International Journal of Biological Macromolecules 253 (2023) 126969

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International Journal of Biological Macromolecules

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

Microencapsulation of bioactive compound extracts using maltodextrin and

gum arabic by spray and freeze-drying techniques
Emanuele Joana Gbur Laureanti a, Thainnane Silva Paiva b, Luiz Mário de Matos Jorge a, b, c,
Regina Maria Matos Jorge a, b, *
a
Graduate Program in Chemical Engineering, Department of Chemical Engineering, Federal University of Paraná, Coronel Francisco Heráclito dos Santos Avenue,
Curitiba 81531-980, Brazil
b
Graduate Program in Food Engineering, Department of Chemical Engineering, Federal University of Paraná, Coronel Francisco Heráclito dos Santos Avenue, Curitiba
81531-980, Brazil
c
Chemical Engineering Department, State University of Maringá (UEM), Colombo Avenue, 5790, CEP, 87020-900, Maringá, PR, Brazil

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

Keywords: Microencapsulation techniques establish a protective barrier around a sensitive compound, reducing vulnera­
Pink pepper bility to external influences and offering controlled release. This work evaluates microencapsulation of Brazilian
Gum Arabic seed known as pink pepper (Schinus terebinthifolius) extract incorporated with green propolis extract, (main
Green propolis
propolis font from the South America native plant Baccharis dracunculifolia DC) to enhancement antioxidant
activity through synergic interaction, comparing to the extracts individually. Four treatments were produced
using maltodextrin and combined with gum arabic as encapsulating agent, employing two different microen­
capsulation technique applied (spray drying and freeze drying) to assess their impact on physicochemical
properties. The incorporation of gum arabic into matrix yielded higher encapsulation efficiency values, exhib­
iting significant differences for both encapsulation techniques. Combining the two encapsulation agents afforded
greater protection of the bioactive compounds, resulting in an increase of approximately 31 % in the inhibition of
the DPPH● radical. In controlled release analysis, maltodextrin exhibits the best protective effect on total
phenolic compounds during intestinal release, whereas combining maltodextrin and gum arabic enhanced
protection during gastric phase. Microcapsules may contribute to the protection of important bioactive com­
pound, possessing a wide range of applications such as flavors encapsulation in food industry, lipids, antioxidants
and pharmaceutical industry for controlled drug release.

1. Introduction phenolic compounds, anthocyanins, biflavonoids, hydrolyzable tannins

There has been a growing interest in the use of raw materials to
develop products that are rich in bioactive compounds for use as health
promoting agents in the food, pharmaceutical and cosmetics industries.
These products can be prepared and extracted from various vegetable
sources using a variety of methodologies that involve extraction by
means of solvents with different polarities [1,2].
Different bioactive attributes are linked to pink pepper (PP), such as
antioxidative, antitumor, and antimicrobial properties, often correlated
with its flavonoid, anthocyanin, and carotenoid content. Although few
researchers have analyzed the phenolic profile of PP, it is established
that the seed has important bioactive compounds, such as ascorbic acid,
and carotenoids [3,4]. As well as PP, green propolis (GP) is antioxidant,
anti-inflammatory, antibacterial, immunomodulatory and anti­
mutagenic [5]. Its characteristic chemical composition contains mainly
prenylated phenolic compounds, such as artepillin C, bacarin and dru­
panin, in addition to phenolic acids, such as its biosynthetic precursor p-
coumaric acid [6].
Although propolis contains many bioactive compounds, its applica­
tion is limited due to low oral bioavailability. When orally administered,
propolis is rapidly degraded in the body, especially in the gastrointes­
tinal tract. Moreover, the pronounced taste and aroma pose a barrier to
its direct application. As a result, there is a significant emphasis on
discovering innovative strategies capable of effectively utilizing the full

* Corresponding author at: Chemical Engineering Department, Federal University of Paraná (UFPR), Av. Coronel Francisco Heráclito dos Santos, s.n., CEP 81530-
900 Curitiba, PR, Brazil.
E-mail address: rjorge@ufpr.br (R.M.M. Jorge).

https://doi.org/10.1016/j.ijbiomac.2023.126969
Received 6 April 2023; Received in revised form 3 September 2023; Accepted 15 September 2023
Available online 18 September 2023
0141-8130/© 2023 Elsevier B.V. All rights reserved.
E.J.G. Laureanti et al.
potential of propolis. The combination of propolis and pink pepper ex­
tracts can lead to both anti-inflammatory and antioxidant activities
enhancement, indicating a synergic interaction when compared to the
extracts individually [1].
The industrial production of functional materials for foods involves
the incorporation of bioactive compounds that enhance color, flavor,
and texture, as well as the addition of health-promoting properties
(these include antioxidant, antimicrobial, antifungal, and anticarcino­
genic properties, among others) [7,8].
However, the phenolic compounds and anthocyanins found in
vegetable extracts tend to be unstable under various types of stress (high
temperatures, changes in pH, presence or absence of light and oxygen,
etc.), some of which occur naturally in the environment, and some of
which occur during processing. These factors limit the application of the
compounds in active products [7,9].
One strategy that has proven effective in solving this problem is the
technique known as microencapsulation [9]. Encapsulation refers to the
capture of an active compound within a polymeric matrix that protects it
from conditions in the environment and prevents interaction with other
components, or even controls its release, thus increasing the stability of
bioactive compounds and preserving their functional potential [7,10].
Among the various methods available for encapsulating bioactive are
spray-drying, freeze-drying, inclusion complexation, coacervation,
cocrystallization and emulsification [9]. Two of the most used micro­
encapsulation techniques are spray-drying and freeze-drying. Spray-
drying is a low-cost and flexible industrial method that is commonly
used to transform liquid products into dry powders. When used for
microencapsulation purposes, the bioactive compounds are covered by
the carrier material, which protects them from stresses in the environ­
ment. Freeze-drying is particularly useful for drying compounds that are
sensitive to heat, since in this method the food substance is exposed to
freezing temperatures at a very low pressure, resulting in the formation
of ice crystals that subsequently undergo sublimation [9,11,12].
The final properties of the microencapsulated materials, such as ef­
ficiency and microcapsule size, depend on the type and characterization
of the coating agent used for encapsulation. Maltodextrin is the most
commonly wall material used in microencapsulation technique due the
low cost and its encapsulation efficiency of hydrophilic core materials,
such as antocyanidins and gallic acid. In contrast, for hydrophobic
compounds (catechins, curcumin and resveratrol), wall materials as
proteins and hydrophilic gums leads to larger stability as carbohydrates,
which has high porosity and low emulsifying capacity. In order to
enhance the encapsulation efficiency, recent researches have been using
the wall materials combination to achieve functional properties that the
carbohydrates do not have when used alone [9,11,13].
Numerous applications could be cited from recent studies involving
microencapsulation of fruit and plant extracts from different botanical
sources: functional foods and natural antioxidants [9,14–17], controlled
release in the digestive tract [18–20], microencapsulation of vitamins
[21,22], cosmetic ingredients [23], and biodegradable films [24–26].
However, no studies have been published involving the microen­
capsulation of pink pepper extract (PPE) in conjunction with green
propolis extract (GPE), and no analysis exists of the advantages of
combining the two extracts with regard to antioxidant properties, an
essential aspect of industrial application. The goal of the current study
was to evaluate the use of maltodextrin (MD) as an encapsulation agent,
both alone and in combination with gum arabic (GA) and determine the
impact of the inherent mixture value from bioactive extracts of the
Atlantic Forest on properties such as solubility, hygroscopicity, water
activity, Fourier-transform infrared spectroscopy, morphology, thermal
properties and release of phenolic content in environments that simulate
gastrointestinal pH. The association of both bioactive compounds allows
for the creation of a functional ingredient that could be applied in
different areas, such as food industry to encapsulation of flavors, lipids,
antioxidants, as weel as for controlled drug release and pharmaceutical
industry.
2
International Journal of Biological Macromolecules 253 (2023) 126969
2. Materials and methods
2.1. Materials
Pink pepper fruits (Shinus terebinthifolius Raddi) were harvested from
trees in the city of São José dos Pinhais (Brazil), 2022 harvest. They were
then dried at 40 ◦ C for 24 h in an oven with air circulation (Nova Ética,
400/6ND) and conditioned in a freezer at − 20 ◦ C in absence of light,
according to the methodology adopted by the authors [27]. The green
propolis from the Apis melífera bee was collected in the city of Muzam­
binho, Minas Gerais – MG, 2021 harvest.
2.2. Preparation of the extracts
The pink pepper extract was prepared according to the process
described by Laureanti et al. [28]. Samples containing 5 g of pink pepper
were extracted using a 10 mL ethanol:water solution (80:20 v/v) and
kept in a warm bath (Lucadema, 155/10) at 90 ◦ C for 20 min, after
which they were placed in an ultrasonic bath (Odontobrás, 1440 DA) for
15 min. The hydroalcoholic solution was filtered under vacuum using
qualitative filter paper (Prismatec, 131); finally, the mixture was
concentrated in a rotary vacuum evaporator (Fisatom) at 65 ◦ C until the
ethanol had completely evaporated. The supernatant, hereafter referred
to as pink pepper extract (PPE), was stored in an amber container and
conditioned in absence of light in a freezer at − 20 ◦ C.
The green propolis was extracted using a slightly modified form of
the methodology described by Dalponte et al. [29]. The propolis was
ground using a manual coffee grinder (Botini), and a 70 % ethanol so­
lution (v/v; 1:25 m/v) was added to the resulting dry material. The
mixture was kept in absence of light under magnetic agitation (Fisatom,
752 A) for 48 h, after which it was submitted to ultrasound (1440 DA
Biodont) for 1 h at a frequency of 40 kHz. The extract solution was
filtered using a Buchner funnel with a glass microfiber filter, coupled to a
Kitasato flask under vacuum. The green propolis extract (GPE) was
stored in an amber flask and conditioned in absence of light in a freezer
− 20 ◦ C.
2.3. Production of microcapsules
The encapsulation of the PPE with the GPE was carried out using MD
and a combination of MD and GA (1:1 w/w) as encapsulation agents,
according to a modified form of the methodology proposed by Sarabandi
et al. [9]. Both agents were added directly into a mixture of pink pepper
and green propolis extracts at a fixed concentration of 20 % w/v, in a
proportion of 1:1 v/v. The solution was kept under magnetic agitation
(Fisatom, 752 A) for 30 min and then stored at ambient temperature for
12 h. The two drying techniques employed were spray drying and freeze-
drying. The microcapsules produced were labeled as follows: IA – PPE
and GPE produced with MD as an encapsulation agent using the freeze-
drying technique; IIA – PPE and GPE produced with MD as an encap­
sulation agent using the spray-drying technique; IB – PPE e GPE mi­
crocapsules produced with MD and GA as an encapsulation agent using
the freeze-drying technique; IB – PPE e GPE produced with MD and GA
as an encapsulation agent using the freeze-drying technique.
2.3.1. Spray-drying
The drying process was carried out in a spray-dryer (Industrie Werke
Karlsruhe, LZT C280A), into which the solution was fed using a peri­
staltic pump with a flow of 33.39 L/h and a pressure of 1 bar. The
following controlled parameters were selected based on preliminary
tests: inlet temperature (180 ± 5 ◦ C); outlet temperature (90 ± 5 ◦ C);
atomizer rotational speed 18,000 rpm. The microcapsules thus produced
were transferred to a desiccator in order to achieve constant tempera­
ture and avoid moisture changes, after which they were stored in an
opaque flask for further analysis.
E.J.G. Laureanti et al. International Journal of Biological Macromolecules 253 (2023) 126969

2.3.2. Freeze-drying 100 mL of distilled water and stirred at 400 rpm (Go Stirrer MS-H-S10)
Using the same technique that was used for spray-drying, solutions for 30 min. The solution was centrifuged at 3000 ×g for 5 min and an
were prepared having the same concentrations of encapsulation agents aliquot (25 mL) was transferred to a Petri dish, after which it was dried
dissolved in the extracts. For the freeze-drying process, the dispersions in an oven (Marconi MA035/2) at 105 ◦ C for 5 h. Solubility was deter­
were frozen in a freezer at − 18 ◦ C for 48 h. The samples were placed in a mined as the percentage of the weight of the dried solution as compared
freeze dryer (Christ Alpha 1LD Plus) and dried for 48 h at − 58.8 ◦ C, at a to the weight of sample originally added (1.0 g).
pressure of 6.11 mbar, vacuum of 0.42 mbar. After freeze-drying, the
samples were ground using a mortar and pestle [30]. 2.5.4. Hygroscopicity and water activity
The hygroscopicity was performed using the methodology described
by Rezende, Nogueira e Narain [30]. One gram of microcapsules was
2.4. Drying yield
placed in a desiccator containing a saturated sodium chloride solution
(75.3 % NaCl) at 25 ◦ C. After 1 week the samples were weighed and their
The drying yield for both spray-drying and freeze-drying was eval­
hygroscopicity expressed as a percentage (%) of adsorbed moisture.
uated based on the percentage between the total mass of the product
Water activity was determined in triplicate using a Decagon, Aqualab
recovered upon its exit from the equipment and the mass of the extract
Lite (BrasEq-Séries, 3B) [35].
fed into the system, according to Eq. (1) (dry basis):
Mass of microcapsules (g) 2.5.5. Colorimetric analysis
Y (%) = × 100 (1)
Total mass of the extract fed into the system (g) The color of the microcapsules was measured according to the CIE
L*a*b* color parameters using a colorimeter (HunterLab, MiniScan EZ
4500 L). L* indicates brightness, ranging from 0 (black) to 100 (white),
2.5. Characterization of the microcapsules
a* is the variation from green (− ) to red (+) and b* is the variation from
blue (− ) to yellow (+). The variation in color difference compared to a
2.5.1. Total phenolic content and phenolic compound encapsulation
white standard was calculated in triplicate using Eq. (3):
efficiency
√̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅
Total phenolic content (TPC) was determined by releasing the
ΔE = (ΔL* )2 + (Δa* )2 + (Δb* )2 (3)
phenolic compounds from the microcapsules by completely destroying
the coating material, according to a modified form of the methodology
where: ΔE = color difference; ΔL* = L*standard – L*sample; Δa* =
described by Tolun, Altintas and Artik [31]. A total of 15 mg of micro­
a*standard – a*sample; and Δb* = b*standard – b*sample. Standard
capsules were weighed and added to 3 mL of an ethanol, acetic acid and
values were obtained on a white plate: L = 93.41, a = − 1.35 and b =
water solution (50:8:42, v/v). The solution was then agitated for 1 min
+0.83.
using a vortex mixer (Scientific Industries, G-560), after which it was
placed in an ultrasound (MaxiClean1650A, Indaiatuba, SP, Brasil) for
2.5.6. Fourier transform infrared spectroscopy (FTIR)
20 min and vacuum filtered using qualitative filter paper (0.45 μm,
The microcapsules were prepared by grinding with potassium bro­
Millipore filter).
mide (KBr) (1 % m/m) and analyzed in a spectrometer (Bruker, vertex
An analysis was conducted in triplicate using a slightly modified
70) using Fourier transform infrared spectroscopy. Transmittance
form of the Folin-Ciocalteu [32] method. In a 10 mL volumetric flask, 5
spectra were determined in the frequency range of 4000–400 cm− 1 with
mL distilled water, 500 μL Folin Ciocalteu reagent (2 N) and 200 μL of
a resolution of 4 cm− 1 [36].
the extracts being evaluated were added. The solutions were agitated for
1 min using a vortex mixer (Scientific Industries, G-560), after which 2
2.5.7. Thermogravimetric analysis
mL Na2CO3 solution at 15 % and 5 mL distilled water were added and
The thermogravimetric curves (TGA) were obtained in a thermal
agitated again with the vortex mixer for 30 s. The flasks were kept in
analyzer (PerkinElmer, TGA 4000) according to the methodology
absence of light for 120 min. Absorbance was measured at 760 nm, and a
described by De Araújo et al. [37]. The analysis was performed under an
standard curve was used to calculate the results expressed in mg of gallic
inert atmosphere of nitrogen (50 mL/min) and the samples were heated
acid equivalent (GAE) per g of dry sample.
from 30 to 600 ◦ C at a constant rate of 10 ◦ C/min.
The encapsulation efficiency was determined using to a slightly
modified form of the methodology described by Mousavi Kalajahi and
2.5.8. Surface morphology analysis
Ghandiha [33]. The superficial phenolic content was determined by
The microparticle morphology was obtained using scanning electron
extraction from 20 mg of microcapsules in 1 mL of water:ethanol
microscopy (SEM) (JEOL, JSM 6360-LV) [38]. The microcapsule sam­
mixture (1:1 v/v). The solution was agitated in a vortex mixer for 10s,
ples were fixed on stubs using double-sided adhesive carbon tape,
after which it was centrifuged for 10 min at 600 xg. The supernatant was
metallized with a thin layer of gold (Balzers Union, FL 9496) and the
allocated in flasks and enlarged by 10 mL with 40 % ethanol.
images were captured using an acceleration of 20 kV.
The phenolic compound quantities were quantified as described
previously using the Folin-Ciocalteu method as described by Singleton
2.5.9. Determination of antioxidant activity using DPPH● and ABTS●+
and Rossi [32]. The tests were performed in triplicate, and the bioactive
radicals
compound encapsulation efficiency was determined using Eq. (2).
As in the procedure for determining total phenolic compounds, the
Superficial phenolic content of microcapsules antioxidant compounds present in the microcapsules must be released in
EE% = 1 − × 100 (2)
Total phenolic content of microcapsules order to determine antioxidant activity on the DPPH● and ABTS●+
radicals. The procedure used for this purpose was the same as that
2.5.2. Moisture content described above.
The moisture content of the powder was determined gravimetrically Antioxidant activity was determined by the sequestration of the
at 105 ◦ C until a stable weight was reached, according AOAC (2012) DPPH● radical (1.1-difenil-2-picrilhidrazil), according to a modified
[34], n◦ 943.06 (section 37.1.10B). form of the process described by Brand-Williams et al. [39]. First,
0.00472 g of DPPH● was weighed and dissolved in a flask containing
2.5.3. Solubility 200 mL of PA methanol and kept in absence of light, after which 100 μL
The solubility was evaluated according to the method proposed by of the sample extract and 3.9 mL of the DPPH● (0.06 mM) methanol
Rezende, Nogueira e Narain [30]. One gram of powder was added to solution was placed in opaque tubes using a pipette. They were then

3
E.J.G. Laureanti et al.
mixed, and the absorbance of the reaction mixture was measured at 515
nm after 30 min at ambient temperature in absence of light using a
UV–visible spectrophotometer (Shimadzu, UV-1800).
The ABTS●+ radical (2.2′-azino-bis) test was conducted using a
modified form of the methodology described by Re et al. [40]. The
ABTS●+ saline solution (7 mM) was prepared by diluting 0.0392 g of
ABTS in 10 mL sodium acetate buffer (20 mmol/L; pH 4.5), after which
0.37845 g of potassium persulfate was weighed and dissolved in 10 mL
sodium acetate buffer (20 mmol/L; pH 4.5). Subsequently, 176 μL of
potassium persulfate were mixed into the 10 mL of ABTS●+ solution and
kept at ambient temperature in absence of light for 16 h (for the com­
plete generation of the radical).
Finally, the absorbance of the ABTS●+ was adjusted using the so­
dium acetate buffer (80 mM), after which 3 mL of ABTS●+ reagent was
added to 30 μL of the sample. The mixture was kept in absence of light
for 30 min and absorbance was measured at 734 nm. The radical inhi­
bition percentage was calculated using Eq. (4):
(Ab − Am )
%Radical Scavenging Activity = 100 × (4)
Ab
where Ab is the absorbance of the white, and Am is the absorbance of the
microcapsule.
2.5.10. Analysis of the release of total phenolic content
For the analysis of the release of total phenolic compounds and
monomeric anthocyanins from the spheres, the system was exposed to
simulated gastrointestinal pH conditions, according to the methodology
described by Dalponte Dallabona et al. [29]. First, 5 g of microcapsules
were weighed and submerged in glass beakers containing 10 mL of
hydrochloric acid 0.1 N (pH 1.2, similar to gastric conditions) and a
potassium chloride buffer (pH 7.2, similar to the small intestine). The
samples were then incubated in a shaker at 37 ◦ C for 240 min and slightly
agitated 100 rpm. The supernatant solution was analyzed at specific
intervals (0, 10, 20, 30, 60, 120 and 240 min) using the pH differential
Folin Ciocalteau methods. Total phenolic content of the samples was
determined and the release from the microcapsules was calculated as a
percentage.
2.5.11. Statistical analysis
A statistical analysis of the results was conducted using ANOVA p ≤
0.05, and the statistically different means were then analyzed using a
Tukey test for post hoc analysis, with the aid of Statistica® 10.0 statis­
tical software (Statsoft, Inc).
3. Results and discussion
3.1. Total phenolic compound and efficiency of microencapsulation of
phenolic compounds
The analyses used to evaluate antioxidant capacity and determine
total phenolic content are an essential aspect of the pharmaceutical,
cosmetics and food industries used to ensure the quality of functional
foods, though their main purpose is to study the efficiency of antioxi­
dants in the prevention and treatment of diseases associated with
oxidative stress and evaluate the protection provided against oxidation
and deterioration (reactions that may lead to a significant loss in the
quality of the product and in its nutritional value) [41,42]. The results of
the total phenolic compound analysis of the four different samples are
shown in Table 1, expressed in mg GAE/g.
The total phenolic compounds of pink pepper and green propolis
extracts results in an approximate 35 % increase in total phenolic con­
tent compared to pink pepper extract alone, and a 12 % increase
compared to green propolis extract alone. This phenomenon indicates
synergistic interaction of the constituents possibly leads to the potenti­
ation of total phenolic content, as evidenced by the results of the Tukey
4
International Journal of Biological Macromolecules 253 (2023) 126969
Table 1
Results of total phenolic compounds present in the PPE:GPE microcapsules.
Treatment Total phenolic compounds (mg GAE/g)
IA 18.25 ± 0.52e
IIA 24.39 ± 0.35d
IB 19.93 ± 0.46e
IIB 25.15 ± 0.43d
PPE 27.19 ± 0.45c
GPE 32.88 ± 0.77b
PPE:GPE 36.83 ± 0.32ª
NOTE: Different lowercase letters in the same column indicate a significant
difference among the samples.
PPE – pink pepper extract; GPE – green propolis extract; PPE:GPR – pink
pepper and green propolis extract combined.
test (Tukey test, p ≤ 0.05) [29]. Regarding the microcapsules, a reduc­
tion in total phenolic content is observed, possibly due to the conditions
of the microencapsulation techniques, which might not entirely retain
the phenolics within the microcapsules, potentially causing losses.
The microcapsules exhibited total phenolic compound concentra­
tions that ranged from 18.25 ± 0.52 to 25.15 ± 0.43, with a significant
difference (Tukey test, p ≤ 0.05), according to the drying technique
used. From these data it may be concluded that the microcapsules pro­
duced by spray-drying exhibited a greater amount of released phenolic
compounds; that is, this technique better encapsulated and protected the
bioactive compounds. However, in this case, the use of different
encapsulation agents was irrelevant.
Andrade et al. [43] produced and characterized microcapsules made
using spray-drying that contained brown, green and red Brazilian
propolis extract, with MD and GA as an encapsulating agent. These
authors reported values ranging from 23.36 ± 0.02 to 48.38 ± 0.38 mg
GAE/g per microcapsule. The greatest total phenolic compound value
was obtained for microcapsules produced with GA, suggesting that the
gum exhibits the best characteristics for the preservation of the bioactive
compounds during spray-drying as compared to other agents. This result
corroborates those observed in the present study, in which the addition
of GA to the formulation increased phenolic compound concentration,
indicating enhanced protection of bioactive compounds when GA is
combined with MD.
The efficiency of phenolic compound microencapsulation is an
extremely important factor for evaluating the success of the encapsu­
lation. This analysis makes it possible to evaluate the quality of the
protection given the phenolic compounds present in the extracts ac­
cording to the drying and encapsulation methods used (spray-drying vs.
freeze-drying; MD vs. MD and GA combination) [44]. Values between
89.45 ± 0.01 % and 98.33 ± 0.45 % were obtained (Fig. 1). The Tukey
test revealed significant differences for all samples (p ≤ 0.05).
The gradual loss of bioactive compounds during the drying processes
is a result of numerous factors, such as the nature of the encapsulation
material and the drying technique used. In the spray-drying process,
fissures may form on the surface of the microcapsules due to the rapid
evaporation of water (this occurs due to the high temperature of the
process). In the freeze-drying process, pores may form in the micro­
capsules due to the sublimation of the water during the process, leading
to the premature release of the encapsulated component and possible
degradation [30]. The GA and MD mixture exhibited greater encapsu­
lation efficiency values for both the freeze-drying (in which efficiency
increased from 93.28 ± 0.35 % to 98.33 ± 0.45 %) and the spray-drying
(89.45 ± 0.005 % to 91.07 ± 0.12 %) processes.
Similar results were obtained by Saikia, Mahnot and Mahanta [45]
who used microencapsulation to encapsulate phenolic extract from
Averrhoa carambola bagasse with MD using the spray-drying and freeze-
drying methods. The authors obtained phenolic compound microen­
capsulation efficiency values of 78–97 % for freeze-drying and 63–79 %
for spray-drying, accounting for the lower values obtained using the
spray-drying method by the susceptibility of some phenolic acids that
E.J.G. Laureanti et al. International Journal of Biological Macromolecules 253 (2023) 126969

Fig. 1. Efficiency of microencapsulation of phenolic compounds in the microcapsules.

are destroyed during the application of heat during the drying process. techniques are greater than those reported for the encapsulation of
opuntia fig (Opuntia fícus indica), using spray-drying and freeze-drying
[47]. Using opuntia fig starch as the encapsulation agent, the authors
3.2. Drying yield, moisture content, solubility, hygroscopicity and water reported results that varied between 42.2 ± 0.5 % - 64.5 ± 1.6 % for the
activity spray-drying method, and 44.3 ± 0.8 % – 56.0 ± 1.9 % for the freeze-
drying method.
The encapsulation yield corresponds to the percentage between the Properties such as moisture content and water activity in the
total mass of the collected microcapsules and the mass of the solids in microcapsule samples directly affect the stability and storage properties
the extract fed into the system. The microencapsulation yield values for of the powder. When the microcapsules transition from a vitreous state
the spray-drying technique (Table 2) were lower than those for the to an amorphous state at higher moisture levels, the material stored in
freeze-drying technique, a significant difference being observed be­ the nucleus is released and degraded [48].
tween the samples (Tukey test, p ≤ 0.05). This behavior may be The microcapsules produced in the present study exhibited a mois­
explained by the high viscosity of the feeding solution, which causes ture content that varied between 2.52 ± 0.11 % and 6.07 ± 0.15 %
more solids to stick to the wall of the drying chamber [46]. When GA (Table 2). The Tukey test revealed that the four treatments exhibited
was added, no significant differences were observed among the samples significant differences among themselves (p ≤ 0.05), possibly due to the
for microencapsulation yield. different proportions of wall material and the drying technique used.
Karrar et al. [44] reported a microencapsulation yield between 85.25 It was observed that the treatments that used only MD (IA e IIA)
and 92.80 % using the spray drying technique. The results showed that exhibited lower humidity contents as compared to the formulations that
the formulation with an encapsulating agent based on MD and GA included GA (IB e IIB). This behavior may be related to differences be­
achieved the highest yield (92.80 %). Furthermore, there were no sig­ tween the chemical structures of GA and MD; for example, GA has a
nificant differences (p ≤ 0.05) observed between the formulation based larger number of hydrophilic groups, allowing it to bond easily with
on MD and GA and the formulation based on whey protein isolate, GA water molecules and therefore increase the moisture of the particles
and MD. This behavior could be attribuited to the presence of GA in [49]. The samples dried using the spray-drying technique (IIA e IIB)
these formulations, which has a high film-forming capacity. exhibited an increase in moisture when GA was added, resulting in a
In general, the yield values obtained for both encapsulation more viscous emulsion and therefore retarding the diffusion of the water
molecules [49].
Table 2 From the evaluation of the variations in moisture content of the
Drying yield, moisture content, solubility, hygroscopicity and water activity of samples with regard to the technique used, the authors concluded that
the microcapsules produced. the microcapsules produced by spray-drying exhibited smaller content
Treatment Drying Moisture Solubility Hygroscopicity Water values as compared to those produced by freeze-drying (IIA, IIB < IA,
yield content (%) (%) activity IB). This difference may be related to the fact that spray-drying is con­
(%) (%) ducted at higher temperatures, thus increasing the heat transfer rate
IA 80.99 4.32 ± 81.35 ± 15.56 ± 0.23ª 0.21 ± within the particle and leading to a faster evaporation of the water,
± 0.32a 0.05b 1.13ª 0.01ª resulting in a lower moisture content in the product [31].
IB 81.33 6.07 ± 82.59 ± 10.93 ± 0.49b 0.22 ±
Hygroscopicity, which is related to the capacity of the microcapsules
± 0.25a 0.15a 0.32ª 0.01ª
IIA 73.84 2.52 ± 82.23 ± 16.43 ± 0.34ª 0.22 ± to absorb humidity present in the environment, also affects physical-
± 0.44b 0.11d 1.35ª 0.01ª chemical stability and shelf-life of the product, as well as other param­
IIB 74.27 3.30 ± 81.61 ± 11.69 ± 0.28b 0.20 ± eters, such as the fluidity of the powders [14,50]. According to Table 2,
± 0.16b 0.09c 0.75ª 0.01ª the use of the GA and MD combination as wall material significantly
NOTE: Different lowercase letters in the same column indicate a significant affected the hygroscopicity of the microcapsules (the various treatments
difference among the samples.

5
E.J.G. Laureanti et al.
exhibited significant differences among themselves, p ≤ 0.05). However,
it was also observed that the use of different techniques used did not
affect the hygroscopicity of the samples.
Hygroscopicity is affected by inherent composition, the type and
concentration of the encapsulation agent used, and microcapsule size
[51]. It was observed that the increase in hygroscopicity values was
inversely proportional to the moisture content, so that lower moisture
contents indicated higher hygroscopicity. According to Akhavan Mah­
davi et al. [52], this behavior is related to the greater water concen­
tration gradient between the product and the air. In other words, the
microcapsules exhibited a higher hygroscopicity due to their smaller
humidity content.
Sarabandi et al. [9] reported similar results for the encapsulation of
natural eggplant extract using various encapsulation agents. The authors
observed a smaller value for microcapsules produced with MD and GA as
compared to those produced with only MD, an observation that they
attributed to the fact that GA has a greater glass transition temperature
than MD. Moreover, the increase in drying temperature, from 140 to
170 ◦ C, resulted in an increase in the hygroscopicity of the powders,
which was possible due to the increase in the difference between the
moisture of the compounds and that of the environment.
Solubility is an important characteristic for analysis due to its impact
on possible applications of the microcapsules, since the release of the
encapsulated compounds is largely dependent upon the dissolution of
the encapsulation agent. A desirable factor in the food industry is that
the microcapsules exhibit good solubility, allowing them to be used as
ingredients [25,53]. However, in the pharmaceutical industry, low sol­
ubility limits the incorporation of the microcapsules in certain vehicles,
resulting in an ineffective topical therapy [54].
The solubility of the microcapsules varied between 81.35 ± 1.13 %
and 82.59 ± 0.32 %. The samples did not exhibit significant differences
as determined by the Tukey test (p ≤ 0.05); therefore, they were not
affected either by the type of technique used (spray-drying or freeze-
drying) or by the by the formulation of the encapsulation agent.
Recent studies conducted in order to evaluate the effect of GA and MD
on the solubility products dried using spray-drying and freeze-drying
showed different results [48,55–57].
In contrast, Fernandes, Borges and Botrel [53] obtained relatively
soluble particles despite the hydrophobic nature of the core material,
with results ranging from 41.85 % to 47.72 % (values about 45 % lower
than the present study), showing no significant difference for the
different types of encapsulants used (GA, MD, inulin and starch). The
authors related the low solubility to rosemary essential oil (encapsulated
material) which at room temperature is not soluble in pure water
Remarkably, the encapsulation of the essential oil resulted in better
solubility when compared to the pure oil.
Water activity (aw) corresponds to the equilibrium moisture of a
material; in other words, it is the point at which there is no gain or loss of
water to the environment. Water activity refers to the water available for
interaction with aspects in the environment such as microorganisms.
Greater water activity results in better development and growth of mi­
croorganisms such as fungi, yeasts and bacteria [58].
The results of the water activity analyses conducted on the micro­
capsules varied between 0.20 ± 0.01 and 0.22 ± 0.01, values considered
typical for industrial products dried using freeze-drying and spray-
drying. As in the case of solubility, water activity was not affected
either by the technique used or by the formulation of the encapsulation
agent (Tukey p ≤ 0.05).
Rezende, Nogueira and Narain [30] used spray-drying and freeze-
drying to produce microcapsules with extracts of bioactive compounds
obtained from the pulp and waste products of acerola (Malpighia emar­
ginata DC). These microcapsules exhibited moisture values between 3.12
and 7.05 %. As in the present study, the authors observed greater con­
tent values for the treatment containing MD and GA using the freeze-
drying technique.
Sarabandi et al. [9] developed microcapsules using GA and MD to
6
International Journal of Biological Macromolecules 253 (2023) 126969
encapsulate eggplant peel extract as an antioxidant and natural dye.
Moisture contents ranged from 2.34 ± 0.22–4.11 ± 0.28 %, with the
highest values for microcapsules produced with GA, as found in this
study. This result was related to the greater ability of gums to maintain
particle moisture when compared to starch derivatives. The authors also
revealed that the humidity was significantly influenced by the spray
dryer inlet temperature, decreasing the moisture contents of the mi­
crocapsules with the increase in temperature.
However, for the water activity analysis, Rezende, Nogueira and
Narain [30] used the mixture of GA and MD in equal proportions and
obtained very close results to this research, ranging from 0.10 to 0.27
with a significant difference between the samples in the Tukey test (p ≤
0. 05).
3.3. Colorimetric analysis
The optical properties of the microcapsules, such as color parameters
(L*, a* and b*) and color variation (ΔE) are relevant for the application
of the microcapsules due to their direct impact on the presentation of the
products to be applied. They are related to color, brightness and trans­
parency. The results of the optical properties of the microcapsules are
shown in Table 3.
The a* and b* values show that all the data appeared in the first
quadrant (+a*, +b*), indicating a tendency toward red (positive a*
values varying between 0.18 ± 0.03 and 2.20 ± 0.05) and yellow
(positive b* values varying between 9.50 ± 0.27 and 18.97 ± 0.71). An
increase in the L* value occurred in conjunction with the technique
used, and the samples exhibited a significant difference according to the
Tukey test (p ≤ 0.05). The decreased luminosity exhibited by the freeze-
dried product may be related to the freezing of the samples, which re­
sults in the formation of ice crystals and alters the pore structure after
the sublimation of the water. Thus, the surface of these particles is
darker, due to the light dispersion properties of the empty spaces left
after sublimation [59]. The addition of GA as wall material did not result
in any significant difference between the samples (Tukey test, p ≤ 0.05).
The microcapsules produced using the freeze-drying technique
exhibited a lower L* value and higher a* and b* values (more intense red
and yellow), whereas those produced using spray-drying exhibited a
higher L* value and lower a* and b* values. This behavior may be
related to the lower drying capacity of freeze-drying for encapsulation of
pigments, or to the difference in thickness of the materials in the
microcapsule walls [38]. A similar result was reported by Kuck and
Noreña [59] for the aqueous extract of grape skins (Vitis labrusca var.
Bordo) encapsulated using spray-drying, which exhibited a more intense
red coloring than that of the freeze-dried product.
3.4. Fourier transform infrared spectroscopy (FTIR)
Fourier-transform infrared spectroscopy (FTIR) is a non-destructive
technique that allows data to be gathered quickly and with minimal
preparation and volume requirements from limited samples, charac­
teristics that allow it to be used for a wide variety of applications [60].
The FTIR spectrum may also be used as a powerful tool for the structural
analysis of active molecules and their polymers due to its capability of
showing the molecular structure and chemical bonds characteristic of
each substance [61].
FTIR spectroscopy was used to evaluate the effectiveness of the
Table 3
Optical properties of the PPE:GPE microcapsules.
Treatment L* a* b* ΔE
IA 76.40 ± 0.87b 2.20 ± 0.05a 17.44 ± 0.18b 24.04 ± 0.70b
IIA 87.34 ± 0.87a 0.65 ± 0.07b 9.50 ± 0.27c 10.79 ± 0.54c
IB 74.09 ± 1.21b 1.87 ± 0.23a 18.97 ± 0.71a 26.70 ± 1.21a
IIB 86.03 ± 0.81a 0.18 ± 0.03c 10.54 ± 0.17c 12.30 ± 0.51c
E.J.G. Laureanti et al.
loading of the PPE:GPE extracts in the microcapsules and to investigate
the functional groups of the microcapsules produced. The spectra of the
samples are shown in Fig. 2.
Overall, the spectra of microcapsules exhibited peak positioning
(wavenumber) very similar as other works reported in literature, which
used MD and combination of MD and GA as carrier materials [62,63].
The bands of the IA and IIA samples (those produced using only MD
as the encapsulation agent, by freeze-drying and spray-drying, respec­
tively), exhibited characteristics commonly observed in the absorption
bands of microcapsules made from MD. The absorption appeared with
very strong and broad intensity of band at around 3375 cm− 1 indicate
vibrations from the stretching of O–H hydroxyl groups [44,63,64],
suggesting that they are related to the bonding of intermolecular
hydrogen between the wall materials and the antioxidant compounds.
This behavior may be said to be expected, due to the number of OH
groups in the materials and in the antioxidants. The peak is also related
to the presence of carboxylic acids and residual water [9].
The peaks with different intensities found between 2921 and 2927.3
cm− 1 were attributed to vibration from the stretching of the C–H bond
of alkenes present in the samples. The remaining absorption bands
characteristic of MD may be seen in Fig. 2 at the ranges 1639.3–1650.7
cm− 1, 1384.3–1390 cm− 1 and 1024.4–1047.1 cm− 1, which correspond
to the vibration from the asymmetrical stretching of the -C=O, the
folding of the OH, and finally, the stretching of the C–O and folding of
the C-O-H, respectively [44,63,64]. The bands below 1000 cm− 1 were
associated with the vibration of the pyran ring [49].
The spectra observed for the samples IB and IIB (those using MD and
GA as encapsulation agents and dried by freeze-drying and spray-drying,
respectively), also exhibited characteristics commonly observed in ab­
sorption bands of microcapsules made from MD, with a few differences,
possibly due to the addition of GA in the matrix (Fig. 2).
The first band, present in the spectrum between 3375 and 3382.1
cm− 1 corresponds to the stretching of the O–H hydroxyl group, as
indicated also in IA and IIA microcapsules. However, it may be seen that
this peak shown reduction in intensity when GA was added in the mi­
crocapsules matrix. This behavior can indicate the breakage of the
hydrogen bonds in the maltodextrin molecules, forming new bonds with
GA molecules, participating in chemical reactions during the dryer such
Fig. 2. FTIR spectra of the PPE:GPE microcapsules produced by the spray-drying and freeze-drying techniques, using MD and GA as wall material.
7
International Journal of Biological Macromolecules 253 (2023) 126969
as hydrogen bonding and/or esterification between MD and GA [49].
The spectra found at 2920.2–2930.1 cm− 1, 1608.2–1618.1 cm− 1,
1401.3–1409.8 cm− 1 and 1025.8–1027.2 cm− 1 correspond to the
stretching of C–H, the stretching of C–
– O as well as the folding of N–H,
the folding of C–H and CH3 and the stretching of C–H [9,63,64]. In
regions between 900 cm− 1 to 1600 cm− 1, as well, numerous peaks
corresponding to phenolic compounds were identified. Some peaks
disappeared in spray-dried samples (IA and IIA), suggesting that the
carrier offered protection to the antioxidants during the microencap­
sulation process. [9]
The bands found between 575.3 and 578.1 cm− 1 may be related to
the variations in the vibrations from O–H deformation [63]. The sim­
ilarity of the bands observed for the microcapsules to those associated
with the pure material [49,65–69] indicates that the MD and GA pre­
served their chemical structures after the drying processes, thus
revealing their effectiveness for protecting the antioxidant compounds
present in the nucleus of the microcapsules.
3.5. Thermogravimetric analysis
The TGA and DTG curves provided information related to the ther­
mal stability and composition of the material, aiding the understanding
of maximum weight loss or weight gain of the analyzed material based
on temperature [63]. The TGA thermograms and their differential
curves (DTG), corresponding to the intensity of the weight loss during
thermal depolymerization, are shown in Fig. 3. Mass loss and peak
temperature (the temperature at which there is maximum mass varia­
tion rate) values for each of the events are shown in Table 4.
As may be observed in Fig. 3, the thermal decomposition of the
microcapsules occurred in three main states. The microcapsules
analyzed exhibited similar values for mass loss percentage, showing only
slight variations that may be related to the presence of the encapsulation
agent and the techniques used.
For all microcapsules produced, the first thermal event exhibited a
weight loss of <10 %. The first mass loss corresponds to the evaporation
of free water and residual moisture on the surfaces of the microcapsules,
as well as the evaporation of bound molecular water [63,70]. The loss in
mass at this stage was between 5.78 and 9.99 %, the start and end
E.J.G. Laureanti et al. International Journal of Biological Macromolecules 253 (2023) 126969

Fig. 3. TGA and DTG curves of pink pepper extract and green propolis microcapsules produced using maltodextrin and a mixture of maltodextrin and gum arabic.

loss in which the “husk” is broken, causing the soy oil to evaporate.
Table 4
Finally, a third stage was observed between 375 and 500 ◦ C, corre­
Thermal events from the thermogravimetric analysis of the developed films.
sponding to the additional decomposition of the wall material, the rapid
Treatment First event Second event Third Event loss of the oil, and the carbonization of the residual material.
TP1 (◦ C) m (%) TP2 (◦ C) m (%) TP4 (◦ C) m (%) Tang et al. [61]conducted microencapsulation of gardenia yellow
IA 64.49 9.99 314.92 54.49 476.18 34.07 pigment using four types of encapsulating agents: maltodextrin, gum
IIA 60.80 5.78 315.26 65.49 487.25 29.12 arabic, isolated soy protein, and whey protein isolate. In contrast to the
IB 90.63 6.42 316.27 60.06 480.21 29.94 present study, the authors identified four degradation stages for the
IIB 65.16 7.23 313.92 65.64 461.77 20.61 agents whey protein isolate, isolated soy protein, and MD:GA, which
correlated as follows: at 30–140 ◦ C, the rate of mass loss of the three
temperatures of the event varying between 34.31 and 165.73 ◦ C. types of microcapsules was about 6 %, primarily due to the evaporation
A second thermal event was observed in the 123.49–401.42 ◦ C of free water; the second stage was between 140 and 220 ◦ C, which was
temperature range; it was associated with a loss in mass that varied from caused by loss of bound water and volatile decomposition products
54.49 to 65.64 %. According to Sanchez-Reinoso e Gutiérrez [70], it may (mass loss rate was about 10 %); the third stage was from 220 to 400 ◦ C,
be related to the thermal decomposition of long chains of poly­ and correlates with the loss of mass of the wall material and the pigment
saccharides from the materials that constitute the wall, polymerization (resulting in intermediates such as CO2 and H2O); finally, the fourth
processes and isothermal reactions associated with dehydration. More­ stage was 400–900 ◦ C, and the intermediate products were subsequently
over, it may be seen on all thermograms from the various samples that charred.
the second event occurred in a consecutive reaction; that is, slight
shoulders and a peak are present in each of the DTG curves. The 3.6. Surface morphology analysis
shoulders were present at temperatures between 123.49 and 165.73 ◦ C,
whereas the peaks occurred between 254.91 and 272.35 ◦ C. Scanning electron microscopy is frequently used to evaluate the ef­
The last stage occurred at temperatures between 396.73 and ficiency of microencapsulation, the shape of the microparticle, and its
587.49 ◦ C, and mass loss varied between 20.61 and 34.07 %. At this general characterization. The evaluation of the structure of micro­
stage, additional decomposition of the material of the wall was encapsulated products is of great importance, since this aspect is related
observed, as well as the rapid loss of the encapsulated extracts and to the amount of protection afforded by the use of various polymers. This
carbonization of residual materials (intermediate products) [71]. From protection capacity arises from the degree of integrity and porosity of
this thermal behavior, it may be concluded that the microcapsules the microparticles [72]. The micrographs of the microcapsules may be
produced may be submitted to the thermal processes used in the food, seen in Fig. 4.
pharmaceutical, and cosmetics industries, without their properties being The morphological characteristics of the microcapsules varied ac­
altered due to thermal decomposition. cording to the drying method used. As may be seen in Fig. 4, the freeze-
Similar results were observed by Zhu et al. [71] for the production of dried microparticles exhibited larger sizes (IA and IB). According to
spray-dried corporal microcapsules of soy oil using maltodextrin. As in Rezende, Nogueira and Narain [30], this may be due to the low tem­
the present study, these authors identified three stages of degradation. peratures used during the process and the absence of resistance to break
Approximately 4.0 % of the mass loss occurred below 150 ◦ C, due to the the frozen drops or alter the surface during drying. No additional
loss of residual moisture on the surfaces of the microcapsules. The sec­ agglomeration or fusion of the particles was observed.
ond stage was observed between 200 and 375 ◦ C, which resulted in mass When compared to the freeze-dried microparticles, those produced
losses between 18 and 60 %; this stage is related to the structure of the using the spray-drying technique exhibited surfaces that were more
microcapsules, which are severely damaged during this stage of mass spherical and smoother, having shapes that were more regular (Fig. 4;
IIA and IIB). Moreover, these microparticles did not exhibit cracks or

8
E.J.G. Laureanti et al. International Journal of Biological Macromolecules 253 (2023) 126969

Fig. 4. Morphological analysis of the surface of the microcapsule produced by spray and freeze-drying, using maltodextrin and gum arabic as an encapsulation agent
(a. 100 x; b. 800 x; c. 5000 x).

fractures. Spray-drying resulted in the formation of some particles

whose surfaces were more wrinkled and smashed, an observation that
may be explained by the rapid removal of moisture and rapid cooling of
the particles produced.
With regard to the encapsulation agents, it may be observed that the
maltodextrin and gum arabic combination resulted in rougher particles
with more irregular shapes that were smashed and had deep cavities.
The ratio between coating material and encapsulated substance
(coating:nucleus) may be responsible for the roughness of the micro­
capsules, a characteristic that is also associated with the sudden loss of
moisture and cooling [31].
In Fig. 4 (IIB – c.), two orifices may be seen on the surface. According
to Sarabandi et al. [9], these orifices indicate the existence of hollow
(empty) structures in the microparticles, representing the production of
particles with a matrix-type structure. In these structures, the material of
the nucleus is uniformly spread throughout the entire matrix at the
circumference of the particles. This may be explained by the fact that the
majority of the coating material:nucleus is hydrophilic, expanding and
combining uniformly to form the film and membrane.

Fig. 5. Inhibition activity of the DPPH● and ABTS● + radical in the pink
3.7. Determination of antioxidant activity using DPPH● and ABTS●+ pepper and green propolis extract microcapsules produced from maltodextrin
radicals and a mix of maltodextrin and gum arabic.

The results for the DPPH● radical inhibition percentages (%I) ranged
from 59.91 ± 1.56 % to 79.64 ± 0.59 % for the four samples, the
calculated values of which are shown in Fig. 5. In general, the IIB
treatment (MD:GA in the formulation, produced by spray-drying)
exhibited a greater inhibition percentage than all other samples and
was therefore shown to be the best option for protecting the antioxi­
dants. However, the IIB sample did not exhibit any significant difference
as determined by the Tukey test (p ≤ 0.05) when compared to the IB
sample (which used the same formulation but was dried using the freeze-
drying technique). Therefore, the technique used for producing the
microcapsules did not affect the results for the inhibition of the DPPH●
radical, possibly due to drying time, which is shorter for spray-drying
than for freeze-drying so that the process occurs almost instanta­
neously and results in a considerably low loss in bioactive compounds
and does not affect degradation, despite the higher temperatures used
[30].
With regard to the encapsulation agent, it was observed that the

9
E.J.G. Laureanti et al.
addition of GA to the formulation resulted in an increase of approxi­
mately 31 % in the inhibition of the DPPH● radical. The ability to
produce microcapsules having a high level of antioxidant potential by
combining MD with GA is greater than when only MD is used in the
formulation, indicating a greater protection for the bioactive com­
pounds. This may be related to the structural characteristics of the wall
materials used [37].
The inhibition percentage observed using the ABTS●+ method
ranged from 70.40 ± 0.71 % to 85.71 ± 0.50 %; once again, the greatest
value was observed for the sample with the MD:GA combination, pro­
duced using the spray-drying technique. As was observed in the DPPH●
analysis, the encapsulation agent used affected the results, a 17 % in­
crease in inhibition being observed for the samples using MD and GA as
encapsulation agents.
Sarabandi et al. [9] reported results for the microencapsulation of
eggplant skin extract, using GA and MD (individually) as encapsulation
agents for the production of a natural antioxidant and coloring agent.
The DPPH● radical inhibition percentages ranged from 55.48 ± 0.97 %
to 73.38 ± 1.03 %, whereas those of the ABTS●+ analysis ranged from
86.87 ± 0.39 % to 90.54 ± 0.22 %, values similar to those observed in
the present study.
3.8. Analysis of the release of total phenolic content
The protection of antioxidant compounds during storage is not the
only use being reported by researchers for the encapsulation technique;
recent studies also report the behavior of the microcapsules as they pass
through the human gastrointestinal tract in order to monitor how the
antioxidant is released at specific points of the tract in which absorp­
tion/activity may occur [73]. The digestibility of the microencapsulated
bioactive compounds in simulated gastric fluid (SGF) and simulated
intestinal fluid (SIF) is shown in Fig. 6.
Fig. 6 shows a final incubation time of 2 h and reveals that the values
for the TPC released from the freeze-dried microcapsules (IA and IB)
were significantly greater (Tukey test, p ≤ 0.05) than those obtained
with the spray-drying technique (IIA and IIB). This behavior is possibly
related to the decreased effectiveness of the encapsulation technique of
freeze-drying, leading to an increase in the release of bioactive com­
pounds; this corroborates the results obtained for the
Fig. 6. Percentage of phenolic compound release after 2 h test.
10
International Journal of Biological Macromolecules 253 (2023) 126969
microencapsulation efficiency evaluation [74].
In Fig. 6, it may be seen that the release of TPC from the microcap­
sules produced using only MD as an encapsulation agent (IA e IIA)
exhibited greater values for SGF than with SIF. On the other hand, mi­
crocapsules produced with MD and GA (IB and IIB) exhibited the
opposite behavior with regard to the release of TPC, the highest values
being observed for SIF. The greater percentages observed for release in
the intestinal phase may be explained by greater quantities of phenolic
compounds and flavonoids being released from the microcapsules,
especially from the GA encapsulation agent, which undergoes minor
degradation than MD upon contact with a pH neutral (7.4) environment
and before reaching the SIF [75].
These results show that MD provides greater protection for total
phenolic content with regard to release in the intestinal phase, whereas
the MD and GA combination provides greater protection in the gastric
phase. The difference in the proportion of the total phenolic content
release may be related to the differences in the characteristics of the wall
material and the interactions that occur between the total phenolic
content and the wall materials [76]. The main goal of encapsulation is to
protect phenolic compounds from degradation in the gastric phase
before they reach their target, that is, the intestine. It is therefore
essential to understand how the phenolic compounds are released from
the encapsulated structures during digestion [73].
The low levels of activity observed in the gastric stage of digestion
may be related to the low content of phenolic compounds released in this
pH from the surface of the microcapsules and/or by the penetration of
the simulated gastric fluid into the microcapsules through their surface
pores. Similar results were reported by Dadi et al. [74] for the produc­
tion of Moringa stenopetala extract microcapsules produced by freeze-
drying and spray-drying using MD and high-methoxyl pectin. The au­
thors attribute the behavior exhibited by the microcapsules to differ­
ences in the breakage of the coating material depending on composition
and gastrointestinal conditions. Methoxyl pectin is more soluble when
the pH is approximately 7, as in intestinal fluid.
Kinetic modeling is essential for devising a system that exhibits a
predictable and specific behavior. Therefore, four different models (zero
order, first order, Higuchi and Korsmeyer-Peppas) were fit to the
experimental release data in order to analyze the kinetic behavior of the
PPE:GPE extract microparticles coated with MD and MD:GA. The results
E.J.G. Laureanti et al. International Journal of Biological Macromolecules 253 (2023) 126969

obtained are shown in Table 5.
The adjusted and calculated determination coefficients (R2), root
mean square error (RMSE) and the corrected Akaike information crite­
rion (AICc) were evaluated. The Korsmeyer-Peppas model [77,78],
which best described the system, is a simple, semi-empirical model
(higher R2; lower RMSE and AICc). It is described by Eq. (5):
Mt
= ktn
M∞
The n release exponent values were 0.5083–0.6441 (pH 1.2) and
0.6964–0.7680 (pH 7.4). These values obtained indicate a mass transfer
that follows a non-Fickian diffusion mechanism (values between 0.43 <
n < 0.85 for spherical particles). Therefore, the type of transport is
“anomalous”, which means that in this case there is an overlap of
different types of phenomena, including potentially bioactive diffusion
and polymer swelling [79].
Maltodextrin exhibited better protection of total phenolic content
regarding the release in the intestinal phase, whereas the MD and GA
combination exhibited better protection in the gastric phase. Since the
objective of encapsulation is to protect the phenolic compounds from
degradation in the gastric segment, before their arrival in the intestinal
segment, the use of maltodextrin combined with gum arabic is a better
choice for this purpose. Moreover, these particles, as compared to those
obtained by spray drying, showed better results and were produced
using a simpler and faster technology at lower costs. Based on these
aspects, it may be concluded that the spray-drying technique is the best
option for industrial applications.
4. Conclusions
The encapsulation of PP and GP using spray drying and freeze-drying
techniques, with MD and GA as encapsulating agent, was successfully
achieved. The microcapsules produced using the combination of MD and
GA as wall materials exhibited higher encapsulation efficiency values for
both techniques. All results exhibited a moisture content of <7 %, which
is considered a relevant characteristic for microcapsules, particularly in
the food industry, where the maximum moisture content is generally
around 4 %, which aligns with the results obtained for treatments IIA
and IIB. The water activity values in all samples was within the range
expected for powdered products, as well as within the range of values
recommended to guarantee a stable shelf life against microbe growth
(5) (<0.3). The addition of GA to the formulation resulted in a 31 % increase
in the inhibition of the DPPH● radical and 17 % increase being observed
in the ABTS●+ inhibition percentage, revealing the greater potential of
the MD and GA combination for producing microcapsules with high
antioxidant values. Finally, from the data obtained using the total
phenolic content release analysis, it has been concluded that the opti­
mum encapsulation process, primarily due to its superiority in most of
properties, involves the spray-dried microcapsules using the MD and GA
combination. This treatment provided enhanced protection during the
gastric stage (protecting the phenolic compounds from degradation in
the gastric segment, before reaching the intestinal segment), and
therefore represent the best formulation for a future application in the
microcapsule industry. Further researches are required to investigate
controlled release of these microcapsules in specific applications, such as
such as the encapsulation of flavors, lipids, antioxidants in the food in­
dustry, and for controlled drug release in the pharmaceutical industry.
CRediT authorship contribution statement
Emanuele Joana Gbur Laureanti: Conceptualization, Data curation,
Formal analysis, Investigation, Methodology, Resources, Roles/Writing -
original draft, Writing - review & editing, Visualization; Thainnane Silva
Paiva: Data curation; Luiz Mário de Matos Jorge: Supervision; Concep­
tualization, Methodology, Validation; Regina Maria Matos Jorge: Su­
pervision, Conceptualization, Data curation, Formal analysis,
Investigation, Methodology, Validation, Resources, Writing - original
draft, Writing - review & editing, Visualization;

Table 5
Analysis of the release kinetics models of the PPE:GPE microcapsules.
Treatment Condition/ Model Zero-order First-order Higuchi Korsmeyer-Peppas n* Release mechanism

IA pH 1.2 R2adjusted 0.7993 0.7807 0.9961 0.9943 0.6441 Non-Fickian diffusion

R2calculated 0.9486 0.6980 0.9961 0.9943
RMSE 7.0438 17.0704 1.9348 0.0537
AICc 49.52 58.37 36.60 35.69
pH 7.4 R2adjusted 0.9534 0.9190 0.9523 0.9610 0.7680 Non-Fickian diffusion
R2calculated 0.9340 0.8446 0.9523 0.9610
RMSE 7.1593 10.9832 6.0857 0.1703
AICc 49.68 53.96 48.06 33.01
IIA pH 1.2 R2adjusted 0.7944 0.7039 0.9106 0.9643 0.5083 Non-Fickian diffusion
R2calculated 0.7944 0.5388 0.9106 0.9643
RMSE 10.6463 15.9439 7.0217 0.1077
AICc 53.65 57.69 49.49 46.62
pH 7.4 R2adjusted 0.9685 0.8771 0.9780 0.9798 0.6993 Non-Fickian diffusion
R2calculated 0.9640 0.8285 0.9784 0.9798
RMSE 4.4806 9.7148 3.4515 0.1106
AICc 45.00 52.74 42.39 33.16
IB pH 1.2 R2adjusted 0.9195 0.7696 0.9812 0.9907 0.6391 Non-Fickian diffusion
R2calculated 0.9195 0.6389 0.9812 0.9907
RMSE 8.6033 18.2211 4.1607 0.0682
AICc 51.52 59.03 44.26 33.19
pH 7.4 R2adjusted 0.9730 0.9458 0.8907 0.9418 0.7249 Non-Fickian diffusion
R2calculated 0.9730 0.9528 0.8907 0.9331
RMSE 5.3772 7.0456 10.7267 0.2305
AICc 45.82 49.52 53.73 56.78
IIB pH 1.2 R2adjusted 0.7762 0.6904 0.8908 0.9439 0.5972 Non-Fickian diffusion
R2calculated 0.7764 0.4392 0.8908 0.9390
RMSE 11.6251 18.4094 8.1243 0.1676
AICc 54.53 59.13 50.95 49.60
pH 7.4 R2adjusted 0.8963 0.9451 0.9066 0.9011 0.6964 Non-Fickian diffusion
R2calculated 0.8790 0.9532 0.9066 0.9011
RMSE 9.0839 5.6535 7.9864 0.2540
AICc 52.06 47.32 50.78 51.74

11
E.J.G. Laureanti et al.
Declaration of competing interest
The authors declare no conflict of interest.
Acknowledgments
The authors gratefully acknowledge the University of Paraná for
making their research possible, the Center for Electron Microscopy of
the UFPR (CME) for the production of all the micrographs, and the
financial support provided by the Coordenação de Aperfeiçoamento de
Pessoal de Nível Superior (CAPES) and National Council for Scientific
and Technological Development (CNPq, Brazil) (grant numbers:
312215/2017-7 and 315598/2020-4.
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