract in hydrophilic (10% ethanol)
and hydrophobic (50% ethanol) food simulants. The hybrid aerogel
formulations containing PVA + cellulose/nanocellulose, and PVA +
cellulose presented a more sustainable release of agar extracts. In the
first 5 h, both the hybrid aerogel formulation exhibited 60% release in
hydrophilic and 40–50% release in hydrophobic foods. However, after
48 h bioaerogels formulated only with cellulose presented 70% and 60%
release in hydrophobic and hydrophilic foods, respectively. The highest
release rate of 80% in hydrophilic and 90% in hydrophobic foods were
observed in bioaerogels formulated with nanocellulose. This was due to
the large surface area of the nanocellulose which increased the presence
of free hydroxyl groups in aerogels for interaction with water molecules
thereby elevating the water swelling kinetics and water vapor sorption
(de Oliveira, Bruni, Fabra, et al., 2019). The functional bioaerogels
possessing high water absorbing capacity are advantageous as they
could be used to intake the exudates from packaged food products. The
accumulation of liquids inside the packages can be eliminated which
further hinders or prolongs the growth of microorganisms. Moreover,
bioaerogel packing system in the form of absorbent can be utilized for
shelf life extension of food products by incorporating bioactive com­
pounds (da Silva et al., 2020). As an example, during refrigerated stor­
age, superabsorbent bioactive cellulose aerogel pads containing aqueous
extracts of Arundo donax reduced the lipid oxidation and color loss in red
meat (Fontes-Candia, Erboz, Martínez-Abad, López-Rubio, & Martí­
nez-Sanz, 2019a).
The excellent thermal insulation property of bioaerogels due to the
low thermal conductivity is favorable for thermal insulation packaging
of temperature-sensitive foodstuffs. Temperature, as well as humidity,
are the significant external parameter reported to be negatively influ­
encing the chocolate quality (Selvasekaran & Chidambaram, 2021a).
16
Food Hydrocolloids 131 (2022) 107760
Chen et al. (2020) incorporated silica aerogels into PVA-based films and
developed thermal insulation materials for the multilayer packaging of
chocolates. The improved thermal stability, oxygen, and water vapor
barrier property were achieved in PVA films containing 3% aerogel.
Further, the crystallinity degree and thermal conductivity of films
decreased with a simultaneous increase in the aerogel content. At
ambient temperature (10 ◦ C) the hardness of chocolates packed with
PVA films without aerogels was 8.17 N. This further increased to 16.16
N for chocolates packed with PVA films containing 7% aerogels. This
proved that the softening of chocolates could be prevented upon
increasing the aerogel content in the films as they inhibit the heat
transfer from outside into the package. Similarly, Lin et al. (2020)
developed chitosan-nano-silicon aerogel-based composite edible and
functional packaging films through the incorporation of the okra pow­
der. The obtained films exhibited effective antibacterial properties
against S. aureus and E. coli which are gram-positive and gram-negative
bacteria, respectively. The thickness, oil resistance, structural integrity,
and, moisture permeability of the composite film were improved
whereas the tensile strength, flexibility, hydrophobicity, and finely
cracked surface decreased upon increasing the nano-silicon aerogel
level. The authors concluded that composite films derived from chitosan
by the inclusion of nano-silicon aerogel can be used to contain oily
foods. Nešić et al. (2018) demonstrated that aerogels obtained from
pectin-titanium oxide nanoparticles are highly potential for the storage
of food products that are sensitive to high temperature. The thermal
conductivity property of nanocomposite aerogels was reduced signifi­
cantly in comparison to other materials that are regularly utilized in
food packaging industries such as cellulose foams and polystyrene. The
addition of titanium oxide nanoparticles increased the thermal stability,
and mechanical properties, and exhibited strong antibacterial properties
against E. coli. under UV and dark illumination conditions. As the visual
impression of food packages is important for consumer acquisition, the
bioaerogel based packaging system should be highly transparent. Con­
cerning this Plappert, Nedelec, Rennhofer, Lichtenegger, and Liebner
(2017) developed highly transparent cellulose aerogels with excellent
thermal insulation and intriguing mechanical properties intended for
food packaging.
Above all, it is important to highlight that bioaerogels as food
packaging materials should not liberate their elements into foods at
levels detrimental to human well-being. They should not deteriorate the
odor, taste, and food composition. Also, these materials should be sub­
jected to safety evaluation as defined in the European Food Safety Au­
thority guidelines (https://efsa.onlinelibrary.wiley.com/doi/epdf/10
.2903/j.efsa.2008.2 1r). A major concern with the use of bioaerogels
as food packaging materials is their cost. Low-value side streams can be
upgraded to produce bioaerogels intended for packaging applications
from renewable resources. This could highly curtail the cost contribu­
tion of raw materials. However, the multi-step production process that
uses a large amount of solvent such as supercritical CO2 is expensive.
Minimizing the use of fresh solvents and a continuous supercritical
drying process could decrease the production cost of bioaerogels on an
industrial scale in comparison to batch production (Manzocco et al.,
2021).
7. Conclusion and future directions
In this review, the commonly used precursors and steps involved in
the production process of bioaerogels, the characterization techniques of
bioaerogels, and their food related applications were summarized. Bio­
aerogels are being produced from various polysaccharides, proteins, and
seed mucilages. Owing to their sole properties viz. high surface area,
ultra-low density, and highly porous nature, bioaerogels could be used
as advanced food materials. As an example, the novelty of bioaerogels as
carrier materials encourages its potential application in the micro­
nutrient fortification of food and food products. The encapsulation of
micronutrients in bioaerogels favors higher loading capacity, higher
P. Selvasekaran and R. Chidambaram
encapsulation efficiency, increased stability, and better control over the
release profile of micronutrients. The dietary fiber and protein content
of various polysaccharides and protein-based aerogels, along with
encapsulated micronutrients could function as a source of nutrients in
fortified food products. Moreover, bioaerogels offer interesting oppor­
tunities for thermal insulation and mechanical protection of food
products through a smart packaging system which is highly efficient in
releasing or adsorbing sensitive compounds. The structure of bio­
aerogels offers a rousing basis for researchers to engineer material
shapes that are essential in food packaging designs.
One of the major advantages of bioaerogels includes improved sta­
bility. Specifically, protein-based aerogels remain stable and do not
disintegrate upon contact with water. The higher inner surface area of
the bioaerogels is favorable for adsorption, whereas higher porosity is
beneficial for the capillary condensation of sensitive compounds.
Excellent biocompatibility and biodegradability features are the unique
advantages of bioaerogels over other inorganic aerogels. Owing to the
low toxicity and functional biocompatibility properties, bioaerogels can
be successfully used for food-related applications. Despite various ad­
vantages, the production of bioaerogels with a controlled pore size
distribution, mesopores, and macropores is an existing challenge.
Moreover, it is not possible to fabricate stable bioaerogels without the
use of crosslinkers. The major disadvantages include the structural
destruction of end bioaerogels upon contact with the coating solution for
a longer time period and higher volume shrinkage in comparison to
synthetic aerogels. Also, the production of bioaerogels is highly time-
consuming and requires sophisticated instruments.
Future prospects regarding bioaerogels should focus on a) explora­
tion of various seed mucilages as precursors for bioaerogels production.
b) in-depth studies on biodegradation, in-vitro digestion, and swelling
kinetics of bioaerogels. c) understanding the impregnation of various
micronutrients into bioaerogels. d) investigating the direct application
of bioaerogels as fillers, thickeners, and stabilizers in various food for­
mulations. e) additives and flavors incorporation into bioaerogels to
develop them as consumable food products. f) calorific value reduction
of processed and packaged foods through the incorporation of highly
porous and ultra-low density bioaerogels. g) analyzing the real-time
effectiveness of bioaerogel packaging system on various food products.
h) evaluating the storage stability and shelf life of bioaerogels. i)
investigation of possible adverse food reactions associated with the
intake of bioaerogels. Till date, foods containing bioaerogels are not
marketed but the outlook for those products is considered major.
Therefore, rapid research on direct food applications of bioaerogels as
an ingredient and smart food packaging system is of utmost importance.
Funding
This work did not receive any specific grant from funding agencies in
public, commercial, or not-for- profit sector.
Declaration of competing interest
The authors declare no conflict of interest.
CRediT authorship contribution statement
Pavidharshini Selvasekaran: &, Acquisition of data, Formal anal­
ysis, and/or interpretation of data, Drafting the manuscript, Revising the
manuscript critically for important intellectual content, &. Ram­
alingam Chidambaram: Conception and, design of the study, Approval
of the version of the manuscript to be published.
17
Food Hydrocolloids 131 (2022) 107760
Declaration of competing interest
The authors declare no conflicts of interest.
Author’s name (typed) Author’s signature Date
Pavidharshini Selvasekaran 17–02–2022
Ramalingam Chidambaram 17–02–2022
Acknowledgment
We are thankful to the Vellore Institute of Technology for the con­
stant support of this study.
References
Abhari, N., Madadlou, A., & Dini, A. (2017). Structure of starch aerogel as affected by
crosslinking and feasibility assessment of the aerogel for an anti-fungal volatile
release. Food Chemistry, 221, 147–152. https://doi.org/10.1016/j.
foodchem.2016.10.072
Agostinho, D. A. S., Paninho, A. I., Cordeiro, T., Nunes, A. V. M., Fonseca, I. M.,
Pereira, C., et al. (2020). Properties of κ-carrageenan aerogels prepared by using
different dissolution media and its application as drug delivery systems. Materials
Chemistry and Physics, 253, 123290. https://doi.org/10.1016/j.
matchemphys.2020.123290
Ahmadi, M., Madadlou, A., & Saboury, A. A. (2016). Whey protein aerogel as blended
with cellulose crystalline particles or loaded with fish oil. Food Chemistry, 196,
1016–1022. https://doi.org/10.1016/j.foodchem.2015.10.031
Alnaief, M., Alzaitoun, M. A., & Smirnova, I. (2011). Preparation of biodegradable
nanoporous microspherical aerogel based on alginate. Carbohydrate Polymers, 84(3),
1011–1018. https://doi.org/10.1016/j.carbpol.2010.12.060
Alnaief, M., Antonyuk, S., Hentzschel, C. M., Leopold, C. S., Heinrich, S., & Smirnova, I.
(2012). A novel process for coating of silica aerogel microspheres for controlled drug
release applications. Microporous and Mesoporous Materials, 160, 167–173. https://
doi.org/10.1016/j.micromeso.2012.02.009
Alnaief, M., Obaidat, R., & Mashaqbeh, H. (2018). Effect of processing parameters on
preparation of carrageenan aerogel microparticles. Carbohydrate Polymers, 180,
264–275. https://doi.org/10.1016/j.carbpol.2017.10.038
Alnaief, M., & Smirnova, I. (2011a). Polysaccharide-based aerogels — promising
biodegradable carriers for drug delivery systems. Carbohydrate Polymers, 86,
1425–1438. https://doi.org/10.1016/j.carbpol.2011.06.066
Alnaief, M., & Smirnova, I. (2011b). In situ production of spherical aerogel
microparticles. The Journal of Supercritical Fluids, 55(3), 1118–1123. https://doi.org/
10.1016/j.supflu.2010.10.006
Amaral-Labat, G., Grishechko, L., Szczurek, A., Fierro, V., Pizzi, A., Kuznetsov, B., et al.
(2012). Highly mesoporous organic aerogels derived from soy and tannin. Green
Chemistry, 14(11), 3099–3106. https://doi.org/10.1039/c2gc36263e
Andlinger, D. J., Bornkeßel, A. C., Jung, I., Schröter, B., Smirnova, I., & Kulozik, U.
(2020). Microstructures of potato protein hydrogels and aerogels produced by
thermal crosslinking and supercritical drying. Food Hydrocolloids, 112, 106305.
https://doi.org/10.1016/j.foodhyd.2020.106305
Antonyuk, S., Heinrich, S., Gurikov, P., Raman, S., & Smirnova, I. (2015). Influence of
coating and wetting on the mechanical behaviour of highly porous cylindrical
aerogel particles. Powder Technology, 285, 34–43. https://doi.org/10.1016/j.
powtec.2015.05.004
Arboleda, J. C., Hughes, M., Lucia, L. A., Laine, J., Ekman, K., & Rojas, O. J. (2013). Soy
protein-nanocellulose composite aerogels. Cellulose, 20(5), 2417–2426. https://doi.
org/10.1007/s10570-013-9993-4
Athamneh, T., Amin, A., Benke, E., Ambrus, R., Leopold, C. S., Gurikov, P., et al. (2019).
Alginate and hybrid alginate-hyaluronic acid aerogel microspheres as potential
carrier for pulmonary drug delivery. The Journal of Supercritical Fluids, 150, 49–55.
https://doi.org/10.1016/j.supflu.2019.04.013
Betz, M., García-gonzález, C. A., Subrahmanyam, R. P., Smirnova, I., & Kulozik, U.
(2012). Preparation of novel whey protein-based aerogels as drug carriers for life
science applications. The Journal of Supercritical Fluids, 72, 111–119. https://doi.org/
10.1016/j.supflu.2012.08.019
Blanco, A., Monte, M. C., Campano, C., Balea, A., Merayo, N., & Negro, C. (2018).
Nanocellulose for industrial use. In Handbook of nanomaterials for industrial
applications. https://doi.org/10.1016/b978-0-12-813351-4.00005-5
Budtova, T. (2019). Cellulose II aerogels: A review. Cellulose, 26. https://doi.org/
10.1007/s10570-018-2189-1
Cardoso, R. V. C., Fernandes, Â., Gonzaléz-Paramás, A. M., Barros, L., &
Ferreira, I. C. F. R. (2019). Flour fortification for nutritional and health
improvement: A review. Food Research International, 125, 108576. https://doi.org/
10.1016/j.foodres.2019.108576
Chadare, F. J., Idohou, R., Nago, E., Affonfere, M., Agossadou, J., Fassinou, T. K., et al.
(2019). Conventional and food-to-food fortification: An appraisal of past practices
and lessons learned. Food Sciences and Nutrition, 7(9), 2781–2795. https://doi.org/
10.1002/fsn3.1133
Chen, C., Ding, R., Yang, S., Wang, J., Chen, W., Zong, L., et al. (2020). Development of
thermal insulation packaging film based on poly(vinyl alcohol) incorporated with
P. Selvasekaran and R. Chidambaram
silica aerogel for food packaging application. Lebensmittel-Wissenschaft & Technologie,
129, 109568. https://doi.org/10.1016/j.lwt.2020.109568
Chen, H. B., Wang, Y. Z., & Schiraldi, D. A. (2013). Foam-like materials based on whey
protein isolate. European Polymer Journal, 49(10), 3387–3391. https://doi.org/
10.1016/j.eurpolymj.2013.07.019
Chen, K., & Zhang, H. (2019). Alginate/pectin aerogel microspheres for controlled
release of proanthocyanidins. International Journal of Biological Macromolecules, 136,
936–943. https://doi.org/10.1016/j.ijbiomac.2019.06.138
Comin, L. M., Temelli, F., & Saldaña, M. D. A. (2012). Barley β-glucan aerogels as a
carrier for flax oil via supercritical CO 2. Journal of Food Engineering, 111(4),
625–631. https://doi.org/10.1016/j.jfoodeng.2012.03.005
Comin, L. M., Temelli, F., & Saldaña, M. D. A. (2015). Flax mucilage and barley beta-
glucan aerogels obtained using supercritical carbon dioxide: Application as flax
lignan carriers. Innovative Food Science & Emerging Technologies, 28, 40–46. https://
doi.org/10.1016/j.ifset.2015.01.008
De Cicco, F., Russo, P., Reverchon, E., García-González, C. A., Aquino, R. P., & Del
Gaudio, P. (2016). Prilling and supercritical drying: A successful duo to produce
core-shell polysaccharide aerogel beads for wound healing. Carbohydrate Polymers,
147, 482–489. https://doi.org/10.1016/j.carbpol.2016.04.031
De Marco, I., Baldino, L., Cardea, S., & Reverchon, E. (2015). Supercritical gel drying for
the production of starch aerogels for delivery systems. Chemical Engineering
Transactions, 43, 307–312. https://doi.org/10.3303/CET1543052
De Marco, I., & Reverchon, E. (2017). Starch aerogel loaded with poorly water-soluble
vitamins through supercritical CO2 adsorption. Chemical Engineering Research and
Design, 119, 221–230. https://doi.org/10.1016/j.cherd.2017.01.024
De Marco, I., Riemma, S., & Iannone, R. (2019). Life cycle assessment of supercritical
impregnation: Starch aerogel + А-tocopherol tablets. The Journal of Supercritical
Fluids, 143, 305–312. https://doi.org/10.1016/j.supflu.2018.09.003
Dekamin, M. G., Karimi, Z., Latifidoost, Z., Ilkhanizadeh, S., Daemi, H., Naimi-
Jamal, M. R., et al. (2018). Alginic acid: A mild and renewable bifunctional
heterogeneous biopolymeric organocatalyst for efficient and facile synthesis of
polyhydroquinolines. International Journal of Biological Macromolecules, 108,
1273–1280. https://doi.org/10.1016/j.ijbiomac.2017.11.050
Dhat, S., Naik, S. R., Amruta, A., & Parimal, K. (2009). Vitamin E loaded pectin alginate
microspheres for cosmetic application. Journal of Pharmacy Research, 2(6),
1098–1102.
Dogenski, M., Navarro-Díaz, H. J., de Oliveira, J. V., & Ferreira, S. R. S. (2020).
Properties of starch-based aerogels incorporated with agar or microcrystalline
cellulose. Food Hydrocolloids, 108, 106033. https://doi.org/10.1016/j.
foodhyd.2020.106033
Druel, L., Bardl, R., Vorwerg, W., & Budtova, T. (2017). Starch aerogels: A member of the
family of thermal superinsulating materials. Biomacromolecules, 18(12), 4232–4239.
https://doi.org/10.1021/acs.biomac.7b01272
El-Naggar, M. E., Othman, S. I., Allam, A. A., & Morsy, O. M. (2020). Synthesis, drying
process and medical application of polysaccharide-based aerogels. International
Journal of Biological Macromolecules, 145, 1115–1128. https://doi.org/10.1016/j.
ijbiomac.2019.10.037
Ephrem, E., Najjar, A., Charcosset, C., & Greige-Gerges, H. (2018). Encapsulation of
natural active compounds, enzymes, and probiotics for fruit juice fortification,
preservation, and processing: An overview. Journal of Functional Foods, 48, 65–84.
https://doi.org/10.1016/j.jff.2018.06.021
Escudero, R. R., Robitzer, M., Di Renzo, F., & Quignard, F. (2009). Alginate aerogels as
adsorbents of polar molecules from liquid hydrocarbons : Hexanol as probe
molecule. Carbohydrate Polymers, 75, 52–57. https://doi.org/10.1016/j.
carbpol.2008.06.008
Falahati, M. T., & Ghoreishi, S. M. (2019). SC. In The journal of supercritical fluids. https://
doi.org/10.1016/j.supflu.2019.04.003
Farhat, G., Lees, E., Macdonald-Clarke, C., & Amirabdollahian, F. (2019). Inadequacies of
micronutrient intake in normal weight and overweight young adults aged 18–25
years: A cross-sectional study. Public Health, 167, 70–77. https://doi.org/10.1016/j.
puhe.2018.10.016
Fontes-Candia, C., Erboz, E., Martínez-Abad, A., López-Rubio, A., & Martínez-Sanz, M.
(2019a). Superabsorbent food packaging bioactive cellulose-based aerogels from
Arundo donax waste biomass. Food Hydrocolloids, 96, 151–160. https://doi.org/
10.1016/j.foodhyd.2019.05.011
Gabor, F., Ertl, B., Wirth, M., & Mallinger, R. (1999). Ketoprofen-poly(D,L-lactic-co-
glycolic acid) microspheres: Influence of manufacturing parameters and type of
polymer on the release characteristics. Journal of Microencapsulation, 16(1), 1–12.
https://doi.org/10.1080/026520499289266
Ganesan, K., Budtova, T., Ratke, L., Gurikov, P., Baudron, V., Preibisch, I., et al. (2018).
Review on the production of polysaccharide aerogel particles. Materials, 11(11),
1–37. https://doi.org/10.3390/ma11112144
Ganesan, K., & Ratke, L. (2014). Facile preparation of monolithic κ-carrageenan aerogels.
Soft Matter, 10(18), 3218–3224. https://doi.org/10.1039/c3sm52862f
García-González, C. A., Alnaief, M., & Smirnova, I. (2011). Polysaccharide-based aerogels
- promising biodegradable carriers for drug delivery systems. Carbohydrate Polymers,
86(4), 1425–1438. https://doi.org/10.1016/j.carbpol.2011.06.066
García-González, C. A., Camino-Rey, M. C., Alnaief, M., Zetzl, C., & Smirnova, I. (2012).
Supercritical drying of aerogels using CO 2: Effect of extraction time on the end
material textural properties. The Journal of Supercritical Fluids, 66, 297–306. https://
doi.org/10.1016/j.supflu.2012.02.026
García-González, C. A., Jin, M., Gerth, J., Alvarez-Lorenzo, C., & Smirnova, I. (2015a).
Polysaccharide-based aerogel microspheres for oral drug delivery. Carbohydrate
Polymers, 117, 797–806. https://doi.org/10.1016/j.carbpol.2014.10.045
18
Food Hydrocolloids 131 (2022) 107760
García-González, C. A., & Smirnova, I. (2013a). Use of supercritical fluid technology for
the production of tailor-made aerogel particles for delivery systems. The Journal of
Supercritical Fluids, 79, 152–158. https://doi.org/10.1016/j.supflu.2013.03.001
Gawkowska, D., Cybulska, J., & Zdunek, A. (2018). Structure-related gelling of pectins
and linking with other natural compounds: A review. Polymers, 10(7). https://doi.
org/10.3390/polym10070762
Giannouli, P., & Morris, E. R. (2003). Cryogelation of xanthan. Food Hydrocolloids, 17(4),
495–501. https://doi.org/10.1016/S0268-005X(03)00019-5
Goimil, L., Braga, M. E. M., Dias, A. M. A., Gómez-Amoza, J. L., Concheiro, A., Alvarez-
Lorenzo, C., et al. (2017). Supercritical processing of starch aerogels and aerogel-
loaded poly(ε-caprolactone) scaffolds for sustained release of ketoprofen for bone
regeneration. Journal of CO2 Utilization, 18, 237–249. https://doi.org/10.1016/j.
jcou.2017.01.028
Gonçalves, V. S. S., Gurikov, P., Poejo, J., Matias, A. A., Heinrich, S., Duarte, C. M. M.,
et al. (2016). Alginate-based hybrid aerogel microparticles for mucosal drug
delivery. European Journal of Pharmaceutics and Biopharmaceutics, 107, 160–170.
https://doi.org/10.1016/j.ejpb.2016.07.003
Goslinska, M., Selmer, I., Kleemann, C., Kulozik, U., Smirnova, I., & Heinrich, S. (2019).
Novel technique for measurement of coating layer thickness of fine and porous
particles using focused ion beam. Particuology, 42, 190–198. https://doi.org/
10.1016/j.partic.2018.03.002
Groult, S., & Budtova, T. (2018a). Thermal conductivity/structure correlations in
thermal super-insulating pectin aerogels. Carbohydrate Polymers, 196, 73–81.
https://doi.org/10.1016/j.carbpol.2018.05.026
Groult, S., & Budtova, T. (2018b). Tuning structure and properties of pectin aerogels.
European Polymer Journal, 108, 250–261. https://doi.org/10.1016/j.
eurpolymj.2018.08.048
Gupta, P., Singh, B., Agrawal, A. K., & Maji, P. K. (2018). Low density and high strength
nanofibrillated cellulose aerogel for thermal insulation application. Materials and
Design, 158, 224–236. https://doi.org/10.1016/j.matdes.2018.08.031
Haimer, E., Wendland, M., Schlufter, K., Frankenfeld, K., Miethe, P., Potthast, A., et al.
(2010). Loading of bacterial cellulose aerogels with bioactive compounds by
antisolvent precipitation with supercritical carbon dioxide. Macromolecular
Symposia, 294(2), 64–74. https://doi.org/10.1002/masy.201000008
Jeffery, H., Davis, S. S., & O’Hagan, D. T. (1991). The preparation and characterisation of
poly(lactide-co-glycolide) microparticles. I: Oil-in-water emulsion solvent
evaporation. International Journal of Pharmaceutics, 77(2–3), 169–175. https://doi.
org/10.1016/0378-5173(91)90314-E
Jiménez-Saelices, C., Seantier, B., Cathala, B., & Grohens, Y. (2017). Spray freeze-dried
nanofibrillated cellulose aerogels with thermal superinsulating properties.
Carbohydrate Polymers, 157, 105–113. https://doi.org/10.1016/j.
carbpol.2016.09.068
Jin, C., Han, S., Li, J., & Sun, Q. (2015). Fabrication of cellulose-based aerogels from
waste newspaper without any pretreatment and their use for absorbents.
Carbohydrate Polymers, 123, 150–156. https://doi.org/10.1016/j.
carbpol.2015.01.056
Kadokawa, J.-I. (2011). Preparation of polysaccharide-based materials compatibilized
with ionic liquids. Ionic liquids: Applications and perspectives. https://doi.org/10.5
772/13940.
Kastner, H., Einhorn-Stoll, U., & Senge, B. (2012). Structure formation in sugar
containing pectin gels - influence of Ca2+ on the gelation of low-methoxylated
pectin at acidic pH. Food Hydrocolloids, 27(1), 42–49. https://doi.org/10.1016/j.
foodhyd.2011.09.001
Kayser, H., Müller, C. R., García-González, C. A., Smirnova, I., Leitner, W., & Domínguez
De María, P. (2012). Dried chitosan-gels as organocatalysts for the production of
biomass-derived platform chemicals. Applied Catalysis A: General, 445–446, 180–186.
https://doi.org/10.1016/j.apcata.2012.08.014
Kenar, J. A., Eller, F. J., Felker, F. C., Jackson, M. A., & Fanta, G. F. (2014). Starch aerogel
beads obtained from inclusion complexes prepared from high amylose starch and
sodium palmitate. Green Chemistry, 16(4), 1921–1930. https://doi.org/10.1039/
c3gc41895b
Kleemann, C., Schuster, R., Rosenecker, E., Selmer, I., Smirnova, I., & Kulozik, U. (2020).
In-vitro-digestion and swelling kinetics of whey protein, egg white protein and
sodium caseinate aerogels. Food Hydrocolloids, 101, 105534. https://doi.org/
10.1016/j.foodhyd.2019.105534
Kleemann, C., Selmer, I., Smirnova, I., & Kulozik, U. (2018). Tailor made protein based
aerogel particles from egg white protein, whey protein isolate and sodium caseinate:
Influence of the preceding hydrogel characteristics. Food Hydrocolloids, 83, 365–374.
https://doi.org/10.1016/j.foodhyd.2018.05.021
Kumar, A., Mishra, R., Reinwald, Y., & Bhat, S. (2010). Cryogels: Freezing unveiled by
thawing. Materials Today, 13(11), 42–44. https://doi.org/10.1016/S1369-7021(10)
70202-9
Lee, S., Kang, K. Y., Jeong, M. J., Potthast, A., & Liebner, F. (2017). Evaluation of
supercritical CO2 dried cellulose aerogels as nano-biomaterials. Journal of the Korean
Physical Society, 71(8), 483–486. https://doi.org/10.3938/jkps.71.483
Lehtonen, M., Kekäläinen, S., Nikkilä, I., Kilpeläinen, P., Tenkanen, M., &
Mikkonen, K. S. (2020). Active food packaging through controlled in situ production
and release of hexanal. Food Chemistry X, 5, 100074. https://doi.org/10.1016/j.
fochx.2019.100074
Levi, S., Rac, V., Manojlovi, V., Raki, V., Bugarski, B., Flock, T., et al. (2011). Limonene
encapsulation in alginate/poly (vinyl alcohol). Procedia Food Science, 1, 1816–1820.
https://doi.org/10.1016/j.profoo.2011.09.266
Lin, D., Zheng, Y., Huang, Y., Ni, L., Zhao, J., Huang, C., et al. (2020). Investigation of the
structural, physical properties, antioxidant, and antimicrobial activity of chitosan-
nano-silicon aerogel composite edible films incorporated with okara powder.
P. Selvasekaran and R. Chidambaram
Carbohydrate Polymers, 250, 116842. https://doi.org/10.1016/j.
carbpol.2020.116842
Li, J., Ye, T., Zhou, B., & Li, B. (2014). Facile preparation of clay reinforced konjac
glucomannan aerogels. RSC Advances, 4(42), 22251–22254. https://doi.org/
10.1039/c4ra03165b
Logeshwaran, A., Selvasekaran, P., & Chidambaram, R. (2020). Infant milk formulas. In
T. J. Guti´errez (Ed.), Food science, technology and nutrition for babies and children (pp.
3–34). https://doi.org/10.1007/978-3-030-35997-3_2
Long, L., Shen, F., Wang, F., Tian, D., & Hu, J. (2019). Synthesis, characterization and
enzymatic surface roughing of cellulose/xylan composite films. Carbohydrate
Polymers, 213, 121–127. https://doi.org/10.1016/j.carbpol.2019.02.086
Lopes, J. M., Mustapa, A. N., Pantić, M., Bermejo, M. D., Martín, Á., Novak, Z., et al.
(2017a). Preparation of cellulose aerogels from ionic liquid solutions for
supercritical impregnation of phytol. The Journal of Supercritical Fluids, 130, 17–22.
https://doi.org/10.1016/j.supflu.2017.07.018
Luiz De Paula, E., Mano, V., & Pereira, F. V. (2011). Influence of cellulose nanowhiskers
on the hydrolytic degradation behavior of poly(d,l-lactide). Polymer Degradation and
Stability, 96(9), 1631–1638. https://doi.org/10.1016/j.
polymdegradstab.2011.06.006
Maleki, H., Durães, L., García-González, C. A., del Gaudio, P., Portugal, A., &
Mahmoudi, M. (2016). Synthesis and biomedical applications of aerogels:
Possibilities and challenges. Advances in Colloid and Interface Science, 236, 1–27.
https://doi.org/10.1016/j.cis.2016.05.011
Manzocco, L., Mikkonen, K. S., & García-González, C. A. (2021). Aerogels as porous
structures for food applications: Smart ingredients and novel packaging materials.
Food Structure, 28, 100188. https://doi.org/10.1016/j.foostr.2021.100188
Manzocco, L., Valoppi, F., Calligaris, S., Andreatta, F., Spilimbergo, S., & Nicoli, M. C.
(2017). Exploitation of κ-carrageenan aerogels as template for edible oleogel
preparation. Food Hydrocolloids, 71, 68–75. https://doi.org/10.1016/j.
foodhyd.2017.04.021
Marin, M. A., Mallepally, R. R., & McHugh, M. A. (2014). Silk fibroin aerogels for drug
delivery applications. The Journal of Supercritical Fluids, 91, 84–89. https://doi.org/
10.1016/j.supflu.2014.04.014
Martins, M., Barros, A. A., Quraishi, S., Gurikov, P., Raman, S. P., Smirnova, I., et al.
(2015). Preparation of macroporous alginate-based aerogels for biomedical
applications. The Journal of Supercritical Fluids, 106. https://doi.org/10.1016/j.
supflu.2015.05.010
Maurya, V. K., Bashir, K., & Aggarwal, M. (2020). Vitamin D microencapsulation and
fortification: Trends and technologies. The Journal of Steroid Biochemistry and
Molecular Biology, 196, 105489. https://doi.org/10.1016/j.jsbmb.2019.105489
Mehling, T., Smirnova, I., Guenther, U., & Neubert, R. H. H. (2009). Polysaccharide-
based aerogels as drug carriers. Journal of Non-crystalline Solids, 355(50–51),
2472–2479. https://doi.org/10.1016/j.jnoncrysol.2009.08.038
Mikkonen, K. S., Parikka, K., Ghafar, A., & Tenkanen, M. (2013). Prospects of
polysaccharide aerogels as modern advanced food materials. Trends in Food Science &
Technology, 34(2), 124–136. https://doi.org/10.1016/j.tifs.2013.10.003
Milovanovic, S., Jankovic-Castvan, I., Ivanovic, J., & Zizovic, I. (2015). Effect of starch
xero- and aerogels preparation on the supercritical CO2 impregnation of thymol.
Starch Staerke, 67(1–2), 174–182. https://doi.org/10.1002/star.201400134
Mißfeldt, F., Gurikov, P., Lölsberg, W., Weinrich, D., Lied, F., Fricke, M., et al. (2020).
Continuous supercritical drying of aerogel particles: Proof of concept. Industrial &
Engineering Chemistry Research, 59(24), 11284–11295. https://doi.org/10.1021/acs.
iecr.0c01356
Mujumdar, A., Benali, M., & Boumghar, Y. (2014). Supercritical fluid-assisted drying.
Handbook of industrial drying, fourth edition, (july). https://doi.org/10.1201/
b17208-68, 1261-1270.
Mustapa, A. N., & Al, E. (2018). Alginate aerogels dried by supercritical Co 2.
HerbalGram, 22(3), 522–531.
Mustapa, A. N., Martin, A., Sanz-Moral, L. M., Rueda, M., & Cocero, M. J. (2016).
Impregnation of medicinal plant phytochemical compounds into silica and alginate
aerogels. The Journal of Supercritical Fluids, 116, 251–263. https://doi.org/10.1016/
j.supflu.2016.06.002
Muthukumar, J., Selvasekaran, P., Lokanadham, M., & Chidambaram, R. (2020). Food
and food products associated with food allergy and food intolerance - an overview.
Food Research International, 138, Article 109780. https://doi.org/10.1016/j.
foodres.2020.109780
Nayak, A. K., & Das, B. (2018). Introduction to polymeric gels. In Polymeric gels. https://
doi.org/10.1016/b978-0-08-102179-8.00001-6
Nešić, A., Gordić, M., Davidović, S., Radovanović, Ž., Nedeljković, J., Smirnova, I., et al.
(2018). Pectin-based nanocomposite aerogels for potential insulated food packaging
application. Carbohydrate Polymers, 195, 128–135. https://doi.org/10.1016/j.
carbpol.2018.04.076
Ni, X., Ke, F., Xiao, M., Wu, K., Kuang, Y., Corke, H., et al. (2016). The control of ice
crystal growth and effect on porous structure of konjac glucomannan-based aerogels.
International Journal of Biological Macromolecules, 92, 1130–1135. https://doi.org/
10.1016/j.ijbiomac.2016.08.020
Niknia, N., Kadkhodaee, R., & Eshtiaghi, M. N. (2020). Gum tragacanth-polyvinyl alcohol
aerogel for oral delivery of silymarin. International Journal of Biological
Macromolecules, 157, 151–157. https://doi.org/10.1016/j.ijbiomac.2020.04.202
Obaidat, R. M., Alnaief, M., & Mashaqbeh, H. (2018). Investigation of carrageenan
aerogel microparticles as a potential drug carrier. AAPS PharmSciTech, 19(5),
2226–2236. https://doi.org/10.1208/s12249-018-1021-4
de Oliveira, J. P., Bruni, G. P., el Halal, S. L. M., Bertoldi, F. C., Dias, A. R. G., & da
Zavareze, E. R. (2019). Cellulose nanocrystals from rice and oat husks and their
application in aerogels for food packaging. International Journal of Biological
Macromolecules, 124, 175–184. https://doi.org/10.1016/j.ijbiomac.2018.11.205
19
Food Hydrocolloids 131 (2022) 107760
de Oliveira, J. P., Bruni, G. P., Fabra, M. J., da Rosa Zavareze, E., López-Rubio, A., &
Martínez-Sanz, M. (2019). Development of food packaging bioactive aerogels
through the valorization of Gelidium sesquipedale seaweed. Food Hydrocolloids, 89,
337–350. https://doi.org/10.1016/j.foodhyd.2018.10.047
de Oliveira, J. P., Bruni, G. P., Fonseca, L. M., da Silva, F. T., da Rocha, J. C., & da Rosa
Zavareze, E. (2020). Characterization of aerogels as bioactive delivery vehicles
produced through the valorization of yerba-mate (Illex paraguariensis). Food
Hydrocolloids, 107, 105931. https://doi.org/10.1016/j.foodhyd.2020.105931
de Oliveira, J. P., Bruni, G. P., Lima, K. O., El Halal, S. L. M., da Rosa, G. S., Dias, A. R. G.,
et al. (2017). Cellulose fibers extracted from rice and oat husks and their application
in hydrogel. Food Chemistry, 221, 153–160. https://doi.org/10.1016/j.
foodchem.2016.10.048
Pantić, M., Knez, Ž., & Novak, Z. (2016). Supercritical impregnation as a feasible
technique for entrapment of fat-soluble vitamins into alginate aerogels. Journal of
Non-crystalline Solids, 432, 519–526. https://doi.org/10.1016/j.
jnoncrysol.2015.11.011
Pantić, M., Kotnik, P., Knez, Ž., & Novak, Z. (2016). High pressure impregnation of
vitamin D3 into polysaccharide aerogels using moderate and low temperatures. The
Journal of Supercritical Fluids, 118, 171–177. https://doi.org/10.1016/j.
supflu.2016.08.008
Plappert, S. F., Nedelec, J. M., Rennhofer, H., Lichtenegger, H. C., & Liebner, F. W.
(2017). Strain hardening and pore size harmonization by uniaxial densification: A
facile approach toward superinsulating aerogels from nematic nanofibrillated 2,3-
dicarboxyl cellulose. Chemistry of Materials, 29(16), 6630–6641. https://doi.org/
10.1021/acs.chemmater.7b00787
Plazzotta, S., Calligaris, S., & Manzocco, L. (2019). Structure of oleogels from
κ-carrageenan templates as affected by supercritical-CO 2 -drying, freeze-drying and
lettuce-filler addition. Food Hydrocolloids, 96, 1–10. https://doi.org/10.1016/j.
foodhyd.2019.05.008
Plazzotta, S., Calligaris, S., & Manzocco, L. (2020). Structural characterization of oleogels
from whey protein aerogel particles. Food Research International, 132, 109099.
https://doi.org/10.1016/j.foodres.2020.109099
Quignard, F., Valentin, R., & Di Renzo, F. (2008). Aerogel materials from marine
polysaccharides. New Journal of Chemistry, 32(8), 1300–1310. https://doi.org/
10.1039/b808218a
Quraishi, S., Martins, M., Barros, A. A., Gurikov, P., Raman, S. P., Smirnova, I., et al.
(2015). Novel non-cytotoxic alginate–lignin hybrid aerogels as scaffolds for tissue
engineering. The Journal of Supercritical Fluids, 105, 1–8. https://doi.org/10.1016/j.
supflu.2014.12.026, 2015.
Ribeiro, A., Ruphuy, G., Lopes, J. C., Dias, M. M., Barros, L., Barreiro, F., et al. (2015).
Spray-drying microencapsulation of synergistic antioxidant mushroom extracts and
their use as functional food ingredients. Food Chemistry, 188, 612–618. https://doi.
org/10.1016/j.foodchem.2015.05.061
Robitzer, Mike, Di Renzo, F., & Quignard, F. (2011a). Natural materials with high surface
area. Physisorption methods for the characterization of the texture and surface of
polysaccharide aerogels. Microporous and Mesoporous Materials, 140(1–3), 9–16.
https://doi.org/10.1016/j.micromeso.2010.10.006
Robitzer, M., Tourrette, A., Horga, R., Valentin, R., Boissière, M., Devoisselle, J. M., et al.
(2011). Nitrogen sorption as a tool for the characterisation of polysaccharide
aerogels. Carbohydrate Polymers, 85(1), 44–53. https://doi.org/10.1016/j.
carbpol.2011.01.040
Rudaz, C., Courson, R., Bonnet, L., Calas-Etienne, S., Sallée, H., & Budtova, T. (2014).
Aeropectin: Fully biomass-based mechanically strong and thermal superinsulating
aerogel. Biomacromolecules, 15(6), 2188–2195. https://doi.org/10.1021/
bm500345u
Şahin, İ., Özbakır, Y., İnönü, Z., Ulker, Z., & Erkey, C. (2017). Kinetics of supercritical
drying of gels. Gels, 4(1), 3. https://doi.org/10.3390/gels4010003
Salgado, M., Santos, F., Rodríguez-Rojo, S., Reis, R. L., Duarte, A. R. C., & Cocero, M. J.
(2017). Development of barley and yeast β-glucan aerogels for drug delivery by
supercritical fluids. Journal of CO2 Utilization, 22, 262–269. https://doi.org/
10.1016/j.jcou.2017.10.006
Sekar, P., Selvasekaran, P., Kar, A., Varalwar, T., Godli, C., & Chidambaram, R. (2020).
Lactose-free food products for lactose intolerant children. In T. J. Guti´errez (Ed.),
Food science, technology and nutrition for babies and children (pp. 143–168). https://
doi.org/10.1007/978-3-030-35997-3_7
Selmer, I., Karnetzke, J., Kleemann, C., Lehtonen, M., Mikkonen, K. S., Kulozik, U., et al.
(2019a). Encapsulation of fish oil in protein aerogel micro-particles. Journal of Food
Engineering, 260, 1–11. https://doi.org/10.1016/j.jfoodeng.2019.04.016
Selmer, I., Kleemann, C., Kulozik, U., Heinrich, S., & Smirnova, I. (2015). Development of
egg white protein aerogels as new matrix material for microencapsulation in food.
The Journal of Supercritical Fluids, 106. https://doi.org/10.1016/j.
supflu.2015.05.023
Selvasekaran, P., & Chidambaram, R. (2021a). Advances in formulation for the
production of low-fat, fat-free, low-sugar, and sugar-free chocolates: An overview of
the past decade. Trends in Food Science & Technology, 113, 315–334. https://doi.org/
10.1016/j.tifs.2021.05.008
Selvasekaran, P., & Chidambaram, R. (2021b). Trends in Food Science & Technology
Food-grade aerogels obtained from polysaccharides , proteins , and seed mucilages :
Role as a carrier matrix of functional food ingredients. Trends in Food Science &
Technology, 112, 455–470. https://doi.org/10.1016/j.tifs.2021.04.021
Selvasekaran, P., Mahalakshmi Roshini, F., Angalene, L. A., Chandini Sunil, T., &
Chidambaram, R. (2021). Fungal exopolysaccharides: Production and
biotechnological industrial applications in food and allied sectors. https://doi.org
/10.1007/978-3-030-68260-6_12.
da Silva, F. T., de Oliveira, J. P., Fonseca, L. M., Bruni, G. P., da Rosa Zavareze, E., &
Dias, A. R. G. (2020). Physically cross-linked aerogels based on germinated and non-
P. Selvasekaran and R. Chidambaram
germinated wheat starch and PEO for application as water absorbers for food
packaging. International Journal of Biological Macromolecules, 155, 6–13. https://doi.
org/10.1016/j.ijbiomac.2020.03.123
Soorbaghi, F. P., Isanejad, M., Salatin, S., Ghorbani, M., Jafari, S., & Derakhshankhah, H.
(2019). Bioaerogels: Synthesis approaches, cellular uptake, and the biomedical
applications. Biomedicine & Pharmacotherapy, 111, 964–975. https://doi.org/
10.1016/j.biopha.2019.01.014
Spagnol, C., Rodrigues, F. H. A., Pereira, A. G. B., Fajardo, A. R., Rubira, A. F., &
Muniz, E. C. (2012). Superabsorbent hydrogel nanocomposites based on starch-g-
poly(sodium acrylate) matrix filled with cellulose nanowhiskers. Cellulose, 19(4),
1225–1237. https://doi.org/10.1007/s10570-012-9711-7
Stievano, M., & Elvassore, N. (2005). High-pressure density and vapor-liquid equilibrium
for the binary systems carbon dioxide-ethanol, carbon dioxide-acetone and carbon
dioxide- dichloromethane. The Journal of Supercritical Fluids, 33(1), 7–14. https://
doi.org/10.1016/j.supflu.2004.04.003
Subrahmanyam, R., Gurikov, P., Dieringer, P., Sun, M., & Smirnova, I. (2015). On the
road to biopolymer aerogels—dealing with the solvent. Gels, 1(2), 291–313. https://
doi.org/10.3390/gels1020291
Tkalec, G., Knez, Ž., & Novak, Z. (2015a). Fast production of high-methoxyl pectin
aerogels for enhancing the bioavailability of low-soluble drugs. The Journal of
Supercritical Fluids, 106. https://doi.org/10.1016/j.supflu.2015.06.009
Tkalec, G., Knez, Ž., & Novak, Z. (2015b). Formation of polysaccharide aerogels in
ethanol. RSC Advances, 5(94), 77362–77371. https://doi.org/10.1039/c5ra14140k
Ubeyitogullari, A., Brahma, S., Rose, D. J., & Ciftci, O. N. (2018). In vitro digestibility of
nanoporous wheat starch aerogels. Journal of Agricultural and Food Chemistry, 66(36),
9490–9497. https://doi.org/10.1021/acs.jafc.8b03231
Ubeyitogullari, A., & Ciftci, O. N. (2016). Phytosterol nanoparticles with reduced
crystallinity generated using nanoporous starch aerogels. RSC Advances, 6(110),
108319–108327. https://doi.org/10.1039/c6ra20675a
Ubeyitogullari, A., & Ciftci, O. N. (2019). In vitro bioaccessibility of novel low-
crystallinity phytosterol nanoparticles in non-fat and regular-fat foods. Food Research
International, 123, 27–35. https://doi.org/10.1016/j.foodres.2019.04.014
Ubeyitogullari, A., & Ciftci, O. N. (2020). Fabrication of bioaerogels from camelina seed
mucilage for food applications. Food Hydrocolloids, 102, 105597. https://doi.org/
10.1016/j.foodhyd.2019.105597
20
Food Hydrocolloids 131 (2022) 107760
Veronovski, A., Tkalec, G., Knez, Z., & Novak, Z. (2014). Characterisation of
biodegradable pectin aerogels and their potential use as drug carriers. Carbohydrate
Polymers, 113, 272–278. https://doi.org/10.1016/j.carbpol.2014.06.054
Villegas, M., Oliveira, A. L., Bazito, R. C., & Vidinha, P. (2019). Development of an
integrated one-pot process for the production and impregnation of starch aerogels in
supercritical carbon dioxide. The Journal of Supercritical Fluids, 154. https://doi.org/
10.1016/j.supflu.2019.104592
Wang, Y., Su, Y., Wang, W., Fang, Y., Riffat, S. B., & Jiang, F. (2019). The advances of
polysaccharide-based aerogels: Preparation and potential application. Carbohydrate
Polymers, 226, 115242. https://doi.org/10.1016/j.carbpol.2019.115242
Wang, Y., Wu, K., Xiao, M., Riffat, S. B., Su, Y., & Jiang, F. (2018). Thermal conductivity,
structure and mechanical properties of konjac glucomannan/starch based aerogel
strengthened by wheat straw. Carbohydrate Polymers, 197, 284–291. https://doi.org/
10.1016/j.carbpol.2018.06.009
Wang, L., & Zhao, S. (2009). Synthesis and characteristics of mesoporous silica aerogels
with one-step solvent exchange/surface modification. Journal of Wuhan University of
Technology-Materials Science Edition, 24(4), 613–618. https://doi.org/10.1007/
s11595-009-4613-8
Xin, C., Chen, J., Liang, H., Wan, J., Li, J., & Li, B. (2017). Confirmation and
measurement of hydrophobic interaction in sol-gel system of konjac glucomannan
with different degree of deacetylation. Carbohydrate Polymers, 174, 337–342.
https://doi.org/10.1016/j.carbpol.2017.06.088
Zheng, Q., Tian, Y., Ye, F., Zhou, Y., & Zhao, G. (2020). Fabrication and application of
starch-based aerogel: Technical strategies. Trends in Food Science & Technology, 99
(March), 608–620. https://doi.org/10.1016/j.tifs.2020.03.038
Zhu, F. (2019). Starch based aerogels: Production, properties and applications. Trends in
Food Science & Technology, 89, 1–10. https://doi.org/10.1016/j.tifs.2019.05.001
Zhu, T., Mao, J., Cheng, Y., Liu, H., Lv, L., Ge, M., et al. (2019). Recent progress of
polysaccharide-based hydrogel interfaces for wound healing and tissue engineering.
Advanced Materials Interfaces, 6(17), 1–22. https://doi.org/10.1002/
admi.201900761
Zuo, L., Zhang, Y., Zhang, L., Miao, Y. E., Fan, W., & Liu, T. (2015). Polymer/carbon-
based hybrid aerogels: Preparation, properties and applications. Materials, 8. https://
doi.org/10.3390/ma8105343