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International Journal of Food Science and Technology 2022, 57, 4441–4450 4441

Original article
Characterisation of hydrogels and aerogels as carriers for sea
buckthorn pomace extract

Greta Švermickaitė, Viktorija Eisinaitė,* Rimantė Vinauskienė, Ina Jasutienė & Daiva Leskauskaitė
Department of Food Science and Technology, Kaunas University of Technology, Radvilenu pl 19, Kaunas LT-50254, Lithuania

(Received 25 February 2022; Accepted in revised form 19 April 2022)

Summary In this study, aerogels were prepared from kognac glucomannan (KG) or whey proteins loaded with bio-
active sea buckthorn pomace extract. KG was diacetylated with Na2CO3 (0.1; 0.2; 0.3; 0.4 M) resulting
hydrogel formation that were further freeze-dried to obtain an aerogel structure. Whey protein aerogels
were prepared by removing pore fluid from alcogels using supercritical CO2 drying. Produced aerogels
evaluated for microstructure, porosity, specific surface area, absorption capacity, encapsulation efficiency
and antioxidant capacity of the extract. It was found that higher concentration of alkali induced higher
hardness, resilience and elastic modulus values. It was also obtained that pores in the konjac glucoman-
nan aerogels were irregular in shape and a decrease in total pore volume (0.026 to 0.019 cc/g) and surface
area (12.39 to 11.40 m2/g) after increasing the carbonate concentration was observed. These aerogels were
found to have better encapsulation efficiency properties for sea buckthorn pomace extract (17 to 20%) in
comparison to whey protein aerogels (0.05 to 0.36%). Overall, the KG aerogels show potential for appli-
cations in the food industry as a carrier of bioactive sea buckthorn pomace extract, while whey proteins
must be used in combination with other biopolymers to enhance their bioactive compound loading
capacity.
Keywords Aerogel, encapsulation, food matrix, sea buckthorn.

supercritical CO2 drying (Selvasekaran & Chidam-

Introduction
Bioactive compounds obtained from natural sources
have been increasingly investigated with regard to their
characterisation, application and protection against
degradation. Various encapsulation and delivery
methods are used to protect these unstable compounds
from unfavourable conditions during processing and
storage (Aditya et al., 2017; Niu et al., 2020). It was
previously reported that different techniques such as
freeze-drying, spray-drying, liposomes, molecular
inclusion, coacervation, extrusion, supercritical fluids,
polymeric micelles, nanostructured lipid matrices and
solvent evaporation have been used for bioactive com-
pound encapsulation (Aguiar et al., 2016; Gómez et
al., 2018). The properties and structure of encapsula-
tion systems play an important role in encapsulation
efficiency and the potential application of encapsulated
compounds. Among these systems, aerogels appear to
be a very promising carrier matrix for lipophilic and
hydrophilic bioactive compounds. Aerogels are special
type of porous material obtained from a gel by remov-
ing the pore fluid via air drying, freeze-drying or
*Correspondent: E-mail: viktorija.eisinaite@ktu.lt
baram, 2021). These delivery systems could be fabri-
cated with controlled structural properties, high
specific surface areas and high porosities. Low density
and good mechanical strength of aerogels is associated
with high loading capacity, improved bioavailability
and targeted compound release (Kleemann et al., 2018;
de Oliveira et al., 2020). Another important advantage
is that these systems do not involve high temperatures
during the encapsulation process, which may protect
thermally labile ingredients (Shishir & Chen, 2017).
The properties of aerogels depend on the gelation con-
ditions (gelator type and concentration, gelation
method), solvent exchange step (solvent type) and dry-
ing techniques (Selvasekaran & Chidambaram, 2021).
Of the aforementioned properties, the type of biopoly-
mer used is the most important factor. The most com-
mon bio-based materials that used for the preparation
of aerogels include biopolymers such as polysaccha-
rides (e.g. starch, alginate, pectin, κ-carrageenan, cellu-
lose, konjac glucomannan and xanthan gum) and
proteins (e.g. whey proteins, egg white protein, sodium
caseinate, gelatin, collagen and soy proteins; Selmer et
al., 2015; Wang et al., 2018; Manzocco et al., 2021).
Such natural biopolymers are good precursors for

doi:10.1111/ijfs.15777
© 2022 Institute of Food Science and Technology

4442 Differently structured bioactive extract aerogels G. Švermickaitė et al.
aerogel formation since are non-toxic, economical and
environmentally friendly materials.
Aerogels were already used as carriers for pinhão
coat extract (Fonseca et al., 2021) and yerba-mate (de
Oliveira et al., 2020).
Sea buckthorn (Hippophae rhamnoides L.) is an
exceptional plant since it is a well-known natural
source of vitamins, minerals, antioxidants and flavo-
noids that is valuable for its nutritional and health-
promoting properties (Shah et al., 2007). Its positive
nutritional composition—especially its high amounts
of antioxidants—provides opportunities to use it as a
whole plant or extract its nutritionally abundant by-
products through various extraction techniques. How-
ever, the sensitivity of antioxidants rich extracts to
environmental conditions could cause their degrada-
tion and decreased stability (Zhang et al., 2014). It
was previously reported that sea buckthorn extract
was encapsulated in nanostructured lipid carriers
(Manea et al., 2014) and microcapsules by using beta-
glucan as a wall material (Drozińska et al., 2019).
Moreover, sea buckhorn carotenoids were encapsu-
lated with whey protein isolate by coacervation and
freeze-drying (Mihalcea et al., 2017) or via a transglu-
taminase mediated cross-linking reaction, coacervation
and freeze-drying (Mihalcea et al., 2018). To the best
of our knowledge, the use of food-grade aerogels as a
carrier matrix for sea buckthorn extract has not been
reviewed to date. It is strongly believed that the devel-
opment of suitable delivery systems for hydrophilic
bioactive sea buckthorn pomace extract could over-
come the limitations of its direct application in foods.
Therefore, this study aimed to formulate differently
structured kognac glucomannan (KG) and whey pro-
tein aerogel carriers for bioactive sea buckthorn pom-
ace extract intended for food applications. KG-based
aerogels were obtained by freeze-drying from hydro-
gels with different sodium carbonate concentrations
(0.1, 0.2, 0.3, 0.4 M). Whey protein-based aerogels were
obtained from whey protein alcogels after supercritical
CO2 drying. The prepared aerogels were characterised
using scanning electron microscopy, porosymmetric
method and texture analysis. Finally, extract obtained
from sea buckthorn pomace was encapsulated into
aerogels via the post-drying impregnation method. The
absorption capacity, encapsulation efficiency and anti-
oxidant capacity during the storage of uploaded aero-
gels were analysed.
Materials and methods
Materials
Materials used for aerogel production: whey protein iso-
late (WPI) containing 89.7
0.3% protein, 6.0
0.1%
moisture, 4.0
0.1% ash, 0.2% fat and 0.1% lactose
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(Lacprodan DI-9213, Arla Foods Ingredients Group,
Denmark), KG with a purity of >99.5% (Blackburn Dis-
tributions, Great Britain). Sodium carbonate was
obtained from Sigma-Aldrich (Steinheim, Germany).
The extract was made from sea buckthorn pomace
obtained by pressing berries in a Philips HR1880/01 juicer.
The pomace was immediately dried, ground in a high-
speed centrifugal mill (Retsch ZM200, Haan, Germany)
using a 0.2 mm sieve and extracted with supercritical CO2
in a pilot-scale system (Applied Separation, Allentown,
USA) to remove the lipophilic fraction. The defatted resi-
due was extracted with agricultural origin ethanol (Stum-
bras, Kaunas, Lithuania) in a pilot-scale Soxhlet-type
extractor. Extraction parameters were selected
Ç based on
the previously reported studies (Grunovaite et al., 2016).
The ethanol was removed in a rotary vacuum evaporator
at 40 °C temperature and the solvent-free extract was
stored at 4 °C until use. The extract contained 72.6

0.1 mg/g of polyphenolics (expressed in gallic acid
equivalents) and 333.1
7.0 mg/g procyanidins (deter-
mined spectrophotometrically). Consequently, the extract
may be considered rich in phenols.
Methods
Kognac glucomannan hydrogel preparation
The KG hydrogels were prepared by diacetylation
according to Herranz et al. (2012) with modifications.
Briefly, 2 g of KG was mixed with 0.1, 0.2, 0.3 or
0.4 M Na2CO3 aqueous solutions (pH 11.40 to 11.64).
It has been reported that KG gelation starts at pH
11.3 to 12.6 (Liu et al., 2018). The obtained mixtures
were placed in an 80 °C water bath (Isotemp 205,
Thermo Fisher Scientific Baltics, Vilnius, Lithuania) for
30 min. The prepared gels were cooled to room tem-
perature and aged at 5 °C for 24 h until further testing
or aerogel production. Each sample was prepared in
triplicate for technological replicates.
Kognac glucomannan aerogel preparation
KG aerogels were prepared according to the previ-
ously reported method with slight modifications (Wu
et al., 2022). The KG hydrogels (prepared according
to the aforementioned description) were cut into
square cubes (1.5 × 1.5 × 1.5 cm3) and placed in a
freezer (−18 °C) for 24 h. The frozen cube-shaped gels
were dried in a freeze-dryer (Sublimator 3 × 4 × 5 Zir-
bus technology, Bad Grund, Germany) for 48 h by
reducing the pressure from 0.20 to 0.01 mbar and
increasing the plate temperature from 20 to 35 °C The
obtained aerogels were stored in sealed containers at
room temperature until further analysis.
Whey protein aerogel preparation
Whey protein aerogels were prepared by the solvent
exchange and the supercritical extraction procedure
© 2022 Institute of Food Science and Technology

described by other authors (Selmer et al., 2015; Klee-
mann et al., 2018), with some minor modifications.
Firstly, 20% w/w of WPI was dissolved into distilled
water on a magnetic stirrer for 2 h. The protein solu-
tion was then placed in a water bath at 80 °C for
10 min and the obtained gel was cooled to room tem-
perature (
20 °C). Cylindrical thermogel samples
(10 mm in diameter) were then placed in a beaker and
filled with pure ethanol (98%). The solvent exchange
with pure ethanol was repeated three times to obtain
alcogel. The obtained alcogels were then dried with
supercritical CO2 in a Helix extractor (Applied Separa-
tion, Allentown, PA, USA). Thereafter, samples were
wrapped in ethanol-soaked filter paper and placed in a
50 cm3 extractor vessel, where dynamic extraction was
carried out for 5 to 6 h (P = 12 Mpa; T = 40 °C)
using a continuous supercritical flow. A static time of
10 min was included in the total extraction time.
Kognac glucomannan hydrogel characterisation
Swelling ratio. For the swelling ratio (SR) evaluation,
the weight changes of hydrogels were recorded as a
function of immersion time. The hydrogels were
immersed in distilled water at room temperature and
changes in the weights of hydrated hydrogels were
monitored at different time intervals (0, 30, 60, 90,
120, 150, 180, 210 and 240 min). The SR was calcu-
lated according to the following equation:
WAFI  WI
SR ð%Þ ¼  100 (1)
WI
where SR—swelling ratio, %; WAFI—weight of hydro-
gel after immersion in water, g; WI—initial weight of
hydrogel, g.
Texture profile analysis. The texture profile analysis of
hydrogels was performed using a texture analyser
(TA.XTplus, StableMicro Systems, UK) equipped with
a cylinder aluminium probe (P/100; ø 100 mm)). Cube-
shaped samples (20 × 30 × 30 cm3) were placed on the
texture analyser base and exposed by uniaxial two-cycle
compression to 50% of their initial height. Test condi-
tions were as follows: pre-test speed = 3 mm/s; test
speed = 1 mm/s; post-test speed = 5 mm/s. The evalu-
ated parameters included hardness, springiness and
resilience.
Rheological behaviour of hydrogels. The rheological
behaviour of hydrogels was analysed using a Physica
MCR 502 rheometer (Anton Paar, Messtechnik, Stutt-
gart, Germany) equipped with a temperature control
unit (CF41 Cryo-Compact Circulator, Julabo, Zel-
bach, Germany) and plate–plate geometry (PP/50,
diameter 24.966 mm) with a 1-mm gap. Temperature
sweep experiments were performed within the linear
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Differently structured bioactive extract aerogels G. Švermickaitė et al. 4443
viscoelastic region. Two sweeps (heating-cooling) were
performed between 25 and 85 °C at a rate of 5 °C/
min. A solvent trap was used to prevent sample
dehydration.
Kognac glucomannan and whey protein aerogel
characterisation
Microstructure. The microstructures of aerogels were
examined using an FEI Quanta 200 FEG scanning
electron microscope (SEM; Eindhoven, The Nether-
lands). Samples were placed on the microscope stubs
using double-sided adhesive carbon tape. Samples were
analysed in low-vacuum mode at an accelerated volt-
age (10 kV).
Porosity and specific surface area. The porosities of the
aerogels were determined via the porosymmetric
method from nitrogen adsorption–desorption iso-
therms at 196 °C (77 K) using an automatic gas sorp-
tion analyser (Quantachrome Autosorb-iQ-KR/MP,
USA). Prior to the nitrogen adsorption analysis, the
samples were degassed under vacuum at 80 °C. The
specific surface areas of the samples were calculated
using the Brunauer-Emmett-Teller (BET) equation.
The total pore volume of the samples was determined
from the nitrogen adsorption isotherms at a relative
pressure p/p0 of 0.99. All calculations were performed
using AsiQwin (version 2.0; Quantachrome).
Absorption capacity of sea buckthorn pomace extract. The
absorption capacity test was carried out by preparing
aqueous solutions with three different concentrations
(15%, 20% and 25%) of sea buckthorn pomace
extract measured as a function of time. Briefly, a
known amount of aerogel was immersed in 50 ml of
extract solution and stored for 240 h. After 24, 72,
120, 168 and 240 h, the aerogel samples were removed,
tapped with filter paper to remove free solution, and
weighing (wet aerogels). The absorption capacity of
sea buckthorn pomace extract was calculated accord-
ing to the following equation:
ASW  ASD
AC ð%Þ ¼  100 (2)
ASD
where AC—absorption capacity, %; ASW—weight of
swollen aerogel sample, g; ASD—weight of dry aerogel
sample, g.
Encapsulation efficiency of sea buckthorn pomace extra-
ct. The encapsulation efficiency of sea buckthorn
pomace extract in the aerogel structures was deter-
mined by the spectrophotometric method. Extract-
absorbed aerogel samples were centrifuged (Heraeus
Labofuge 200, ThermoScientific, Osterode, Germany)
at 3312 x g for 30 min. The absorbance of the released
International Journal of Food Science and Technology 2022

4444 Differently structured bioactive extract aerogels G. Švermickaitė et al.
supernatant was measured with an Evolution 300 spec-
trophotometer (Thermo Fisher Scientific, Roskilde,
Denmark) at 520 nm. A calibration curve was used to
calculate the actual concentration. This was prepared
by adding a known amount of sea buckthorn pomace
extract to the distilled water. The calibration curve
had an R2 correlation coefficient of 0.9934. The encap-
sulation efficiency was calculated using the following
equation:
CEN
EE ð%Þ ¼  100 (3)
CT
where EE—encapsulation efficiency, %; CEN—concen-
tration of encapsulated SBPE; CT—concentration of
total absorbed SBPE.
Antioxidant capacity. Antioxidant capacity was deter-
mined using an e-BQC lab device (Bioquochem, Astu-
rias, Spain) to measure redox potential. Extract-
absorbed aerogel samples were centrifuged (Heraeus
Labofuge 200, Thermo Scientific, Osterode, Germany)
and the separated supernatants were used for the anti-
oxidant capacity evaluation. The obtained results are
expressed as QT, which is the sum of the antioxidant
capacities of the compounds with the highest (Q1) and
the lowest (Q2) rates of free radical scavenging. The
results are expressed in microcoulombs (μC).
Statistical analysis
All analyses were carried out in triplicate. The results
are presented as the mean
standard deviation. The
Figure 1 Temperature sweep curves of KG hydrogels obtained after deacetylation with different sodium carbonate concentration at heating (a)
and cooling stages (b). Full marks—G0 values, empty marks—G″ values.
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data were analysed using one-way ANOVA with Statis-
tica 12.0 (StatSoft, Inc., 2013). The means were com-
pared by the Duncan multiple-range test at P < 0.05.
XLSTAT software was used.
Results and discussion
Kognac glucomannan hydrogel characterisation
As a preliminary step to formulating the KG aerogels
by freeze-drying, we determined the characteristics of
the KG hydrogels. Hydrogels were obtained after dea-
cetylation with different sodium carbonate concentra-
tions and were characterised by their thermal
behaviour, SR and textural properties to assess their
suitability as a matrix for aerogel production. Stable
form-retaining hydrogels were obtained at all tested
concentrations of sodium carbonate and exhibited
solid-like behaviour, whereas G0 was always larger
than G″ (Fig. 1a). This is attributed to the alkaline-
induced deacetylation of KG, which results in hydro-
gen bonding between deacetylated glucomannan mole-
cules (Liu et al., 2018). The strength of the formed
gels was slightly affected by the concentration of the
alkali used for the formulation. After exposure at
80 °C for 30 min, the sample consisting of KG and
0.4 M Na2CO3 exhibited a sharp increase in gel
strength (Fig. 1b), as confirmed by the significant
increase in G0 and G″ values. Meanwhile, a no-change
trend (similar G0 and G″ values) was observed with a
constantly decreasing temperature in the remaining
samples (Fig. 1b). These results indicate that a high
© 2022 Institute of Food Science and Technology

Figure 2 Swelling kinetics of KG hydrogels obtained after deacetyla-
tion with different sodium carbonate concentration (0.1, 0.2, 0.3,
0.4 M) in distilled water.
concentration of alkali induces the formation of a
denser network structure. Gelation is fulfilled after
heating and subsequent cooling, whereas thermally
irreversible gels are formed (and significant agglomera-
tion is initiated) not only by hydrogen bonds but also
by hydrophobic interactions (Zhou et al., 2018).
Water absorption capacity—expressed as SR—indi-
rectly showed the number of structural sites capable of
molecule absorption. The samples displayed similar
swelling behaviour, with some slight differences
(Fig. 2). An increase in water uptake was observed
during the entire hydrogel immersion period. However,
the hydrogels absorbed a very small amount of water
in comparison to other studies (Herranz et al., 2012),
in which the amount of water absorbed differed by 10-
fold.
It was also observed that an increase in alkali con-
centration induced increases in hardness, springiness,
resilience and elastic modulus (G0 ; Table 1). These
results indicate that more intensive intermolecular
interactions occurred at higher alkali concentrations
and caused denser hydrogel matrix formation, which is
in agreement with other studies (Herranz et al., 2012;
Liu et al., 2018). It was also previously reported that
the type of the alkali could also slightly contribute to
Table 1 Textural properties of KG hydrogels obtained after deacetylation with different sodium carbonate concentration
Sample Hardness, N Springiness, mm
KGH_0.1M 0.89
0.02a 0.793
0.013a
KGH_0.2M 0.91
0.08a 0.834
0.053a
KGH_0.3M 1.06
0.02b 0.824
0.001a
KGH_0.4M 1.09
0.09b 0.914
0.040b
Values are means
SD. Means in the same column, followed by the different letters, indicate significant difference between the hydrogels deacety-
lated with different sodium carbonate concentration.
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Differently structured bioactive extract aerogels G. Švermickaitė et al. 4445
the degree of hydration of the structure that related
with the different radius of the ions (Herranz et al.,
2012) Greater structural homogeneity is a desirable
property in the case of hydrogels. However, if these
systems would be used as precursors for aerogel for-
mation, this can be an undesirable phenomenon.
Structures with greater integrity could have a lower
number of pores per unit area, resulting in a lower
degree of absorption and leading to a decrease in the
encapsulation efficiency of bioactive extracts.
Kognac glucomannan aerogel characterisation
One of the main properties of aerogels is the morphol-
ogy of the structure since these systems would be used
for the post-drying impregnation of sea buckthorn
pomace extract. The morphology of aerogels was stud-
ied by SEM to obtain the images presented in Fig. 3.
All aerogels had homogeneous and microporous struc-
tures with randomly oriented pores of unequal size
and shape. This is in line with other studies reporting
that konjac glucomannan aerogels are not charac-
terised as having an orderly structure (Wang et al.,
2019). The morphology of food-grade polysaccharide
aerogels significantly depends on the type of polysac-
charide used; for example, aerogels made with pectin
or cellulose were characterised as having more com-
pact and well-organised structures (de Oliveira et al.,
2020). Again, it is important to note that such a rigid
well-organised structure is sometimes undesirable
because it could slow down the absorption of biologi-
cally active compounds.
With increased alkali concentration, the BET surface
area and total pore volume values became lower (from
12.39 to 11.40 m2/g and from 0.026 to 0.019 cc/g,
respectively), indicating a more organised three-
dimensional network formation (previously discussed
in the hydrogels section) that was also confirmed by
the SEM images (Fig. 3). The obtained results
(Table 2) show that the structure of KG aerogels can
easily be managed as needed by changing the alkali
concentration. The structure of konjac glucomannan
aerogels could also be modified by adding other food-
grade polysaccharides such as potato starch (Wang
et al., 2019), changing the konjac glucomannan
Resilience *
G0 , Pa at 50 Hz
0.236
0.013ab 7163
1550a
0.230
0.040a 7260
2318a
0.258
0.086ab 255 000
4301b
0.350
0.020b 322 433
3528c
International Journal of Food Science and Technology 2022

4446 Differently structured bioactive extract aerogels G. Švermickaitė et al.
Table 2 Physical properties of aerogels obtained after deace-
tylation with different sodium carbonate concentration
Aerogel sample
KGC with different Na2CO3
concentrations
Physical properties 0.2 M 0.3 M 0.4
BET surface area, m /g2
12.39 13.27 11.40
Total pore volume, cc/g 0.026 0.028 0.019
R2 0.999 0.999 0.999
concentration (Ni et al., 2016) and altering the pre-
freezing temperature (Li et al., 2014).
It is well known that aerogel morphology directly
affects the kinetics of absorption as well as the release
of the compounds uploaded to the aerogels (de Oli-
veira et al., 2020). Higher porosity is a desirable prop-
erty if the aerogel is to be used as a carrier matrix for
bioactive compounds. However, it is important to con-
sider that the bioactive compounds must be not only
successfully absorbed but also maintained in the struc-
ture over a longer period. Therefore, to better charac-
terise the produced aerogels, the absorption capacity
and encapsulation efficiency were studied.
The absorption capacity of aerogels was evaluated
by immersion in sea buckthorn pomace extract solu-
tions with varying concentrations (15%, 20% and
25%). It was found (Fig. 4) that the absorption rate of
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Figure 3 SEM morphological images of KG
aerogels obtained after deacetylation with
0.3 M (a, b) and 0.4 M (c, d) sodium carbon-
ate concentration. Yellow scale bars repre-
sent 1 mm (a, c) and 200 µm (b, d).
the extract increased during storage, while the diffu-
sion rate remained the same in all systems for up to
24 h. However, during subsequent storage, the rela-
tionship between the concentration of sodium carbon-
ate used in the production of aerogels and their
absorption capacity was clearly visible. As expected,
the lowest amounts of absorbed extract were observed
M WPA
in the samples with the highest alkali concentration
3.86 since those samples were characterised by a denser and
0.013 less porous structure. Meanwhile, the maximum
0.999 absorption capacity of sea buckthorn pomace extract
(10–14%) was achieved in the samples deacetylated
with 0.2 M sodium carbonate. It is believed that this
was the maximum absorption limit of obtained struc-
ture. According to Esquivel-Castro et al. (2019), a
more porous structure with a larger surface area facili-
tates the movement of a solution through the matrix
via capillarity, which improves the water absorption
capacity. Additionally, the lowest absorption capacity
obtained in the samples was observed for the highest
tested extract concentration (25%). A possible reason
for this phenomenon is the different viscosities of the
extract solutions, which increased from 0.043 to
0.162 Pas with increasing extract concentration (from
15 to 25%). Moreover, it is strongly believed that a
higher viscosity slows down the penetration of extracts
into the structures of aerogels.
Finally, the aerogel with the highest absorption
capacity (0.2 M Na2CO3) was chosen for the
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Differently structured bioactive extract aerogels G. Švermickaitė et al. 4447

Figure 4 Absorption capacity of KG aerogels obtained after deacetylation with different sodium carbonate concentration at different hydro-
philic sea buckthorn pomace extract concentrations (a) 15%, (b) 20%; (c) 25%.

Table 3 Encapsulation efficiency of sea buckthorn pomace extract (15%) in KG aerogels (diacetylated with 0.2 M Na2CO3) and it
antioxidant activity during storage

Time, h

24 48 96 168 240

Encapsulation efficiency, % 16.99
0.71a 19.73
0.34ab 20.21
0.52b 19.97
0.30ab 19.73
0.37ab
Antioxidant capacity, QT µc 48.15
1.21a 87.60
1.03b 125.80
2.97c 150.19
0.89d 146.80
1.41d

Values are means
SD. Means in the same row, followed by the different letters, indicate significant difference in sample during storage.

subsequent analysis of its encapsulation efficiency
and antioxidant capacity. In these analyses, the low-
est tested extract concentration (15%) was used to
achieve the fastest extract diffusion rate. Encapsula-
tion efficiency and antioxidant capacity increased
slightly during the immersion process since these fac-
tors were directly affected by the absorption rate of
the extract solution. Regarding the encapsulation effi-
ciency, it was observed that aerogels retained ~20%
of the total absorbed extract in their network struc-
tures (Table 3). Although the encapsulation efficiency
was not as high as expected, the amount of extract
immobilised in aerogels retained its antioxidant prop-
erties. This shows that the aerogel matrix acts as a
barrier that prevents the degradation and fast action
of bioactive compounds, which is in agreement with
previous studies (de Oliveira et al., 2020; Fonseca
et al., 2021).

© 2022 Institute of Food Science and Technology International Journal of Food Science and Technology 2022

4448 Differently structured bioactive extract aerogels G. Švermickaitė et al.
Figure 6 Absorption capacity of whey protein aerogels at different
sea buckthorn pomace extract solutions (15%, 20% and 25%).
Whey protein aerogel characterisation
Aerogels were also obtained from whey proteins after
supercritical CO2 drying and their properties were
evaluated. When comparing the morphology of whey
protein and KG aerogels, differences were observed in
their porosities, which indicates that the type of the
structuring agent and drying method applied strongly
affected the external and internal appearances of aero-
gels. As shown in Fig. 5, whey protein aerogels had a
more compact—and thus less porous—structure, with
spherical pores that resulted in a lower BET surface
area (3.86 m2/g) and total pore volume (0.013 cc/g; see
Table 2). Higher BET surface area (350–450 m2/g) was
reported in aerogels formulated using other proteins
such as silk fibroin, egg and casein (Marin et al., 2014;
Selmer et al., 2015, 2019). Aerogels with solid and
robust protein network have previously been produced
by other authors (Mine, 1995; Kleemann et al., 2018).
Due to the formation of covalent disulphide bonds
during hydrogel production, the collapse of aerogel
structures was avoided in the aqueous environment,
International Journal of Food Science and Technology 2022
13652621, 2022, 7, Downloaded from https://ifst.onlinelibrary.wiley.com/doi/10.1111/ijfs.15777 by Kaunas University Of, Wiley Online Library on [16/03/2023]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Figure 5 SEM morphological image of whey
protein aerogel prepared with 15% of whey
proteins. Yellow scale bars represent 10 µm
(a) and 20 µm (b).
which makes them very attractive for use in the food
industry (Betz, Hörmansperger, et al., 2012b).
Regarding the absorption capacity of the whey pro-
teins aerogels, their rigid structure was able to absorb
much lower amounts of the extracts (1.0–2.5%) when
compared to the KG aerogels (Fig. 6). These results are
attributed to their lower porosity, which reduced the
ability of the extract to penetrate the aerogel structure
and led to a smaller impregnation yield. Our results are
the complete opposite of those presented by other
authors (Betz, Hörmansperger, et al., 2012b; Betz,
Garcı́a-Gonzalez, et al., 2012a; Kleemann et al., 2020)
who prepared whey protein aerogels with much higher
swelling capacities. One explanation for this could be
gelation around the pI since WPI gels that were pro-
duced at a pH more distant from the pI exhibited lower
water absorption capability. Another reason could be
the hydrophobic character of heat-denatured proteins.
Since the low absorption rate and encapsulation effi-
ciency of whey protein aerogels was very low (only
reached ~0.4%), such results indicate that these sys-
tems are completely unsuitable for encapsulating this
type of extract. However, despite such low absorption
capacity and encapsulation efficiency values, the anti-
oxidant capacity remained high in all obtained systems
(Table 4). This could also be explained by the matrix
suitability for bioactive compound protection—even
with small entrapped extract quantities. Considering
the results obtained, the composition of WP aerogels
must be changed by adding different biopolymers or
changing the preparation conditions to obtain the
desired aerogel network.
Conclusions
Aerogels based on KG deacetylation and whey protein
thermal denaturation incorporated with sea buckthorn
pomace extract were obtained. It was found that absorp-
tion capacity and encapsulation efficiency of KG-based
aerogels was improved after lowering alkali concentra-
tion during deacetylation process. Such results were con-
firmed by the higher BET surface area and total pore
© 2022 Institute of Food Science and Technology

Table 4 Encapsulation efficiency of sea buckthorn pomace extract (15%, 20% and 25%) in whey protein aerogels and it antioxi-
dant activity during storage
Time, h
Amount of SBPE, % 24 48
Encapsulation efficiency, %
15 0.40
0.02ab
20 0.38
0.03b
25 0.39
0.02ab
Antioxidant capacity QT, µc
15 70.45
0.78a 89.00
1.28a
20 103.85
0.21b 125.20
0.99b
25 129.00
0.99c 162.19
9.06c
Values are means
SD. Means in the same column, followed by the different letters, indicate significant difference between the samples with dif-
ferent sea buckthorn pomace extract concentrations.
volume values. Meanwhile whey protein-based aerogels
obtained by supercritical CO2 drying had more compact
less porous structure and was able to absorb much lower
amount of extract (1.0–2.5%). It was also related with
such low encapsulation efficiency (0.5%) values.
Overall, these results demonstrated that sea buck-
thorn pomace extract could be not only successfully
immobilizated in the kognac-glucomannan structure
but also retained its antioxidant properties during the
storage as well. Thus, the KG aerogels show potential
for applications in the food industry as a carrier of bio-
active sea buckthorn pomace extract. Meanwhile, whey
proteins must be used in combination with other bio-
polymers to increase the porosity of these systems and
enhance the loading capacity of bioactive compounds.
Conflict of interest
We declare that we do not have any commercial or
associative interest that represents a conflict of interest
in connection with the work submitted.
Author contribution
Greta Svermickaite: Investigation (equal); Methodol-
ogy (equal). Viktorija Eisinaite: Formal analysis
(equal); Writing—original draft (equal). Rimante
Vinauskiene: Conceptualization (equal); Methodology
(equal). Ina Jasutiene: Validation (equal); Visualization
(equal). Daiva Leskauskaitë: Supervision (equal); Writ-
ing—review & editing (equal).
Ethical approval
Ethics approval was not required for this research.
Peer review
The peer review history for this article is available at
https://publons.com/publon/10.1111/ijfs.15777.
© 2022 Institute of Food Science and Technology
13652621, 2022, 7, Downloaded from https://ifst.onlinelibrary.wiley.com/doi/10.1111/ijfs.15777 by Kaunas University Of, Wiley Online Library on [16/03/2023]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Differently structured bioactive extract aerogels G. Švermickaitė et al. 4449
96 168 240
0.33
0.03a 0.20
0.02ab 0.15
0.00a 0.18
0.01b
0.33
0.04a 0.21
0.04b 0.20
0.00c 0.22
0.03b
0.36
0.05b 0.17
0.03ab 0.17
0.00b 0.04
0.01a
163.90
1.70a 181.00
0.57b 171.80
1.13c
172.69
2.11b 160.25
2.04a 127.00
3.96a
193.19
3.54c 207.65
3.47c 162.80
1.77b
Data availability statement
Data openly available in a public repository that issues
datasets with DOIs
References
Aditya, N.P., Espinosa, Y.G. & Ian, T. (2017). Norton Encapsula-
tion systems for the delivery of hydrophilic nutraceuticals: food
Application. Biotechnology Advances, 35, 450–457.
Aguiar, J., Estevinho, B.N. & Santos, L. (2016). Microencapsulation
of natural antioxidants for food application–the specific case of
coffee antioxidants–a review. Trends in Food Science & Technology,
58, 21–39.
In this publication there are a lot of information about the microen-
capsulation of natural antioxidants. By reading this publication we
perform the analysis and understand what systems are used to
encapsulate antioxidants.
Betz, M., Garcı́a-Gonzalez, C.A., Subrahmanyam, R.P., Smirnova, I.
& Koluzik, U. (2012). Preparation of novel whey protein-based
aerogels as drug carriers for life science. Journal of Supercritical
Fluids, 72, 111–119.
Betz, M., Hörmansperger, J., Fuchs, T. & Kulozik, U. (2012). Swell-
ing behaviour, charge and mesh size of thermal protein hydrogels
as influenced by pH during gelation. Soft Matter, 8, 2477.
Drozińska, E., Kanclerz, A. & Kurek, M.A. (2019). Microencapsula-
tion of sea buckthorn oil with β-glucan from barley as coating
material. International Journal of Biological Macromolecules, 131,
1014–1020.
Esquivel-Castro, T.A., Ibarra-Alonso, M.C., Oliva, J. & Martı́nez-
Luévanos, A. (2019). Porous aerogel and core/shell nanoparticles
for controlled drug delivery: a review. Materials Science and Engi-
neering C, 21, 915–940.
Fonseca, L.M., da Silva, F.T., Bruni, G.P., Borges, C.D., Zavareze,
E.R. & Guerra Dias, G.A. (2021). Aerogels based on corn starch
as carriers for pinhão coat extract (Araucaria angustifolia) rich in
phenolic compounds for active packaging. International Journal of
Biological Macromolecules, 169, 362–370.
Gómez, B., Barba, F.J., Domı́nguez, R. et al. (2018). Microencapsu-
lation of antioxidant compounds through innovative technologies
and its specific application in meat processing. Trends in Food Sci-
ence & Technology,
Ç 82, 135–147.
Ç
Grunovaite, L., Pukalskiene, M., Pukalskas, A. & Venskutonis, P.R.
(2016). Fractionation of black chokeberry pomace into functional
ingredients using high pressure extraction methods and evaluation
International Journal of Food Science and Technology 2022

4450 Differently structured bioactive extract aerogels G. Švermickaitė et al.
of their antioxidant capacity and chemical composition. Journal of
Functional Foods, 24, 85–86.
Herranz, B., Tovar, C.A., Solo-De-Zaldı́var, B. & Borderias, A.J.
(2012). Effect of alkalis on konjac glucomannan gels for use as
potential gelling agents in restructured seafood products. Food
Hydrocolloids, 27, 145–153.
This publication is very important as it contained information about
kognac hydrogels formation process. It also well described alkali
induced deacetylation process.
Kleemann, C., Schusater, 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.
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.
Li, J., Ye, T., Zhou, B. & Li, B. (2014). Facile preparation of clay
reinforced konjac glucomannan aerogels. RSC Advances, 4, 22251–
22254.
Liu, L., Wen, H., Rao, Z. et al. (2018). Preparation and characteriza-
tion of chitosan—collagen peptide/oxidized konjac glucomannan
hydrogel. International Journal of Biological Molecules, 108, 376–382.
Manea, A.M., Ungureanu, C. & Meghe, A. (2014). Effect of vegeta-
ble oils on obtaining lipid nanocarriers for sea buckthorn extract
encapsulation. Comptes Rendus Chimie, 17, 934–943.
Manzocco, L., Mikkonen, K.S. & Garcı́a-González, C.A. (2021).
Aerogels as porous structures for food applications: smart ingredi-
ents and novel packaging materials. Food Structure, 28, 100188.
Marin, M.A., Mallepally, R.R. & McHugh, M.A. (2014). Silk fibroin
aerogels for drug delivery applications. Journal of Supercritical
Fluids, 91, 84–89.
Mihalcea, L., Turturică, M., Ghinea, I.O. et al. (2017). Encapsula-
tion of carotenoids from sea buckthorn extracted by CO2 supercrit-
ical fluids method within whey proteins isolates matrices.
Innovative Food Science & Emerging Technologies, 42, 120–129.
Mihalcea, L., Turturică, M., Barbu, V. et al. (2018). Transglutami-
nase mediated microencapsulation of sea buckthorn supercritical
CO2 extract in whey protein isolate and valorization in highly
value added food products. Food Chemistry, 262, 30–38.
Mine, Y. (1995). Recent advances in the understanding of egg white
protein functionality. Trends in Food Science & Technology, 6, 225–
232.
Ni, X., Ke, F., Xiao, M. 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.
Niu, B., Shao, P., Luo, Y. & Sun, P. (2020). Recent advances of
electrosprayed particles as encapsulation systems of bioactives for
food application. Food Hydrocolloids, 99, 105376.
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
International Journal of Food Science and Technology 2022
13652621, 2022, 7, Downloaded from https://ifst.onlinelibrary.wiley.com/doi/10.1111/ijfs.15777 by Kaunas University Of, Wiley Online Library on [16/03/2023]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
aerogels as bioactive delivery vehicles produced through the valori-
zation of yerba-mate (Illex paraguariensis). Food Hydrocolloids,
107, 105931.
Selmer, I., Karnetzke, J., Leemann, C. et al. (2019). Encapsulation
of fish oil in protein aerogel micro-particles. Journal of Food Engi-
neering, 260, 1–11.
These two publications fully described the methods of aerogels prep-
aration. There are a lot of explanations about aerogel structure for-
mation and also encapsulation possibilities. Aerogels are also well
described and characterized.
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 Supercriti-
cal Fluids, 106, 42–49.
These two publications fully described the methods of aerogels prep-
aration. There are a lot of explanations about aerogel structure for-
mation and also encapsulation possibilities. Aerogels are also well
described and characterized.
Selvasekaran, P. & Chidambaram, R. (2021). 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.
Information provided in this publication helped to understand role
of the structure in the carrier of functional bioactive compounds. It
also contained information about the different biopolymers structure
formation mechanism (differences, similarities, advantages and
disadvantages).
Shah, A.H., Ahmed, D., Sabir, M., Arif, S., Khaliq, I. & Batool, F.
(2007). Biochemical and nutritional evaluations of sea buckthorn
(Hippophae rhamnoides L. spp. Turkestanica) from different loca-
tion of Pakistan. Pakistan Journal of Botany, 39, 2059–2065.
Shishir, M.R.I. & Chen, W. (2017). Trends of spray drying: a critical
review on drying of fruit and vegetable juices. Trends in Food Sci-
ence & Technology, 65, 49–67.
Wang, Y., Su, Y., Wang, W., Fang, Y., Riffat, S. & Jiang, F.
(2019). The advances of polysaccharide-based aerogels: preparation
and potential application. Carbohydrate Polymers, 226, 115242.
Wang, Y., Wu, K., Xiao, M., Riffat, S.B., Su, Y. & Jiang, F. (2018).
Thermal conductivity, structure and mechanical properties of kon-
jac glucomannan/starch based aerogel strengthened by wheat
straw. Carbohydrate Polymers, 197, 284–291.
Wu, K., Wu, H., Wang, R. et al. (2022). The use of cellulose fiber
from office waste paper to improve the thermal insulation-related
property of konjac glucomannan/starch aerogel. Industrial Crops &
Products, 177, 114424.
Zhang, X., Chen, F. & Wang, M. (2014). Antioxidant and antiglyca-
tion activity of selected dietary polyphenols in a cookie model.
International Journal of Agricultural and Food Chemistry, 62, 1643–
1648.
Zhou, Y., Jiang, R., Perkins, W.S. & Cheng, Y. (2018). Morphology
evolution and gelation mechanism of alkali induced konjac gluco-
mannan hydrogel. Food Chemistry, 269, 80–88.
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