| |

Received: 23 April 2020    Revised: 4 July 2020    Accepted: 15 July 2020

DOI: 10.1111/jfpp.14805

ORIGINAL ARTICLE

Microencapsulation of an essential oil (cinnamon oil) by spray

drying: Effects of wall materials and storage conditions on
microcapsule properties

Qirui Hu1 | Xia Li1 | Fang Chen1,2 | Renkou Wan1 | Cheng-Wei Yu1  | Jing Li1  |

David Julian McClements3 | Zeyuan Deng1

1
State Key Laboratory of Food Science
and Technology, College of Food Science, Abstract
Nanchang University, Nanchang, Jiangxi, Microencapsulation of cinnamon essential oil (CEO) by spray drying was carried out
China
2 to protect it from oxidation and facilitate its application within food products. Whey
School of Public Health, Nanchang
University, Nanchang, Jiangxi, China protein isolate (WPI), maltodextrin (MD), and sodium alginate were selected as wall
3
Department of Food Science, University of materials. Initial experiments were carried out to evaluate the emulsifying capacity
Massachusetts, Amherst, MA, USA
and encapsulation efficiency (EE) of the system. The optimum formulation consisted
Correspondence of 70% wall material (WPI: MD: sodium alginate = 1:3:0.01 (w/w)) and 30% CEO. The
Fang Chen and Zeyuan Deng, State Key
Laboratory of Food Science and Technology,
EE of the spray-dried CEO microcapsules formed was over 93%, and their retention
Nanchang University, 235 Nanjing East during storage at 50°C for 30 days was over 95%. Gas chromatography and liquid
Road, Jiangxi, Nanchang, China.
Email: xinganchenfang@163.com (F. C.) and
chromatography in conjunction with mass spectrometry were used to identify the re-
dengzy@ncu.edu.cn (Z. D.) action products formed during oxidation of the CEO and possible oxidation pathways

Funding information
State Key Laboratory of Food Science and
Technology Free Orientation Project, Grant/
Award Number: SKLF-ZZB-201709; National
Natural Science Foundation of China, Grant/
Award Number: 31872890
were proposed. The optimized formulation identified in this study may be suitable
for the efficiency encapsulation and stabilization of essential oils in powdered form.
Practical applications
The optimized spray drying formulation can be applicated in processing essential oil
to improve their storage stability. The spray-dried product in this study can be uti-
lized in meat preservation and pastry (or biscuit) processing as food additives.

1 |  I NTRO D U C TI O N
Cinnamon, which has been widely used historically as an herbal
medicine, belongs to the Lauraceae family and is mainly found in
China and some Southeast Asian countries (Rao & Gan, 2014).
Cinnamon essential oil (CEO) is a volatile substance that is typically
isolated from the bark of the cinnamontree (Ackermann, Aalto-
korte, Jolanki, & Alanko, 2009). CEO contains a range of different
aromatic compounds and terpenes, including cinnamaldehyde
(70%–80%, w/w), acetophenone (0.3%–0.9%, w/w), benzaldehyde,
cinnamyl acetate, and camphor (Li, Kong, & Wu, 2013). In the food
industry, CEO is widely used as a spice and preservative due to its
unique organoleptic, antimicrobial (Goñi et al., 2009; Zhang, Liu,
Wang, Jiang, & Quek, 2016), and antioxidant properties (Özcan &
Arslan., 2011). It has also been proposed that it can be used as a
nutraceutical or medical agent due to its potential anticancer (Yang,
Zheng, Ye, Li, & Chen, 2016) and anti-inflammatory activities (Tung,
Chua, Wang, & Chang, 2008). However, CEO tends to chemically de-
grade when exposed to heat, light, or oxygen (Hermanto, Khasanah,
Kawiji, Manuhara, & Utami, 2016), which leads to a loss in its ben-
eficial biological activities (Turek & Stintzing, 2013). Consequently,
there is a need to develop effective strategies to protect CEO from
degradation during storage.
Microencapsulation is the process where by a substance of
interest (the “core” material) is encapsulated within another sub-
stance (the “wall material”) in the form of tiny capsules (Zuidam &
Shimoni, 2010). Spray drying is a commonly used technology to
encapsulate fragrances, oils, and flavors because it is inexpensive,

J Food Process Preserv. 2020;00:e14805. wileyonlinelibrary.com/journal/jfpp |

© 2020 Wiley Periodicals LLC.     1 of 15
https://doi.org/10.1111/jfpp.14805
 |
2 of 15       HU et al.
reproducible, and easy to scale up (Gharsallaoui, Roudaut, Chambin,
Voilley, & Saurel, 2007). It is particularly suitable for creating pow-
dered forms of heat-sensitive materials because the relatively short
drying times involved (5–30 s) do not lead to excessive thermal dam-
age (Encina, Vergara, Giménez, Oyarzún-Ampuero, & Robert, 2016).
The potential for using spray drying to form CEO microcapsules has
been demonstrated previously, but the encapsulation efficiency (EE)
obtained was relatively low, that is, <85% (Hermanto et al., 2016;
Pratiwi, Darmadji, & Hastuti, 2016). One of the main objectives of
the current study was, therefore, to optimize the formulation and
spray drying conditions so that CEO microcapsules with a higher EE
could be produced. Previous studies have reported that the solubil-
ity and molecular mobility of the core materials within microcapsules
depends on the nature of the wall materials used, which in turn influ-
ences the EE (Gharsallaoui et al., 2007). For this reason, we paid par-
ticular attention to optimizing the formulation of the wall materials
used to encapsulate the CEO.
Proteins, such as whey protein, have good emulsifying and
film-forming properties because of their amphiphilic characteristics
(Sosa, Schebor, & Pérez, 2015). In this study, we examined the po-
tential of using whey protein isolate (WPI) to emulsify the essential
oils. Moreover, proteins like sodium caseinate can play a role in sta-
bilization of emulsion as an electrosteric stabilizer (Patel, Bouwens,
& Velikov, 2010), thereby, improve the qualities of microcap-
sules. Some studies, however, have shown that the microcapsules
formed by proteins after spray drying are deformed and shrunken
(Darniadi, Ho, & Murray, 2018), which may have adverse effects
on the long-term stability of microencapsulated essential oils. For
this reason, carbohydrates like maltodextrin (MD) are often used
as secondary wall materials to enhance the formation and storage
stability of microcapsules (Shamaei, Seiiedlou, Aghbashlo, Tsotsas,
& Kharaghani, 2017; Troya, Tupuna-Yerovi, & Ruales, 2018). Other
studies have shown that polysaccharides, such as sodium alginate,
can also be used as emulsion thickeners to enhance the properties of
microencapsulated oils (Yoo, Song, Chang, & Lee, 2006). For this rea-
son, we examined the impact of using different ratios of WPI, MD,
sodium caseinate and sodium alginate on the formation and perfor-
mance of the wall materials in microencapsulated CEO.
In spite of good film-forming properties, WPI possesses poorer
emulsion capacity than low molecular weight emulsifiers due to its
slower diffusion rate (Lam & Nickerson, 2013). Low molecular weight
emulsifiers can reduce the droplet size, increased the viscosity of the
emulsions, and facilitate the formation of strongly adsorbed film (Lu,
Kelly, & Miao, 2017). Therefore, mixed emulsifiers could be a good
choice to enhance the properties of microencapsulated oils, which
received little attention in related researches to our knowledge.
Previous studies have reported that sucrose esters could enhance
the properties of protein-stabilized emulsion (Zhao et al., 2014).
Moreover, HLB is a vital factor affecting the quality of microencap-
sulated oils (Liu & Yang, 2011), sucrose ester should be used in com-
bination with an emulsifier of low HLB value to obtain an appropriate
HLB value. Monoglyceride is a lipophilic emulsifier and can modify
the properties of protein-stabilized emulsions (Lu et al., 2017). For
these reasons, we used WPI, sucrose esters and monoglyceride as
mixed emulsifiers during preparation of microencapsulated CEO.
The characteristics of the wall materials are known to strongly
influence the functional performance of microencapsulated oils
(Labuschagne, 2018). For this reason, we examined the impact of wall
material (including mixed emulsifiers) composition on the formation and
stability of CEO microcapsules. Initially, the CEO was converted into an
emulsion by homogenization, and then these emulsions were converted
into a powder by spray drying. The impact of the initial formulation on
the physicochemical properties and stability of the CEO emulsions and
microcapsules were then evaluated. In particular, possible oxidation
pathways of CEO during storage were explored. This study may lead to
the development of more effective methods of protecting essential oils
from loss during storage, as well as improving their utilization in meat
preservation and pastry (or biscuit) processing as food additives.
2 | M ATE R I A L S A N D M E TH O DS
2.1 | Materials
Cinnamon essential oil (CEO, ≥95% cinnamaldehyde) was purchased
from Jiangxi Huitong Officinal Perfume Oil (Jiangxi, China). Whey
protein isolate (WPI, food grade, ≥80% whey protein) was pur-
chased from Jiangxi Baiying Biotechnology (Jiangxi, China). Sucrose
ester (food grade, HLB = 15) was purchased from Hangzhou Ruilin
Chemical (Hangzhou, China). Monoglyceride (food grade, HLB = 3.6)
was purchased from Henamsiyuanshengwu Technology (Henan,
China). Maltodextrin (MD, food grade, DE16) was purchased from
Shandongxiwangdianfen (Shandong, China). Sodium alginate (food
grade) was purchased from Hebei Baiwei Biological Technology
(Hebei, China). Sodium caseinate (food grade) was purchased from
Shanghai Tianchen Biological Technology (Shanghai, China). Vitamin
E oil (food grade) was purchased from Henan Together Glorious Food
Ingredients (Henan, China). Acetonitrile (HPLC grade) was purchased
from Merck (Darmstadt, Germany). Cinnamaldehyde standards were
purchased from Aladdin (Shanghai, China). Dipotassium phosphate,
mono potassium phosphate, petroleum ether, ethanol, and ether
were purchased from Xilong Scientific (Guangdong, China),
2.2 | Preparation of microcapsules
The procedure used to prepare the CEO microcapsules is shown
schematically in Figure 1. The aqueous phase was prepared by dis-
solving the wall materials and sucrose ester in distilled water. The
oil phase was prepared by mixing CEO and monoglyceride. The oil
and aqueous phases were then mixed together by simple shear-
ing. The coarse emulsion formed was then passed through a colloid
mill (50LA model, Shanghai Donghua High Pressure Homogenizer
Factory, Shanghai, China) and then a high-pressure homogenizer
(60-6S model, Shanghai Donghua High Pressure Homogenizer
Factory, Shanghai, China) operating at 30 MPa for 3 min. The fine
HU et al. |
      3 of 15

F I G U R E 1   Flow chart of cinnamon essential oil (CEO) microcapsule product preparation

TA B L E 1   Various formulations of
Wall material (g/100 g emulsion)
emulsions Ratio of CEO
Sodium Sodium WPI/MD (g/100 g
Formulation WPI MD alginate caseinate (w/w) emulsion)

1 8.4 12.6 1:1.5 9

2 7 14 1:2 9
3 5.25 15.75 1:3 9
4 5.25 15.75 0.1 1:3 9
5 5.25 15.75 0.05 1:3 9

Abbreviations: CEO, cinnamon essential oil; MD, maltodextrin; WPI, whey protein isolate.

emulsion formed was then spray-dried in a spray drying tower
(MDR-50 model, Wuxi Modern Spray Drying Equipment Co., Ltd,
Jiangsu, China) using an inlet air temperature of 180°C, an outlet air
temperature of 90°C and centrifugal atomizer speed of 0.084 × g.
Oxidation was inhibited by adding a natural antioxidant (0.1% (w/w)
vitamin E) to the CEO at the beginning of the process.
wall materials were mixed together to produce a total “solids” con-
tent (CEO plus wall materials) in the emulsions of 30% (w/v). The
resulting emulsions were then homogenized and spray-dried as de-
scribed earlier. The properties of the CEO microcapsules formed
were analyzed and the results used for the optimization of the wall
material formulation.

2.2.1 | The emulsifying capacity of the 2.2.3 | Identification of the functional groups of

wall materials CEO microcapsules

The emulsifying capacity of the WPI was determined by dissolving
different concentrations (3%–7% w/v) of the powdered protein into
500 ml of distilled water and then adding 45 g of CEO. After being
homogenized at 30 MPa for 3 min, the properties of the emulsions
were analyzed.
2.2.2 | Optimization of the formulation of
wall materials
A variety of wall material formulations with different compositions
were prepared according to Table 1. Afterwards, 30% CEO and 70%
Alterations in the functional groups in the CEO due to microen-
capsulation were determined by analyzing the chemical composi-
tion of the oil before and after the preparation procedure. Fourier
transform infrared spectroscopy (FTIR) transmission spectra were
taken using an FTIR spectrometer (NICOLET5700, Thermo Fisher,
Nicolet, USA) in the wavenumber range from 4,000 to 500 cm−1
at a spectral resolution of 4 cm−1 with 32 scans per sample. Four
samples (wall materials, CEO microcapsules, CEO extracted
from the CEO microcapsules, and free CEO) were mixed with
KBr powder for FTIR measurements. Data were analyzed using
the software that came with the instrument (OMNIC 8.0 and
OriginPro 9.0).
 |
4 of 15       HU et al.
2.3 | Emulsion analysis
2.3.1 | Creaming stability
The creaming stability of the emulsions was evaluated using a
method described previously (Aguiar, Silva, Rezende, Barbero, &
Martínez, 2016), with some slight modifications. Immediately after
an emulsion was prepared, a 10 ml of aliquot was transferred into a
15 ml centrifuge tube. After incubation in a water bath at 60°C for
20 min, the tubes were centrifuged at 1500 × g for 5 min. The height
of the emulsified phase was measured and the creaming index was
calculated as follows:
H1
Creaming index (%) = × 100%
H0
where H0 is the initial height of the emulsion and H1 is height of the
emulsified phase.
2.3.2 | Droplet size and charge characteristics
The emulsions were diluted 20-times using distilled water and then
the mean droplet diameter, polydispersity index (PDI), and surface
potential (ξ-potential) were measured using dynamic light scatter-
ing/electrophoresis (Zetasizer Nano ZS90, Malvern Instruments,
Malvern, UK) at a scattering angle of 90° at 25°C.
2.4 | Microcapsule analysis
2.4.1 | Total and surface oil
The total oil and surface oil were measured using the Rose—Gottlieb
method with some slight modifications.
Total oil: A weighed amount of powdered microcapsules (2 g) was
dispersed in warm distilled water (10 ml) in a 100-ml Erlenmeyer flask
and then 15 ml of ethanol was added. Afterwards, 25 ml of ether was
added and then the Erlenmeyer flask was shaken for 1 min. Petroleum
ether (10 ml) was then added and the Erlenmeyer flask was plugged
and shaken for another 1 min. After stratification, the organic phase
was collected and transferred into a weighed flask (m1). Ethanol (5 ml),
ether (15 ml) and petroleum (5 ml) ether were then added to the re-
maining aqueous phase sequentially and the solvent extraction pro-
cedure was repeated three times (but only 15 ml of diethyl ether was
added the third time). Finally, all the organic phases were combined
together. The organic phase was concentrated using a rotary evapo-
rator (RE -2000A model, Shanghai Yarong Biochemistry Instrument
factory, Shanghai, China) operating at 50°C until all the solvent was
evaporated. The flask containing the solids was weighed (m2) and the
total oil content (OC) calculated: total oil = m2 − m1.
Surface oil: Microcapsule powder (2 g) was put into a 100-ml
Erlenmeyer flask. The Erlenmeyer flask was shaken slightly after ether
(20 ml) was added. After filtration, the filtrate was transferred into
a weighed flask (m3) and the precipitate was extracted with diethyl
ether (15 ml) twice. All the filtrates were combined and concentrated
using a rotary evaporators (RE -2000A model, Shanghai Yarong
Biochemistry Instrument factory, Shanghai, China) at 50°C until the
solvent was evaporated. The flask containing the solids was weighed
(m4), and the surface oil was calculated: surface oil = m3 − m4.
2.4.2 | EE, OC, and retention rate
The EE, OC and retention rate (RR) of the CEO microcapsules were
calculated using the following equations, respectively:
total oil − surface oil
encapsulation efficiency (%) = × 100%
total oil
total oil − surface oil
oil content (%) = × 100%
W0
retention rate (%) =
total oil
× 100%
W1
Here, W0 is the weight of the microcapsule powder and W1 is
the weight of CEO in the microcapsule powder in theory (calculated
from the known amount added at the beginning).
2.4.3 | Particle morphology analysis
The microstructural characteristics of the microcapsules were ana-
lyzed by scanning electron microscopy (SEM) (Hitachi S-3400N,
Hitachi Limited, Japan). The samples were placed on an aluminum
support using a conductive tape and then coated with platinum
using an E-1010 sputter coater (Hitachi Limited, Japan). The images
were taken using an acceleration voltage of 5.00 kV.
2.5 | Oxidative stability of microcapsules
The microcapsules were stored in a constant-temperature oven set
at 25°C, 37°C, or 50°C. A sample of pure CEO was also stored at
50°C for comparison. Samples were removed from the oven at 1,
7, 15, 30, 60, and 90 days to analyze the alteration of RR and the
compositions of the CEO microcapsules. The RR of the initial CEO
microcapsules was set as 100%.
2.5.1 | Fluorescence analysis by HPLC-
fluorescence detector
Changes in the level of fluorescent substances in the CEO mi-
crocapsules was determined using high-performance liquid
HU et al.
TA B L E 2   Effects of WPI concentration on emulsion characteristics
Concentration (%) Ratio of WPI/CEO (W/W) Creaming index (%)
a c
3 3:9 90.7 ± 2.3
b ab
4 4:9 95.4 ± 1.8
5 5:9 100.0 ± 0.0 c
c a
6 6:9 100.0 ± 0.0
7 7:9 100.0 ± 0.0 c
Note: Means followed by different letters within each column are significantly different (p < .05).
Abbreviations: CEO, cinnamon essential oil; PDI, polydispersity index; WPI, whey protein isolate.
chromatography (Agilent 1260 HPLC system, Agilent Technologies,
USA) equipped with a fluorescence detector (FLD). The column was
an Agilent Zorbax Edipse plus C18 (250 mm, 4.6 mm, 5 mm) col-
umn. The elution phases used were: Phase A—0.1% (v/v) aqueous
formic acid; Phase B—acetonitrile modified with 0.1% formic acid.
Elution was carried out in gradient mode as follows: 0–5 min (80%-
87%, B), 5–9 min (87%–90%, B), 9–12 min (90%-95%, B), 12–15 min
(95%–100%, B), 15–38 min (100%, B). The injection volume was 3 μl
and the column temperature was set at 25°C. The flow rate was set
at 0.5 ml/min. The excitation and emission wavelengths were set at
450 nm and 530 nm, respectively.
2.5.2 | Compositions of oxidized CEO
The composition of the CEO after being oxidized was determined
using liquid chromatography coupled with mass spectrometry. The
UPLC-electrospray ionization source (ESI)-QTOF-MS/MS analy-
sis was performed on an Agilent 1290 Infinity LC system (Agilent
Technologies, USA) coupled with an Agilent 6430 triple quadru-
pole mass spectrometer (Agilent Technologies, USA). The chroma-
tographic separations were performed on a Shim-pack GIST C18
column (2.1 mm, 75 mm, 2 μm). The flow rate was 0.2 ml/min, and
the injection volume was 5 μL. The mobile phase consisted of 0.1%
formic acid (A) and acetonitrile modified with 0.1% formic acid (B).
A linear gradient was applied as follows: 20%–25% B at 0–10 min;
25%–80% B at 10–25 min; 80%–100% B at 25–35 min; 100% B at
35–40 min and 20% B at 40–41 min.
An ESI interface was set in positive mode. The conditions were as
follows: capillary voltage, 4 kV; drying gas flow, 10 L/min; gas tem-
perature, 350°C; nebulizer pressure, 40 psi; and fragmentor voltage,
135 V. The potential biomarkers were analyzed by tandem mass
spectrometry (MS/MS) in the Q‑TOF mode. Nitrogen was used as
the collision gas at collision energies of 30 eV. Data were collected in
total ion scan mode from 50 to 1,000 m/z.
GC-MS analysis was on an Agilent 6890N Infinity GC sys-
tem (Agilent Technologies, USA)equipped with an Agilent
19091S-433HP-5 ms column (0–325°C; 30 m × 250 μm × 0.25 μm)
and operated in a program with an initial temperature of 60°C for
2 min, rate of 8°C/min and with a final temperature of 280°C for
10 min. The injection volume was 1 μl and the injector port was op-
erated at 270°C. The carrier gas was helium followed by a 20:1 split
|
      5 of 15
Zeta potential (mV) Mean droplet size (nm) PDI
d
−10.70 ± 0.14 347 ± 12 0.34 ± 0.10a
c
−13.70 ± 0.42 257.0 ± 5.5 0.25 ± 0.01a
−18.50 ± 3.25a 233.5 ± 2.5b 0.28 ± 0.01a
a
−17.10 ± 0.14 197.6 ± 6.2 0.35 ± 0.04a
−14.35 ± 0.49ab 178 ± 12a 0.52 ± 0.06b
and a helium carrier gas flow rate was 1.56 ml/min. The ion source
was set at 230°C and quadrupole mass selective detector at 150°C
was operated in total ion scan mode from 35 to 500 m/z.
2.6 | Statistical analysis
Measurements of the emulsion or microcapsule properties were
performed in triplicate. The resulting data were then evaluated
using analysis of variance (ANOVA) using SPSS statistical software
(version 16.0) and statistically significant tests were analyzed by the
Duncan test and Tukey test at p < .05.
3 | R E S U LT S A N D D I S CU S S I O N
3.1 | Effects of WPI/CEO ratio on emulsion
characteristics
The characteristics of emulsions prepared using different WPI con-
centrations are summarized in Table 2. Stable emulsion is requisite
for spray drying. The creaming index showed that the WPI-CEO
emulsion was kinetically stable (creaming stability = 100%) when the
ratio of WPI/CEO was ≥5:9 (w/w).
Higher is the absolute value of ξ-potential within 30 mV, more sta-
ble is the emulsion (Cano-Sarmiento et al., 2018). The ξ-potential of
the WPI emulsions varied from −18.5 mV to −10.7 mV with the highest
negative value being obtained at a ratio of WPI/CEO of 5:9 (Table 2).
The mean droplet diameter became smaller as the WPI concen-
tration increased, changing from around 350 to 178 nm when the
ratio of WPI/CEO increased from 1:3 (w/w) to 7:9 (w/w). The PDI
of a colloidal dispersion is a measure of the range of particle sizes
present, with PDI < 0.3 meaning a fairly tight distribution (Salleh,
Hamid, Bustami Effendi, & Jamil, 2012). The PDI of the WPI-CEO
emulsion was lower than 0.3 when the ratio of WPI/CEO was 4:9
and 5:9 (w/w). These two emulsions, therefore, had the narrowest
particle size distributions, which can also be seen in Figure 2.
The emulsion with a mass ratio of WPI/CEO = 5:9 had a high
electrical charge, small droplet size, narrow particle size distribution,
and good creaming stability. Adding any extra protein only led to
marginal improvements in emulsion stability. For this reason, we
used the WPI/CEO = 5:9 system in all the subsequent studies.
 |
6 of 15       HU et al.

F I G U R E 2   Particle size distributions of droplets in cinnamon essential oil (CEO) emulsions prepared at weight ratios of WPI/CEO = (a)
1:3, (b) 4:9, (c) 5:9, (d) 2:3, (e) 7:9. WPI, Whey protein isolate

3.2 | Effects of various wall material formulations TA B L E 3   Effects of various formulations on microencapsulation

on microencapsulation Formulation EE (%) OC (%) RR (%)

1 84.18 ± 0.52a 20.70 ± 0.15a 73.77 ± 0.56a

3.2.1 | EE of microcapsules
b ab
2 86.55 ± 0.68 21.02 ± 0.23 73.93 ± 0.42a

To improve the encapsulation properties of the microcapsules, 3 87.28 ± 0.74b 21.42 ± 0.18b 73.90 ± 0.38a

b c
maltodextrin was used as a secondary wall material. The impact 4 87.92 ± 0.46 22.06 ± 0.28 78.12 ± 0.39b

of utilizing different mass ratios of MD-to-WPI on the microcap- 5 89.52 ± 0.52c 22.06 ± 0.26c 80.12 ± 0.41c
sule properties was determined. The microencapsulation quality Note: Means followed by different letters within each column are
was evaluated by calculating the EE, OC, and RR values (Table 3). significantly different (p < .05).
Comparing Formulations 1–3, Formulation 3 had the highest EE Abbreviations: EE, encapsulation efficiency, OC, oil content of the
(87.3%), OC (21.4%) and RR (73.9%) values. The EE and OC increased cinnamon essential oil microcapsule, RR, retention rate.

with decreasing WPI/MD ratio, however, the RR was not significantly

different. A similar trend has been reported for the EE of microcap-
sules when the WPI/MD ratio was varied by other researchers (Koç
et al., 2015). When WPI and MD are used as wall materials in com-
bination, the curing speed of the wall materials during spray drying
decreases when the ratio of WPI/MD becomes too high, which leads
to lower EE or OC of microcapsules containing volatile core materials
(Sheu & Rosenberg, 1998).
Comparing formulations 3 and 5, we concluded that the quality
of the microcapsules became significantly better when sodium al-
ginate was added (Table 2): EE increased from 87.3% to 89.5%; OC
increased from 21.4% to 22.1% and RR increased from 73.9% to
80.1%. However, there was no significant improvement in EE after
sodium caseinate was added (Formulation 4). A possible explanation
is that sodium caseinate mainly acts as an emulsifier, and there was
already sufficient whey protein present to stabilize the emulsions
(Ixtaina, Julio, Wagner, Nolasco, & Tomás, 2015). The addition of so-
dium alginate increases the viscosity of the emulsions, which may
have promoted a faster solidification process of the wall materials
during spray drying, thereby decreasing the amount of volatiles lost
(Lević et al., 2015). Sodium alginate addition, therefore, seemed to
improve the encapsulation quality of the microcapsules prepared
from MD and WPI.
In conclusion, Formulation 5 (WPI: MD: sodium algi-
nate = 1:3:0.01 (w/w)) gave a better encapsulation quality than any
of the other formulations tested.
3.2.2 | Particle morphology of microcapsules
Micrographs of the microcapsules were acquired using scanning
electron microscopy (Figure 3). In all formulations, the microcap-
sules existed as single discrete particles, which suggested that the
level of CEO on the surfaces of the microcapsules was relatively low.
Indeed, previous studies have shown that high levels of free oil on
the surfaces of spray-dried particles leads to agglomeration (Dantas,
Pasquali, Cavalcanti-Mata, Duarte, & Lisboa, 2018). This effect is
probably due to hydrophobic or capillary attraction between the oily
patches on the surfaces of the powder particles. In a previous study,
where avocado oil was encapsulated in powders formulated using
different WPI/MD ratios, it was reported that the microcapsules
aggregated at all WPI/MD ratios used (Bae & Lee., 2008), which is
different from out study. This difference may have been due to dif-
ferences in the nature of the two kinds of core material used in the
HU et al. |
      7 of 15

F I G U R E 3   Scanning electron
microscope micrographs of cinnamon
essential oil microcapsules prepared with
weight ratios of WPI:MD = 1:1.5 (a and
b), WPI:MD = 1:2 (c and d), WPI:MD = 1:3
(e and f), WPI:MD:SC = 1:3:0.02 (g and h)
and WPI:MD:SA = 1:3:0.01 (i and j). WPI,
Whey protein isolate

two studies. CEO mainly consists of aromatic compounds, while avo-
cado oil is mainly composed of aliphatic compounds.
In addition, the electron micrographs showed that irregu-
lar-shaped particles were formed at high WPI/MD ratios, but more
smooth spheroids were formed at low WPI/MD ratios (Figure 3).
Previous researchers have attributed this effect to the formation of
a softer, more porous crust during spray drying when maltodextrin is
present (Darniadi et al., 2018). Compared with Formulations 1, 2, and
3, less pores were observed in Formulation 5. The crust of the micro-
capsules appeared denser after sodium alginate was added, which
 |
8 of 15       HU et al.
should slow down the volatilization of CEO. Previous study also
revealed a fact that sodium alginate combining with other wall ma-
terials could improve the porosity (Belscak-Cvitanovic et al., 2015).
Sodium alginate made contributions to homogeneity of microcap-
sules and other wall materials could occupy the interstitial spaces of
the microcapsules. The difference in the morphology of the micro-
capsules may also explain the higher EE, OC and RR of Formulation 5.
3.3 | The optimized microencapsulation process
3.3.1 | The selection of optimized
microencapsulation process
Initially, the main factors effecting the emulsification process, such
as solid content, emulsification temperature, emulsion pH, and mixed
emulsifier formulation, were optimized using a single-factor test
(Figure S1 and Table S4) and orthogonal test (Tables S1–S3). The mi-
croencapsulation conditions for formation of the CEO microcapsules
were then optimized. The optimum formulation was found to be 70%
wall material (WPI: MD: sodium alginate = 1:3:0.01 (w/w)) and 30%
F I G U R E 4   Infrared spectra of (a) the cinnamon essential oil (CEO) microcapsules components, (b) CEO before and after
microencapsulation
CEO, with emulsifiers (sucrose ester/monoglyceride = 3:1 (w/w)) being
added at 0.1 g per 100 g CEO. Then an emulsion was formed with 40%
(w/v) solid content (wall materials plus CEO) at 55°C and pH 6.5.
Under these optimum conditions, the EE of the CEO microcap-
sules was 93.40 ± 0.21%, which was relatively high in comparison
to other reports. The EE of CEO microcapsules prepared by Pratiwi
et al. (2016) and co-workers ranged from 40.3% to 84.6%. The EE
of CEO microcapsules formulated with MD and arabic gum was re-
ported to range from 59.8% to 70.7% (Hermanto et al., 2016). This
advantage in EE, therefore, implies that proteins might be better for
encapsulating CEO than carbohydrates like arabic gum.
3.3.2 | FTIR features of spray-dried microcapsules
Fourier transform infrared spectroscopy experiments were carried
out in order to analyze molecular changes during the spray drying
process, as well as to detect chemical reactions between the wall
materials matrices and the CEO.
The presence of cinnamaldehyde in the microcapsules was
supported by the FTIR measurements (Figure 4a(i)). There was a
HU et al. |
      9 of 15

weak peak at 3028.24 cm−1, which can be associated with =C–H
stretching vibrations on the benzene ring. The peaks at 1625.11 to
1450.47 cm−1 were attributed to the C=C stretching vibration of
the benzene skeleton. Additionally, the peaks at 1,220 to 950 cm−1
were attributed to the =C–H out-of-plane bending vibration of the
−1
benzene ring and the peak at 747 cm was attributed to the =C–H
in-plane bending vibration. The strong peak at 1676.56 cm−1 was as-
sociated with a C=O stretching vibration and the two weak peaks at
2,820 and 2,720 cm−1 were attributed to the =C–H stretching vibra-
tion of the aldehyde group.
In Figure 4a(ⅲ), the broad peak at 3,420 cm−1 was assigned to
the O-H stretching vibration of the protein carboxyl, the peaks
at 1,850 to 1,650 cm−1 were attributed to the C=O stretch-
−1
ing vibration and the peaks at 1,100 to 1,000 cm were due to
the C–O stretching vibration. These peaks could also be seen
in Figure 4a(ⅱ). What is more, the characteristic absorption
peaks of cinnamaldehyde at 1,620 and 1675 cm−1 still existed in
Figure 4a(ⅱ). It followed that the infrared spectrum of (ⅱ) was
a simple superposition of (ⅰ) and (ⅲ). Meanwhile, there was no
significant difference between the infrared spectra of CEO before
and after microencapsulation (Figure 4b). To conclude, no appar-
ent chemical change of the CEO due to microencapsulation could
be detected by the FTIR method.
In a previous study, where vitamins A, D3, E, K 2, curcumin, and
coenzyme Q10 were dispersed in tuna oil, IR analysis indicated that
there was no chemical bonding between the lipids and the wall
material and that there was no observable lipid oxidation (Wang,
Vongsvivut, Adhikari, & Barrow, 2015). In another study, using atten-
uated total reflectance infrared spectroscopy, it was reported that
folic acid was only physically entrapped inside starch capsules during
microencapsulation (Perez-Masia et al., 2015).
3.4 | Oxidative stability
3.4.1 | RR of CEO during storage
The main aim of this study is to protect CEO from oxidation using
microencapsulation. For this reason, the oxidative stability of the
microcapsules was measured during storage. The RR of the CEO mi-
crocapsules decreased as the storage time increased (Table 4). As ex-
pected, the CEO microcapsules stored at 25°C (room temperature)
were the most stable ones, with the RR value only falling to 95.9%
after 90-days storage. Conversely, the CEO microcapsules stored
at 50°C were the most unstable, with the RR value falling to below
87.1% over the same period. Previous researchers have reported
that both surface and total oil in CEO microcapsules formed using
MD/arabic gum (1:1, w/w) as wall materials decreased during stor-
age (Pratiwi et al., 2016). Moreover, they reported that the loss of oil
increased with increasing storage temperature. As a result, the RR
was reduced by almost 25% after 28-days storage at 50°C (Pratiwi
et al., 2016), which suggested the WPI provided better protection to
CEO than arabic gum during storage.
3.4.2 | Predicting shelf life
As described previously, we fitted zero- and first-order reaction
models to the RR data to estimate the shelf life of the CEO micro-
capsules (Hu, Liu, Hao, Zhang, & He, 2013). The zero-order reac-
tion model had a higher correlation coefficient than the first-order
reaction one at 25 and 50°C and the correlation coefficients of both
models were close at 37°C (Table 5). It was, therefore, reasonable to
conclude that the loss of CEO followed a zero-order kinetics model.

TA B L E 4   Retention rates of essential oil at different storage temperatures of microcapsules

Temperature 1 day 7 days 15 days 30 days 60 days 90 days

a,A a,A a,A a,B a,C
25°C 100 ± 0% 99.80 ± 0.11% 99.76 ± 0.13% 98.27 ± 0.15% 97.02 ± 0.14% 95.86% ± 0.11a,D
b,A a,A b,A a,B a,C
37°C 99.76 ± 0.1% 99.58 ± 0.13% 99.44 ± 0.11% 98.38 ± 0.14% 96.87 ± 0.14% 92.60 ± 0.13%b,D
50°C 99.69 ± 0.1%b,A 98.72 ± 0.15%b,B 97.87 ± 0.12%c,C 96.92 ± 0.13%b,D 94.02 ± 0.12%b,E 87.10 ± 0.11%c,FA

Note: Means followed by different capital letters within each row are significantly different (p < .05).
Means followed by different small cases within each column are significantly different (p < .05).

TA B L E 5   The kinetic models of

First-order kinetics reaction
CEO loss during storage at different
Zero-order kinetics reaction model model
temperature
Temperature Kinetics model R2 Kinetics model R2

25°C y = 0.0485t − 0.0763 .9771 y = 0.2288e 0.037t .8154

37°C y = 0.0761t − 0.3194 .9327 y = 0.3333e 0.0365t .9523
0.0335t
50°C y = 0.1292t − 0.0493 .9459 y = 0.7876e .8253
2
Note: R , correlation coefficient; t, the storage time (day); y, the loss of CEO (%).
Abbreviation: CEO, cinnamon essential oil.
 |
10 of 15       HU et al.

The time for the RR to decrease to 50% of its initial value was used as
a measure of the shelf life of the samples. The shelf life of the micro-
capsules was estimated to be 1,032 days at 25°C, 662 days at 37°C,
and 387 days at 50°C. The storage stability of the microcapsules
was, therefore, better than that reported for the WPI-gum arabic
system mentioned ealier (Pratiwi et al., 2016). This effect might be
related to the fact that a denser (less poriferous) crust was formed
in the microcapsules prepared from WPI, maltodextrin, and sodium
alginate (Figure 3).
3.4.3 | Oxidative product analysis
Changes in the composition of the CEO during storage were
quantified using UPLC-ESI-QTOF-MS/MS and GC-MS analysis. Nine
substances were identified by UPLC-ESI-QTOF-MS/MS (Table 6 and
Figure 6) and seven substances were identified by GC-MS (Table 7
and Figure 7). Three substances were identified by both methods:
cinnamaldehyde, cinnamic acid, and benzyl cinnamate. The sub-
stances identified by the two methods did not, therefore, fully
match, which might be because volatile substances with low polarity
did not fully ionized in the ESI, which hindered their detection in
the LC-MS system (Vaiano, Mari, Busardo, & Bertol, 2014). Another
possible reason for this phenomenon is that high boiling point sub-
stances were not fully volatilized in the GC.

The oxidative stability of the CEO was monitored using HPLC com-
bined with fluorescent detection (Figure 5). The overall fluorescence
intensity, as well the number of different fluorescent substances
generated, increased as the storage time and temperature increased.
As expected, the fluorescent substances present in the free and mi-
croencapsulated CEO were the same before storage. However, they
were different after storage. In particular, the fluorescence intensity
of the free CEO was appreciably higher than that of the encapsu-
lated CEO stored under similar conditions, indicating that microen-
capsulation protected the CEO during storage.
3.4.4 | Possible oxidation pathway
Our results indicate that the CEO chemically degraded during stor-
age at elevated temperatures, no matter it was microencapsulated or
not. Therefore, the possible oxidation pathway should be analyzed
for exploring a way to inhibit the oxidation reactions in future.
Previously, it has been reported that fatty acids, alkanes, ter-
penes, and phenols can generate free radicals in the presence of
light, heat, or oxygen, which promote oxidation of essential oils

F I G U R E 5   (a) Free cinnamon essential oil (CEO) stored at 50°C for 1 day, (b) CEO stored at 50°C for 1 month, (c) microencapsulated
CEO stored at 50°C for 1 day and (d) microencapsulated CEO stored at 50°C for 1 month were analyzed by high-performance liquid
chromatography (HPLC) with Fluorescence Detection (FLD)
HU et al. |
      11 of 15

TA B L E 6   Partial ingredient identification of CEO from UPLC-ESI-QTOF-MS/MS

No. of Molecular [M-H]+

peak Compound formula (m/z) fragment ions (m/z) Molecular structure

2 Styrylglyoxal C10H8O2 161.0584 133.0682, 115.0533, 105.0325, 103.0534,

77.0378

3 Benzylideneacetone C10H10O 147.0425 131.04, 103.05, 77.03

4 Cinnamic acid C 9 H 8 O2 149.0582 131.04, 103.05, 77.0379, 51.02

6 Cinnamaldehyde C 9H 8 O 133.0682 115.0538, 105.06, 103.05, 91.05, 89.03,

79.03, 77.03, 65.03, 55.01

7 2-Naphthyl benzoate C17H12O2 249.0889 231.0891, 115.0531, 105.0321, 77.0375

8 Peroxycinnamic C18H14O2 295.0940 131.0475, 103.0527

anhydride

14 Benzyl cinnamate C16H14O2 239.1098 221.0943, 202.0753, 193.0989, 178.0753,

161.0579, 133.0634, 115.0526,
105.0320, 91.0526, 77.0371

18 Trans,trans- C17H14O 235.1098 215.0832, 202.0755, 157.0633, 128.0600,

dibenzylideneacetone 115.0524, 105.0317, 91.0525, 77.0370,
65.0379

19 2,3-Diphenyl-2- C18H16O 249.1252 215.0835, 128.0602, 115.0526, 105.0315,

cyclohexene-1-ketone 91.0526, 77.0375, 65.0379

Abbreviations: CEO, cinnamon essential oil; ESI, electrospray ionization source.

F I G U R E 6   Ultra-efficient liquid mass flow chart of cinnamon essential oil (CEO) under accelerated oxidation for 1 month
12 of 15      |
(Choe & Min, 2006; Turek & Stintzing, 2013). Aromatics, aldehydes
and ketones can also generate free radicals in the presence of heat
or light, which can promote oxidation of oils in the presence of oxy-
gen (Clinton, Kenley, & Traylor, 1975; Gould, Baretz, & Turro, 1987;
Loury, 1972; Zaikov, Howard, & Ingold, 1969). Based on these re-
actions, a potential oxidation pathway of CEO was postulated
(Figure 8).
Cinnamaldehyde and acetophenone (the main components in
CEO (Li et al., 2013)) are believed to be key players in the oxidation
pathways. Previously, it has been postulated that peroxycinnamic
anhydride is one of the reaction products formed during oxidation
TA B L E 7   Partial ingredient identification of CEO from GS-MS
Retention time Compound Qual
a Peroxycinnamic acid 4 might decomposed into hydroxyl radical, rad-
5.688 Benzaldehyde   96%
11.565 Cinnamaldehydea  97%
14.162 Cinnamic acida  97%
22.070 Quinolineb  91%
23.154 Benzyl cinnamatea  99%
24.218 1,4-Diphenyl-1,4-butanedioneb  90%
24.350 Benzocyclobuteneb  59%
Abbreviation: CEO, cinnamon essential oil.
a
Compounds were identified by being compared with retention time
and results of GC-MS of standards.
b
Compounds were identified according to database.
F I G U R E 7   GC-MS chromatogram of cinnamon essential oil (CEO) under accelerated oxidation for 1 month
HU et al.
of cinnamon oil (Clinton et al., 1975). Initiated by heat or light, the
cinnamaldehyde decomposes into radical 1 and peroxyl radicals 2 in
the presence of oxygen. Two molecules of peroxyl radicals 2 turned
into two molecules of radical 8 with release of one molecule of oxy-
gen. The radical 8 were so unstable that they bond with themselves
to form peroxycinnamic anhydride or continued to break down
into radical 5 (Clinton et al., 1975). Peroxyl radicals 2 could capture
the hydrogen of cinnamaldehyde as described previously (Zaikov
et al., 1969), resulting in the formation of peroxycinnamic acid 4 and
radical 3. The formation of trans,trans-dibenzylideneacetone resulted
from the binding of radical 3 and radical 5. A disproportionation re-
action could happen between peroxycinnamic acid and cinnamalde-
hyde and generate cinnamic acid. It has been postulated that there are
also other possible ways for peroxyacid to be cleaved (Loury, 1972).
ical 5 and carbon dioxide. Phenylacetaldehyde was generated after
the binding of hydroxyl radical and radical 5, which was followed by
a keto-enol tautomerism. The mechanism responsible for phenylac-
etaldehyde turning into radical 7 can be attributed to the following
pathway: cinnamaldehyde-radical 1—peroxyl radical 2—radical 8—
radical 5. Radical 7 and radical 8 bound with each other, which was
followed by the generation of benzyl cinnamate. Phenylacetaldehyde
could also decompose into radical 7 and radical 9. The formation of
styrylglyoxal was based on the combination of radical 9 and radical 1.
Acetophenone could be decomposed into radical 10 and methyl
radical (Glazebrook & Pearson, 1939). The methyl radical bound with
HU et al.
F I G U R E 8   Possible oxidation pathways of cinnamon essential oil (CEO) during storage
radical 1, which resulted in the formation of benzylideneacetone.
Radical 10 could attack acetophenone and become benzaldehyde
(Heller & Gordon, 1956), with radical 11 also forming. The genera-
tion of 1,4-diphenyl-1,4-butanedione was attributed to the binding
of radicals 11.
4 | CO N C LU S I O N
This study examined the impact of wall material composition on
the microencapsulation of CEO by spray drying. The WPI-to-
maltodextrin ratio had to be optimized to create microcapsules
with good particle and encapsulation characteristics. The addition
of sodium alginate improved the properties of the CEO microcap-
sules. For this reason, an optimized mixture of WPI, maltodextrin,
and sodium alginate was identified as a good wall material for micro-
encapsulation of CEO. The optimized formulation (including mixed
emulsifiers) led to a high EE (>93%) and high retention (>95%) of
the CEO during storage at 25°C. In particular, the predicted shelf
life of microcapsules was 1,032 days at 25°C, which demonstrated
the strong protection the optimized formulation could provide dur-
ing storage. In summary, the wall material formulation developed in
this study may be useful for the encapsulation and protection of es-
sential oils in powdered form.
AC K N OW L E D G M E N T S
This work was supported by the National Natural Science Foundation
of China (31872890), and the State Key Laboratory of Food Science
and Technology (SKLF-ZZA-201910).
|
      13 of 15
C O N FL I C T O F I N T E R E S T
The authors have declared no conflicts of interest for this article.
AU T H O R C O N T R I B U T I O N S
Qirui Hu has made substantial contributions to analysis and interpre-
tation of data and was involved in drafting the manuscript. Xia Li and
Renkou Wan have made substantial contributions to conception and
design, and acquisition data. Zeyuan Deng has made contributions
to conception and design of the study and was involved in revising
manuscript critically for important intellectual content. Fang Chen,
Cheng-wei Yu, Jing Li and David Julian McClements were all involved
in revising manuscript critically for important intellectual content.
ORCID
Cheng-Wei Yu  https://orcid.org/0000-0001-5337-9200
Jing Li  https://orcid.org/0000-0002-2271-7761
Zeyuan Deng  https://orcid.org/0000-0001-5650-1507
REFERENCES
Ackermann, L., Aalto-korte, K., Jolanki, R., & Alanko, K. (2009).
Occupational allergic contact dermatitis from cinnamon including
one case from airborne exposure. Contact Dermatitis, 60, 96–99.
https://doi.org/10.1111/j.1600-0536.2008.01486.x
Aguiar, A. C. D., Silva, L. P. S., Rezende, C. A. D., Barbero, G. F., & Martínez,
J. (2016). Encapsulation of pepper oleoresin by supercritical fluid ex-
traction of emulsions. The Journal of Supercritical Fluids, 112, 37–43.
https://doi.org/10.1016/j.supflu.2016.02.009
Bae, E. K., & Lee, S. J. (2008). Microencapsulation of avocado oil by
spray drying using whey protein and maltodextrin. Journal of
Microencapsulation, 25(8), 549–560. https://doi.org/10.1080/02652​
04080​2075682
 |
14 of 15       HU et al.
Belscak-Cvitanovic, A., Komes, D., Karlovic, S., Djakovic, S., Spoljaric,
I., Mrsic, G., & Jezˇek, D. (2015). Improving the controlled delivery
formulations of caffeine in alginate hydrogel beads combined with
pectin, carrageenan, chitosan and psyllium. Food Chemistry, 167,
378–386. https://doi.org/10.1016/j.foodc​hem.2014.07.011
Cano-Sarmiento, C., Téllez-Medina, D. I., Viveros-Contreras, R., Cornejo-
Mazón, M., Figueroa-Hernández, C. Y., García-Armenta, E., …
Gutiérrez-López, G. F. (2018). Zeta potential of food matrices. Food
Engineering Reviews, 10(3), 113–138. https://doi.org/10.1007/s1239​
3-018-9176-z
Choe, E., & Min, D. B. (2006). Mechanisms and factors for edible oil ox-
idation. Comprehensive Reviews in Food Science and Food Safety, 5(4),
169–186. https://doi.org/10.1111/j.1541-4337.2006.00009.x
Clinton, N. A., Kenley, R. A., & Traylor, T. G. (1975). Acetaldehyde autox-
idation. I. Products of termination. Journal of the American Chemical
Society, 97(13), 3746–3751. https://doi.org/10.1021/ja008​46a031
Dantas, D., Pasquali, M. A., Cavalcanti-Mata, M., Duarte, M. E., & Lisboa,
H. M. (2018). Influence of spray drying conditions on the properties
of avocado powder drink. Food Chemistry, 266, 284–291. https://doi.
org/10.1016/j.foodc​hem.2018.06.016
Darniadi, S., Ho, P., & Murray, B. S. (2018). Comparison of blueberry
powder produced via foam-mat freeze-drying versus spray-drying:
Evaluation of foam and powder properties. Journal of the Science of
Food and Agriculture, 98(5), 2002–2010. https://doi.org/10.1002/
jsfa.8685
Encina, C., Vergara, C., Giménez, B., Oyarzún-Ampuero, F., & Robert, P.
(2016). Conventional spray-drying and future trends for the microen-
capsulation of fish oil. Trends in Food Science & Technology, 56, 46–60.
https://doi.org/10.1016/j.tifs.2016.07.014
Gharsallaoui, A., Roudaut, G., Chambin, O., Voilley, A., & Saurel, R. (2007).
Applications of spray-drying in microencapsulation of food ingredi-
ents: An overview. Food Research International, 40(9), 1107–1121.
https://doi.org/10.1016/j.foodr​es.2007.07.004
Glazebrook, H. H., & Pearson, T. G. (1939). The photochemical decom-
position of aromatic ketones: The phenyl radical. Journal of the
Chemical Society, 1939, 589–593. https://doi.org/10.1039/jr939​
0000589
Goñi, P., López, P., Sánchez, C., Gómez-Lus, R., Becerril, R., & Nerín, C.
(2009). Antimicrobial activity in the vapour phase of a combination of
cinnamon and clove essential oils. Food Chemistry, 116(4), 982–989.
https://doi.org/10.1016/j.foodc​hem.2009.03.058
Gould, I. R., Baretz, B. H., & Turro, N. J. (1987). Primary processes in the
type I photocleavage of dibenzyl ketones. A pulsed laser and pho-
tochemically induced dynamic nuclear polarization study. Journal of
Physical Chemistry, 91(4), 925–929. https://doi.org/10.1021/j1002​
88a032
Heller, C. A., & Gordon, A. S. (1956). Isopropyl radical reactions. I.
Photolysis of diisopropyl ketone. Journal of Physical Chemistry, 60,
1315–1318. https://doi.org/10.1021/j1505​6 4a019
Hermanto, R. F., Khasanah, L. U., Kawiji, W. A., Manuhara, G. J., &
Utami, R. (2016). Physical characteristics of cinnamon oil microcap-
sule. IOP Conference Series: Materials Science and Engineering,107,
012064.https://doi.org/10.1088/1757-899x/107/1/012064
Hu, Y., Liu, C., Hao, Q., Zhang, Q., & He, Y. (2013). Building kinetic models
for determining vitamin C content in fresh jujube and predicting its
shelf life based on near-infrared spectroscopy. Sensors (Basel), 13(11),
15673–15681. https://doi.org/10.3390/s1311​15673
Ixtaina, V. Y., Julio, L. M., Wagner, J. R., Nolasco, S. M., & Tomás, M. C.
(2015). Physicochemical characterization and stability of chia oil
microencapsulated with sodium caseinate and lactose by spray-dry-
ing. Powder Technology, 271, 26–34. https://doi.org/10.1016/j.
powtec.2014.11.006
Koç, M., Güngör, Ö., Zungur, A., Yalçın, B., Selek, İ., Ertek, F. K., & Ötles,
S. (2015). Microencapsulation of extra virgin olive oil by spray dry-
ing: Effect of wall materials composition, process conditions, and
emulsification method. Food and Bioprocess Technology, 8(2), 301–
318. https://doi.org/10.1007/s1194​7-014-1404-9
Labuschagne, P. (2018). Impact of wall material physicochemical charac-
teristics on the stability of encapsulated phytochemicals: A review.
Food Research International, 107, 227–247. https://doi.org/10.1016/j.
foodr​es.2018.02.026
Lam, R. S. H., & Nickerson, M. T. (2013). Food proteins: A review on
their emulsifying properties using a structure–function approach.
Food Chemistry, 141(2), 975–984. https://doi.org/10.1016/j.foodc​
hem.2013.04.038
Lević, S., Pajić Lijaković, I., Đorđević, V., Rac, V., Rakić, V., Šolević
Knudsen, T., … Nedović, V. (2015). Characterization of sodium algi-
nate/d-limonene emulsions and respective calcium alginate/d-limo-
nene beads produced by electrostatic extrusion. Food Hydrocolloids,
45, 111–123. https://doi.org/10.1016/j.foodh​yd.2014.10.001
Li, Y.-Q., Kong, D.-X., & Wu, H. (2013). Analysis and evaluation of es-
sential oil components of cinnamon barks using GC–MS and FTIR
spectroscopy. Industrial Crops and Products, 41, 269–278. https://doi.
org/10.1016/j.indcr​op.2012.04.056
Liu, T. T., & Yang, T. S. (2011). Optimization of emulsification and microen-
capsulation of evening primrose oil and its oxidative stability during
storage by response surface methodology. Journal of Food Quality,
34(1), 64–73. https://doi.org/10.1111/j.1745-4557.2010.00358.x
Loury, M. (1972). Possible mechanisms of autoxidative rancidity. Lipids,
7(10), 671–675. https://doi.org/10.1007/BF025​33075
Lu, W., Kelly, A. L., & Miao, S. (2017). Improved bioavailability of encap-
sulated bioactive nutrients delivered through monoglyceride-struc-
tured O/W emulsions. Journal of Agricultural and Food Chemistry,
65(14), 3048–3055. https://doi.org/10.1021/acs.jafc.6b05644
Özcan, M. M., & Arslan, D. (2011). Antioxidant effect of essential oils
of rosemary, clove and cinnamon on hazelnut and poppy oils.
Food Chemistry, 129(1), 171–174. https://doi.org/10.1016/j.foodc​
hem.2011.01.055
Patel, A. R., Bouwens, E. C. M., & Velikov, K. P. (2010). Sodium casein-
ate stabilized zein colloidal particles. Journal of Agricultural and Food
Chemistry, 58(23), 12497–12503. https://doi.org/10.1021/jf102​959b
Perez-Masia, R., Lopez-Nicolas, R., Periago, M. J., Ros, G., Lagaron, J.
M., & Lopez-Rubio, A. (2015). Encapsulation of folic acid in food
hydrocolloids through nanospray drying and electrospraying for nu-
traceutical applications. Food Chemistry, 168, 124–133. https://doi.
org/10.1016/j.foodc​hem.2014.07.051
Pratiwi, I. Y., Darmadji, P., & Hastuti, P. (2016). Effect of Storage
Temperature on the Stability of Microencapsulated Essential Oil
from Cinnamon (Cinnamomum burmanii).1741, 130014. https://doi.
org/10.1063/1.4958558
Rao, P. V., & Gan, S. H. (2014). Cinnamon: A multifaceted medicinal
plant. Evidence-Based Complementary and Alternative Medicine, 2014,
642942. https://doi.org/10.1155/2014/642942
Salleh, S. H. A., Hamid, K. A., Bustami Effendi, T. J., & Jamil, N. (2012).
Characterization and stability evaluation of olive oil nanoemul-
sion-based hydrogel formulation by nanophase emulsification tech-
nique. Business, Engineering and Industrial Applications,824–828.
https://doi.org/10.1109/ISBEIA.2012.6423007
Shamaei, S., Seiiedlou, S. S., Aghbashlo, M., Tsotsas, E., & Kharaghani, A.
(2017). Microencapsulation of walnut oil by spray drying: Effects of
wall material and drying conditions on physicochemical properties of
microcapsules. Innovative Food Science & Emerging Technologies, 39,
101–112. https://doi.org/10.1016/j.ifset.2016.11.011
Sheu, T.-Y., & Rosenberg, M. (1998). Microstructure of microcapsules
consisting of whey proteins and carbohydrates. Journal of Food
Science, 63(3), 491–494. https://doi.org/10.1111/j.1365-2621.1998.
tb157​70.x
Sosa, N., Schebor, C., & Pérez, O. E. (2015). Rheology and stability of
citral/sugar microemulsions. In G. F. Gutiérrez-López, L. Alamilla-
Beltrán, M. del Pilar Buera, J. Welti-Chanes, E. Parada-Arias, & G.
HU et al.
V. Barbosa-Cánovas (Eds.), Water stress in biological, chemical, phar-
maceutical and food systems (pp. 361–366). New York, NY: Springer,
New York.
Troya, D., Tupuna-Yerovi, D. S., & Ruales, J. (2018). Effects of wall ma-
terials and operating parameters on physicochemical properties,
process efficiency, and total carotenoid content of microencapsu-
lated banana passionfruit pulp (Passiflora tripartita var. mollissima)
by spray-drying. Food and Bioprocess Technology, 11(10), 1828–1839.
https://doi.org/10.1007/s1194​7-018-2143-0
Tung, Y. T., Chua, M. T., Wang, S. Y., & Chang, S. T. (2008). Anti-inflammation
activities of essential oil and its constituents from indigenous cin-
namon (Cinnamomum osmophloeum) twigs. Bioresource Technology,
99(9), 3908–3913. https://doi.org/10.1016/j.biort​ech.2007.07.050
Turek, C., & Stintzing, F. C. (2013). Stability of essential oils: A review.
Comprehensive Reviews in Food Science and Food Safety, 12(1), 40–53.
https://doi.org/10.1111/1541-4337.12006
Vaiano, F., Mari, F., Busardo, F. P., & Bertol, E. (2014). Enhancing the sen-
sitivity of the LC-MS/MS detection of propofol in urine and blood
by azo-coupling derivatization. Analytical and Bioanalytical Chemistry,
406(15), 3579–3587. https://doi.org/10.1007/s0021​6-013-7573-y
Wang, B., Vongsvivut, J., Adhikari, B., & Barrow, C. J. (2015).
Microencapsulation of tuna oil fortified with the multiple lipophilic in-
gredients vitamins A, D3, E, K2, curcumin and coenzyme Q10. Journal of
Functional Foods, 19, 893–901. https://doi.org/10.1016/j.jff.2015.03.027
Yang, X.-Q., Zheng, H., Ye, Q., Li, R.-Y., & Chen, Y. (2016). Essential oil of
Cinnamon exerts anti-cancer activity against head and neck squa-
mous cell carcinoma via attenuating epidermal growth factor recep-
tor-tyrosine kinase. Journal of BUON, 20(6), 1518–1525.
Yoo, S.-H., Song, Y.-B., Chang, P.-S., & Lee, H. G. (2006). Microencapsulation
of α-tocopherol using sodium alginate and its controlled release
properties. International Journal of Biological Macromolecules, 38(1),
25–30. https://doi.org/10.1016/j.ijbio​mac.2005.12.013
|
      15 of 15
Zaikov, G. E., Howard, J. A., & Ingold, K. U. (1969). Absolute rate constants
for hydrocarbon autoxidation. XIII. Aldehydes: Photo-oxidation,
co-oxidation, and inhibition. Canadian Journal of Chemistry, 47(16),
3017–3029. https://doi.org/10.1139/v67-131
Zhang, Y., Liu, X., Wang, Y., Jiang, P., & Quek, S. (2016). Antibacterial ac-
tivity and mechanism of cinnamon essential oil against Escherichia
coli and Staphylococcus aureus. Food Control, 59, 282–289. https://
doi.org/10.1016/j.foodc​ont.2015.05.032
Zhao, Q., Liu, D., Long, Z., Yang, B., Fang, M., Kuang, W., & Zhao, M.
(2014). Effect of sucrose ester concentration on the interfacial char-
acteristics and physical properties of sodium caseinate-stabilized
oil-in-water emulsions. Food Chemistry, 151, 506–513. https://doi.
org/10.1016/j.foodc​hem.2013.11.113
Zuidam, N. J., & Shimoni, E. (2010). Overview of microencapsulates for
use in food products or processes and methods to make them. In N.
Zuidam, & V. Nedovig (Eds.), Encapsulation technologies for active food
ingredients and food processing (pp. 3–29). New York, NY: Springer.
S U P P O R T I N G I N FO R M AT I O N
Additional supporting information may be found online in the
Supporting Information section.
How to cite this article: Hu Q, Li X, Chen F, et al.
Microencapsulation of an essential oil (cinnamon oil) by spray
drying: Effects of wall materials and storage conditions on
microcapsule properties. J Food Process Preserv.
2020;00:e14805. https://doi.org/10.1111/jfpp.14805