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Fabrication of biopolymer stabilized microcapsules for enhancing

physicochemical stability, antioxidant and antimicrobial
properties of cinnamon essential oil

Sulafa B.H. Hashim, Haroon Elrasheid Tahir, Amer Ali Mahdi,

Qais Ali Al-Maqtari, Mohammad Rezaul Islam Shishir, Gustav
Komla Mahunu, Halah Aalim, Suliman Khan, Xiaodong Zhai,
Zou Xiaobo, Shi Jiyong

PII: S0141-8130(24)03141-6
DOI: https://doi.org/10.1016/j.ijbiomac.2024.132336
Reference: BIOMAC 132336

To appear in: International Journal of Biological Macromolecules

Received date: 2 January 2024

Revised date: 9 May 2024
Accepted date: 11 May 2024

Please cite this article as: S.B.H. Hashim, H.E. Tahir, A.A. Mahdi, et al., Fabrication of
biopolymer stabilized microcapsules for enhancing physicochemical stability, antioxidant
and antimicrobial properties of cinnamon essential oil, International Journal of Biological
Macromolecules (2024), https://doi.org/10.1016/j.ijbiomac.2024.132336

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© 2024 Published by Elsevier B.V.

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Fabrication of biopolymer stabilized microcapsules for enhancing

physicochemical stability, antioxidant and antimicrobial properties of

cinnamon essential oil

Sulafa B.H. Hashima,b,1*, Haroon Elrasheid Tahira,1, Amer Ali Mahdic, Qais Ali Al-Maqtarid,

Mohammad Rezaul Islam Shishira, Gustav Komla Mahunue, Halah Aalima, Suliman Khana,

Xiaodong Zhaia, Zou Xiaoboa,*, Shi Jiyonga,*

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aSchool of Food and Biological Engineering, Jiangsu University, 301 Xuefu Rd., 212013

Zhenjiang, Jiangsu, China

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bDepartment of Food Technology, Faculty of Agricultural Technology and Fish Sciences,

Alneelain University, Khartoum, Sudan -p

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cDepartment of Food Science and Nutrition, Faculty of Agriculture, Food, and Environment,
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Sana'a University, Sana'a, Yemen.

dMicro-Pollutant Research Centre (MPRC), Institute of Integrated Engineering, Universiti Tun
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Hussein Onn Malaysia (UTHM), 86400, Parit Raja, Batu Pahat, Johor, Malaysia.
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e
Department of Food Science & Technology, Faculty of Agriculture, Food and Consumer Sciences,

University for Development Studies, Tamale, Ghana

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*Corresponding author. Tel: +86 511 88780174; Fax: +86 511 88780201

Email address: [email protected] (Zou Xiaobo); [email protected] (Shi Jiyong);

[email protected] (Sulafa B.H. Hashim)

1
These authors contributed equally.

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Abstract

The current study entails the encapsulation validity to enclose naturally occurring food

preservatives, such as cinnamon essential oil (CM), within various wall materials. This approach

has demonstrated enhanced encapsulated compounds' stability, efficiency, and bioactivity. The

base carrier system consisted of a solid lipid (Berry wax, RW) individually blended with whey

protein (WYN), maltodextrin (MDN), and gum Arabic (GMC) as wall materials. The resulting

formulations were freeze-dried: WYN/RW/CM, MDN/RW/CM, and GMC/RW/CM. The study

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comprehensively analyzed encapsulation efficiency, morphology, crystallinity, thermal, and

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physiochemical properties. When RW was combined with WYN, MDN, and GMC, the

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microcapsule WYN/RW/CM showed the highest efficiency at 93.4%, while the GMC/RW/CM

exhibited the highest relative crystallinity at 46.54%. Furthermore, the investigation assessed
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storage stability, release of bioactive compounds, and oxidative stability during storage at 4°C/ 25%
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RH ± 5% and 25°C/40% RH ± 5% for 55 days, revealing optimal stability in the WYN/RW/CM

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microcapsule. Additionally, the antimicrobial activity was assessed at various concentrations of

microcapsules, revealing their inhibitory effect against Escherichia coli (gram-negative) and
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Staphylococcus aureus (gram-positive) bacteria. The WYN/RW/CM microcapsule exhibited the

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highest inhibition activity in both strains, reaching 40mm. This study demonstrates that combining

WYN with RW as a wall material has greater efficiency in encapsulation and potential uses in

various industrial sectors.

Keywords: Cinnamon essential oil; Berry wax; microcapsules; Total phenolic content; Oxidative

stability; Antibacterial activity.

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1. Introduction

Cinnamon essential oil (CM) is derived from various parts of Cinnamon cassia, with its

primary active components being cinnamaldehyde and eugenol [1]. Renowned for its broad-

spectrum antibacterial, antioxidant, and medicinal properties, cinnamon essential oil possesses a

distinctive aroma; however, its susceptibility to oxidation, degradation, volatilization, and

insolubility in water has limited its application as a preservative in the therapeutic and food sectors

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[2,3]. Certainly, employing nanoemulsions to enhance the protection and availability of cinnamon

essential oil is a promising technological strategy [4]. Nanoemulsions are created by converting

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larger emulsion droplets into nano-droplets across different phases to enhance physicochemical

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and sensory characteristics. However, there are limitations in the control of bioactivity and short-
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term stability in their free nanoemulsions [5]. To tackle these challenges, encapsulated
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technological approaches following the dry powder form are required to protect and ensure the

targeted delivery of these bioactive compounds at a specific rate, with a longer shelf life than liquid
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formulations, enhanced solubility, ease of handling and transportation, and adaptability with
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diverse applications [6,7].

Encapsulation is a technique used to protect core components, such as active compounds in

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essential oils, by entrapping them within capsules or gel matrices made of one or more types of

wall materials and changing them to a solid particle state through freeze-drying [7,8]. Several

factors influence encapsulation properties for sensitive bioactive compounds, including selecting

an appropriate encapsulation strategy, the structural characteristics, and the chemical composition

of the shell material (such as proteins, polysaccharides, and lipids). This process enhances the

longevity of the carrier product/matrix, ensuring the stability and efficacy of the encapsulation of

the core material compounds when they are released into the food matrix [6,9]. Lipid-based

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systems, particularly lipid carriers (solid lipid with liquid lipid), have significant advantages in

various delivery methods, resulting in better physicochemical properties, functions, stabilization

strategies, and controlled release upon encapsulation of active components [10–12]. However, it

is essential to note that these systems may exhibit lower solubility in hydrophilic materials. Due

to the challenges related to lipid carrier solubility and other properties, considerable research has

been conducted into developing a new encapsulated material. This investigation entails using lipids

sourced from natural origins as the solid lipid element, which are then blended with established

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wall materials like maltodextrins (MDN), gum Arabic (GMC), and whey protein (WYN). The

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objective is to boost powder recovery, leverage electrostatic attraction, and enhance stability,

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thereby preserving the time-sensitive quality of the active ingredients.
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Natural waxes are solid lipids with varying chemical compositions and are highly crystallized

[13]. The mature fruit of berries yields Berry wax (RW), which has a whitish appearance. Its
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composition is diverse, encompassing triterpenoids, alkanes, fatty acids, aldehydes, primary

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alcohols, and ketones. The RW production range of these compounds is observed to be within the

range of 108.5–871.1 µg/cm2, a variation attributed to geographical and environmental factors.

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Berry waxes are known for their physiological effects, including UV-B protection provided by
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phenolic acids and triterpenoids that absorb UV-B light [14,15]. Maltodextrin (MDN), derived

from the partial breakdown of starch, possesses various unique qualities, such as excellent

solubility and low viscosity. However, its slightly diminished emulsifying ability necessitates

combining with other materials to enhance its properties [16]. On the other hand, gum Arabic

(GMC) exhibits reasonable emulsifying properties and provides acceptable protective effects.

Nevertheless, its viscosity becomes a limiting factor at high concentrations, restricting its industrial

applications and making it highly cost-effective [17,18]. Whey Protein Isolate (WYN) is a primary

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byproduct derived from the dairy industry, characterized by its distinctive emulsion properties

attributed to hydrophilic and hydrophobic amino acid constituents. This unique composition makes

WYN an excellent candidate for optimal shell wall materials, particularly for hydrophobic

substances. Nevertheless, the food manufacturing sector faces a substantial need for high powder

recovery and the preservation of encapsulated materials [19,20].

This study aimed to assess the process of producing encapsulated cinnamon essential oil by

utilizing berry wax in combination with WYN, MDN, and GMC as wall matrix materials. To the

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best of our knowledge, this specific approach has not been explored previously. Consequently, the

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evaluation considered their physical, morphological, and thermal characteristics. Moreover, the

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study will examine the encapsulation's durability during storage, assess its potential to inhibit
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bacterial growth during storage, and evaluate its potential to inhibit bacterial growth to offer a

comprehensive characterization of the developed encapsulation.

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2. Materials and Methods

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2.1. Materials
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The berry wax was purchased from Union Chemical Ind. Co., Ltd. Shanghai, China.

Cinnamon essential oil (CM), GMC (molecular weight of 406.44 kDa and a viscosity of 0.024
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Pa.s.), and ethanol were acquired from Sinopharm Chemical Reagent Co., Ltd. in Shanghai, China.

MDN (molecular weight: 4.34 kDa, viscosity: 0.003 Pa.s.) and WYN (molecular weight: 40.64

kDa, viscosity: 0.006 Pa.s.) were obtained from Shyuanye Co., Ltd. in Shanghai, China.

Escherichia coli (ATCC 11229) and Staphylococcus aureus (ATCC 6538) were acquired from the

Shanghai Bioresource Collection Centre. Plastic Petri dishes were acquired from Sigma Chemical

Co., St. Louis, MO, USA. Trypticase soy broth and Mueller Hinton Agar plates were acquired

from Guangdong Huankai Microbial Science & Technology Co. Ltd.

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2.2. Preparation of Emulsion

The emulsions were fabricated using a two-step process [11] with some modifications

(Table 1). The aqueous phases were prepared by separately dissolving the polymers (WYN, MDN,

and GMC) in distilled water at 1:2 (w/v). This mixture was continuously stirred overnight at 25°C

to ensure complete hydration. Subsequently, the aqueous phases were homogenized for 15 minutes

at 10,000 rpm (Ultra-Turrax IKA T18, USA). Next, the lipid phase (RW and sunflower oil) with

emulsifier tween 80 (20%) was combined and blended at 70°C until complete dissolution. Then,

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the lipid phases were gradually introduced into the aqueous phases and subjected to mixing using

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a high-speed homogenizer at 10,000 rpm for 15 minutes. The CM essential oil droplets were

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incrementally added to the emulsion mixture and blended for 10 min using the identical high-speed
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homogenizer. Upon completion of the addition process, the emulsions were sonicated at 200w for

5min to obtain homogeneous dispersions. The resultant emulsions were kept at 4 °C until further
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testing and coded as follows: WYN/RW/CM, MDN/RW/CM, and GMC/RW/CM.

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2.2.1. Characterization of emulsions

The dynamic light scattering spectroscopy apparatus was carried out using a particle size
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analyzer (Litesizer 500 Nano-ZS, Model BM10) to determine the droplet size (DS), polydispersity
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index (PDI), and zeta potential (ζ-potential) of CM emulsions.

2.3. Freeze Drying of nanoemulsions

The freeze-drying process transformed the nanoemulsions into dried microcapsules. The

nanoemulsions were frozen at -18 °C for 48 hours. Subsequently, the frozen emulsions were

freeze-dried (48 h). The microcapsules were then packed in airtight, opaque flacon tubes and stored

at 4 °C for further analysis.

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2.4. Properties of CM microcapsules

2.4.1. Encapsulation Efficiency (EE)

The EE of CM microcapsules was conducted using Folin-Ciocalteu's assay [21]. The EE

was estimated based on the total phenolic content on the surface and the total oils contained within

the microcapsules in equation (1).

EE (%) = [(TPCa - TPCb) / TPCb] х 100 (1)

Where TPCa is the total surface phenolic content, and TPCb is the total phenolic content of the

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microcapsules

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2.4.2. Moisture content, Water activity, Hygroscopicity, Solubility, and Wettability

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The moisture content of the different microcapsules was evaluated by subjecting them to drying

techniques until a consistent weight was achieved in an oven set at a temperature of 105 °C [22].
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The water activity was determined at 25 °C using an electronic water activity meter [23]. In
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contrast, the solubility percentage was measured following the published procedure of Karrar et
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al. [20]. Initially, 2 g of microcapsules were added to 50 mL of deionized water, followed by

agitation at a rate of 500 rpm for 4 h. Subsequently, the mixture was centrifuged (3000 rpm for 6
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min), and the resulting supernatant was transferred entirely to a crucible for oven drying at 105 °C
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overnight, and the percentage solubility calculated. The hygroscopicity percentage of the

microcapsules was measured after a 7-day storage period at a relative humidity of 75% using a

saturated sodium chloride solution [24]. The wettability measurement determined the duration

(min) needed to submerge 1 g of a substance in 400 mL of distilled water at 25 °C [25].

2.4.3. Bulk, Tapped, and Particle Density

CM microcapsules' bulk, tapped, and particle densities were determined following the

methodology described by Mohammed et al. [22].

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2.4.4. Cohesiveness and Flowability

Flowability and cohesiveness were evaluated based on the microcapsules' bulk and tapping

densities. The calculation of Carr's index (CI) was employed to quantify the flowability, while the

Hausner ratio (HR) was utilized to assess its cohesiveness, as designated by Karrar et al. [20].

2.4.5. Color

The color (lightness, L*), (redness, a*), and (yellowness, b*) characteristics of

microcapsules were measured using a colorimetric spectrophotometer (Konica Minolta Holding,

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CM2300d, Inc., Japan) as previously described [26].

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2.4.6. Thermal properties of microcapsules

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The thermal analysis of the microcapsules was conducted using a thermogravimetric analyzer
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(TGA, NETZSCH STA 449F3 model) and differential scanning calorimetry (DSC, Universal v3-

9ATA Instrument, New Castle, USA). The analysis was performed carried out at temperatures
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ranging from 50°C to 400°C, with a heating rate of 10°C/min and a nitrogen flow rate of 50
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mL/min, as previously reported [24].

2.4.7. X-ray Diffraction (XRD)

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The crystallinity of the microcapsules was assessed using an X-ray diffractometer (D2
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PHASER, Bruker AXS Co., Ltd., Germany) with scanning angles ranging from 5◦ to 80◦. The X-

ray diffraction patterns were measured using the MDI Jade 6 program, and the relative crystallinity

(%) was determined according to Al-Maqtari et al. [23].

2.4.8. Scanning Electron Microscopy (SEM)

The morphology of the microcapsules was examined using a scanning electron microscope (S-

4800, Hitachi High Technologies Corporation, Japan). The microcapsules were affixed to stubs

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using double-sided tape, followed by a thin coating of gold deposition under vacuum conditions.

A 15 kV accelerating beam then scanned the microcapsules [27].

2.4.9. Fourier transforms infrared spectroscopy (FTIR)

The FTIR spectrophotometer utilized to ascertain the chemical structures of the microcapsules

was a Nicoletis 50 Perkin Elmer 16 PC spectrometer manufactured in Boston, USA. Transmission

spectrum mode was detected at wavelengths ranging from 500 to 4000 cm-1 with a resolution of 4

cm-1 and 32 scans.

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2.4.10. Storage stability of microcapsules

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The microcapsules were subjected to storage conditions at 4 °C and 25 °C at 25% ± 5% and

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50% ± 5% relative humidity (RH), respectively, for 55 days. At 5-day intervals, the microcapsules
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(1:10 w/v) were dissolved in distillation water and analyzed to determine their stability in terms of

release rate, antioxidant activity %, and total phenolic content. Additionally, the oxidative stability
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of the stored microcapsules was evaluated by determining the peroxide value over the storage
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period.

2.4.10.1. Release of Total Phenolic Content (TPC)

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The TPC of microcapsules was calculated by Al-Maqtari et al. [23]. The findings are presented
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as milligrams of gallic acid equivalents per gram (mg GAE g-1) based on the linear equation gallic

acid y = 0.0063x + 0.0448 (R2 = 0.9981).

2.4.10.2. Release of Antioxidant Activity

The microcapsule samples' DPPH free radical scavenging capacity was assessed using the

method described by Mahdi et al. [28]. In brief, 3.5 mL of DPPH in a methanol solution (60 μM)

was combined with a suspension of microcapsules (50 μL) and an incubation period of 30 min.

The absorbance of the mixture was measured at a wavelength of 517 nm. The result was then

expressed as an inhibition percentage in equation (2).

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DPPH (%) = [(A0-A1) /A0] х 100 (2)

Where A0 is the control absorbance, and A1 is the sample absorbance.

2.4.10.3. Oxidative stability

The peroxide value of microcapsules was evaluated using the oxidative stability test. The

amounts of lipid hydroperoxides were measured following the technique reported [23]. The final

combination was kept at room temperature for 20 min in the dark, and the absorbance of the

samples was measured at 510 nm.

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2.5. Antibacterial Activity Test

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The disk diffusion method was employed to assess the antibacterial efficacy of the

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microcapsules [29] with minor modifications. The antibacterial activity of encapsulates against
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gram-negative Escherichia coli and gram-positive Staphylococcus aureus was tested. Individually,

a 0.5 McFarland standard for each bacterium was prepared and then inoculated onto plates
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containing Mueller-Hinton agar. Using a cork borer, wells with a diameter of 6 mm were created.
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The encapsulated substance was then diluted into three concentrations (2%, 4%, and 8%) using

sterile dimethyl-sulfoxide 10% (DMSO). Subsequently, 50 μL of each concentration of the

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encapsulated substance was dispensed into each well in triplicate. All plates were incubated at
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37 °C for 24 hours, and the width of the inhibitory zone was measured in millimeters.

2.6. Statistical analysis

The triplicate data from the findings were subjected to statistical analysis using Minitab

software (State College, Pa.). The statistical evaluation was conducted through one-way analysis

of variance (ANOVA) to determine significant differences, considering a significance level of p ≤

0.05.

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3. Results and discussion

3.1. Droplet size, polydispersity index, and ζ-potential of the emulsions

The critical parameters utilized to assess the efficacy of the emulsions in encapsulation

were indicated by physical stability measurements [droplet size diameter (DS), polydispersity

index (PDI), and zeta potential (ζ-potential)], as detailed in Table 2. Results showed that the DS

of nanoemulsions ranged from 265 to 456 nm, indicating that the droplets were in the nanosize

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range. Among the nanoemulsions, GMC/RW/CM had the lowest droplet size, while there was no

significant difference in DS between WYN/RW/CM and MDN/RW/CM. Similar results were

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reported by Kaliamurthi et al. [5] and Korma et al. [30]. Significant variations in PDI were

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observed among the nanoemulsions. The PDI of the various nanoemulsions followed the order
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MDN/RW/CM > WYN/RW/CM > GMC/RW/CM. This finding illustrates that particles with PDI
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values below 0.5 revealed a consistent and homogeneous distribution within the nanoemulsions.

The stability of the particles against aggregation and precipitation was quantified by the ζ-potential
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of the emulsion, which displayed greater stability values (±30) [26,31]. Nanoemulsions also
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exhibited sufficient negative surface charge, namely -34.57, -27.39, and -23.80 mV, respectively,

in WYN/RW/CM, MDN/RW/CM, and GMC/RW/CM. This indicates the presence of electrostatic

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repulsion forces in the dispersions, thus confirming their stability properties. These findings align

with those of previous studies [30,32].

3.2. Microcapsule properties

3.2.1. Encapsulation efficiency

The assessment of material and processing quality relies on encapsulation efficiency, a

pivotal metric in encapsulation research studies. Analysis of encapsulation efficiency revealed

significant variations (p ≤ 0.05) among the different microcapsules, as shown in Table 3. The

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WYN/RW/CM microcapsules exhibited the maximum EE of >93%, whereas the MDN/RW/CM

microcapsules demonstrated the lowest EE of approximately 81%. This indicates that

microcapsules, particularly WYN/RW/CM, are the most efficient in encapsulating the phenolic

compounds present in essential oil. The results were consistent with the findings of Ozdemir et al.

[33], wherein notable alterations in the EE of several microcapsule formulations were seen. The

observed enhancement in the EE of WYN/RW/CM capsules might be due to the solid molecular

interactions between the WYN/RW complex and cinnamon oil phenolics, which is corroborated

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with previous studies [30,34]. In addition, Jain et al. [35] revealed that using longer chain

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triglyceride wall material in lipid encapsulation of β‐carotene confers further benefits. The

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preservation of the core material is contingent upon the kind and quality of the wall material, with
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these factors being the most influential determinants. Furthermore, Aksoylu Özbek & Günç

Ergönül [36] confirmed whether the EE qualities of the core material increased when it was mixed
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with several wall materials.

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3.2.2. Moisture Content and Water Activity

The moisture content and water activity are the critical properties of dried microcapsules
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that significantly impact their storage stability. Lower levels of moisture content (2.0-4.0%) and
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water activity (<0.4) are recommended for industrial functional food powders to maintain the

oxidative and microbiological stability of food products [37]. According to Table 3, the various

microcapsules showed low moisture content, which ranged from 2.21% to 2.46%. The study by

Barbosa-Barbosa-Cánovas & Juliano [38] showed that the mentioned food powders fulfilled the

specified criteria. Moreover, Chew et al. [39] discovered that these food powders can be preserved

for extended storage periods. The study demonstrated that the observed values were higher than

the reported result by Fernandes et al. [40] for ginger oil microcapsules, which were within the

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range of 0.88% to 1.76%. The water activity results presented in Table 3 fell within the acceptable

range for encapsulate storage stability. Significant differences (p ≤ 0.05) were observed among the

capsules, except for the MDN/RW/CM and GMC/RW/CM capsules, which exhibited no

significant differences. Notably, the water activity results were lower than those reported [28] for

nanocapsules of various essential oils, ranging from 0.03 to 0.04. Still, they were consistent with

the findings of [39] for microcapsules of refined kenaf seed oil. Fluctuations in encapsulated

moisture content and water activity may stem from various factors, including differences in drying

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duration and techniques, as well as the chemical composition of the wall materials employed.

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Microbiological development is deemed unstable when water activity is reduced to levels below

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0.6, hence promoting physicochemical stability and enabling prolonged storage [39,41].
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3.2.3. Wettability, solubility and hygroscopicity
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The wettability of microcapsules plays a crucial role in determining the time required for

complete wetting when they are dropped into the water at a specific temperature. The wettability
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of microcapsules is presented in Table 3. The wettability of the microcapsules varied significantly,

with MDN/RW/CM demonstrating the minimum wettability time of 10.5 min, followed by
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GMC/RW/CM (12.3 min) and WYN/RW/CM (15.1 min). MDN is more likely hydrophilic, which
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could decrease the wettability of MDN/RW/CM microcapsules. In comparison, the refined kenaf

seed oil range of 6–10 min [19] and the encapsulating citrus reticulata essential oil range of 1.8–

5.08 min [24] had a minimum time wettability. The hydrophobic chain formed by whey proteins,

berry wax, and CM (hydrophobic) may produce the most prolonged wettability periods [42].

Solubility stands as a pivotal quality trait in particle dissolution, frequently employed in food

processing either as an additive or an ingredient. As evidenced in Table 3, notable disparities were

observed in the solubility values among the microcapsules. The elevated solubility was observed

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in MDN/RW/CM (82.75%) and GMC/RW/CM (78.41%), whereas WYN/RW/CM exhibits the

lowest value (72.64%). Comparatively, studies [20,39], the microcapsules of gurum seed oil

(86.61–90.90%) and refined kenaf seed oil (85.6–90.2%) were higher than the results examined in

this research.

Hygroscopicity refers to the capacity of microcapsule powder to attract and retain moisture from

the surrounding environment, forming aggregates and adhesions. In Table 3, no significant

difference (p ≤ 0.05) was observed in the hygroscopicity of GMC/RW/CM and MDN/RW/CM

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microcapsules when compared to WYN/RW/CM microcapsules, which exhibited a lower level of

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hygroscopicity. The phenomenon of moisture absorption may be ascribed to hydrogen (H2) among

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water constituents and the accessibility of hydroxyl groups found in GMC and MDN [20].
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Nevertheless, the result exhibited a wide range when compared to values (12.05%–14.42%)

reported for mandarin essential oil [24], as well as for coffee oil microcapsules (13.83%–17.73%)
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[43].
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3.2.4. Bulk, tapped, and particle density

The density characteristics of powdered microcapsules are critical physical parameters to

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consider when estimating storage packing capacity. Table 3 illustrates the bulk density values of
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CM microcapsules, revealing significant variations among them. Specifically, the WYN/RW/CM

microcapsules exhibited a higher bulk density, indicating reduced storage capacity and less air

within the powder. This characteristic plays a vital role in impeding the oxidative degradation of

lipids during prolonged storage periods. The bulk density results of MDN/RW/CM and

GMC/RW/CM are within the range (0.26-0.36 g/cm3) reported by Mahdi et al. [24] and aligned

with the findings of Fernandes et al. [40], who reported a range of 0.27-0.31 g/cm3. The tapped

density values of microcapsules manifest statistically significant differences. The WYN/RW/CM

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revealed the most remarkable value, while the GMC/RW/CM and MDN/RW/CM had the lowest

(Table 3). The observed values were consistent with the tapped densities of ginger essential oil

microcapsules (0.46-0.53 g/cm3) and citrus reticulate essential oil nanocapsules (0.43-0.54 g/cm3)

[24,40]. Similarly, WYN/RW/CM had significantly greater particle density (1.991 g/cm3)

compared to MDN/RW/CM (1.689 g/cm3) and GMC/RW/CM (1.729 g/cm3), surpassing the values

as reported [39,40]. Therefore, it was demonstrated that WYN proved to be the most efficient

polymer for improving the density properties of CM microcapsules.

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3.2.5. Flowability and cohesiveness

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Flowability and cohesiveness are critical quality criteria for assessing powders' flow

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characteristics. These metrics, namely compressibility index (CI) and Hausner ratio (HR), are
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determined based on measurements of bulk and tapped densities [23]. The CI analysis indicates

no statistically significant distinction between the GMC/RW/CM and MDN/RW/CM

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microcapsules (Table 3). Nevertheless, a range of values exists, with WYN/RW/CM exhibiting
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the lowest at 23.05%. The HR values (Table 3) demonstrated considerable variation across the

microcapsules, with WYN/RW/CM having the lowest and MDN/RW/CM the highest. Following
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this, it was noted that the flowability in GMC/RW/CM and MDN/RW/CM was "very poor" and
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"awful," respectively, whereas, in WYN/RW/CM, it was deemed "passable." Additionally, the

findings indicated that the WYN/RW combination enhanced flowability compared to the

alternative combination. This improvement may be attributed to the reduced surface interactions

between their particles, WYN and RW/CM, whose propensity to aggregate results in a

hydrophobic chain that hinders powder flow due to the high particle contact surface area. This

condition permits increased cohesion and attrition force, increasing flow resistance [40]. The

outcomes of this study were comparatively inferior to those HR values (1.68–2.99) and CI values

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(40.62–52.04; 40.9–48.9) obtained from the microencapsulation of refined kenaf seed oil and

gurum seed oil from derived research [20,39].

3.2.6. Color

The color parameters (L*, a*, and b*) of the microcapsule powder are illustrated in Table

3. There were notable variations in the lightness (L*) values of the microcapsules (p ≤ 0.05), with

MDN/RW/CM demonstrating the maximum degree of whiteness, followed by GMC/RW/CM and

WYN/RW/CM having the lowest. Conversely, the (a*) value identified a propensity for redness in

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the WYN/RW/CM microcapsules (2.22), whereas the MDN/RW/CM and GMC/RW/CM exhibited

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greenness. Moreover, a significant contrast was noted in the b* parameter among the

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microcapsules. The WYN/RW/CM combination displayed the highest level of yellowness,
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followed by GMC/RW/CM and MDN/RW/CM, with respective values of 39.64, 15.69, and 3.82.

The observed yellowness can be attributed to the influence of the color of the wall materials and
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the encapsulated cinnamon essential oil, as previously mentioned [44,45].

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3.2.7. FT-IR

Figure 1 displays the FT-IR spectra of wall materials (WYN, MDN, GMC, and RW) and
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various microcapsules, describing the possible molecular interactions during the emulsification
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process among the wall materials and CM. RW spectra revealed notable broadband peaks

corresponding to the bending methylene and aliphatic groups (–CH) at 2918 and 2846 cm-1,

respectively. Additionally, the functional groups of the band stretching from carboxylic and

aldehydic acids in wax represented fatty acids at 1740 cm-1, while the bands (–CH2), (–CH3) bend,

and ester band (C–O) at 1378, 1472, and 1180 cm-1, respectively, similar results for natural waxes

was achieved by Hashim et al. [13]. The CM spectra indicated that the observed band peaks of

aromatic composites were linked to stretching vibration at 1672, 1630, 1299, and 1445 cm-1. The

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(C–H) peaks of olefin and benzene rings emerged at 742 and 680 cm-1, respectively, which were

consistent with the results reported by Wei et al. [46] and Barbosa et al. [1]. The GMC spectra

exhibited bands at 3356, 2913, and 1611 cm-1 representing hydroxyl group (O-H), carboxylic

group (C-H) stretching, and N-H bending. Simultaneously, the peak bands at 1416 cm-1 related to

CH3 and C–H bending and C–O stretching peak at 1048 cm-1 [28]. The spectrum of MDN

displayed absorption bands at 3331 cm-1, 2918 cm-1, 1353 cm-1, 1158 cm-1, 1023 cm-1, as well as

(O-H), (C–H), (C=O), (C–O) and (C–O–H) stretching. Similarly, the pyranoid ring has

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wavelengths of 934, 846, and 760 cm-1 [22]. The spectrum for WYN showed stretching vibrations

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of the N–H bond of amide A at 3288 cm-1, the band N–H bending and C–N stretching vibrations

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at 1391 cm-1, and amino groups primary (1632 cm-1) and secondary (1527 cm-1). Therefore, the

bands stretching at 2931cm-1 (C-H) and C–O–C at (1077 cm-1) were reliable by Cassol & Noreña
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[47].
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In the GMC/RW/CM spectrum, it was noted that the broadband in GMC spectra associated
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with stretching vibration hydroxyl groups (–OH) in the range (3012-3566 cm-1) was comprised of

(3039-3560 cm-1) as evidence of molecular interaction with RW and CM. Furthermore, the band
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of the functional groups of carboxylic and aldehydic acids (-C-O) at 1741cm-1 appears to be
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designated for the fatty acid (RW) construction of the microcapsules. Additionally, the aromatic

compounds at the peak adsorption in 1672, 1445, 1299 cm-1, and C–H vibration of the benzene

ring and olefin at 680 cm-1 and 742 cm-1 because of the interaction of hydrogen bonds formed

between GMC/RW and encapsulate the CM. The spectral analysis of the WYN/RW/CM

microcapsules reveals variations in band intensities, indicating interactions between the wall

material (WYN/RW) and CM. The hydroxyl group peak area deformation shifts from 3113–3660

cm-1 in the WYN spectra to 3130-3429 cm-1 in the microcapsules. This shift is attributed to the

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hydrophobic nature of the microcapsules. The 1740 and 1156 cm-1 microcapsule spectra exhibit

characteristic vibrations corresponding to fatty acids and esters. The CM phenol compounds

interacted at 1445, 690, and 739 cm-1 [46]. The spectra of MDN/RW/CM microcapsules revealed

intermolecular interactions between the various components. Notably, the bands at 1740 and 760

cm-1 corresponded to fatty acids, while those at 1681, 1634, and 1681 cm-1 indicated benzene rings

and phenols. Furthermore, the broadband region, including wavenumbers ranging from 2997 to

3566 cm-1, which correspond to the stretching vibrations of hydroxyl groups (-OH), displays a

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distortion, resulting in a shift towards wavenumbers ranging from 3028 to 3566 cm-1.

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3.2.8. Crystallinity

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The XRD technique assesses the degree of crystallinity and amorphousness in various
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microcapsule forms. Figure 2 displays the microcapsule powder's X-ray diffraction (XRD) pattern.

The microcapsules with MDN/RW/CM composition exhibited the lowest relative crystallinity,
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measuring at 34.67%. Following this, the WYN/RW/CM composition had a slightly higher relative
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crystallinity of 40.28%. The variations in relative crystallinity among microcapsules can be

attributed to their distinct molecular crystallinity structure, wall material composition, and the
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methods employed for processing the interaction of different components, resulting in alterations
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in their diffraction patterns. Crystallinity influences the free volume of barrier permeability in

microcapsules, affecting properties such as wettability and solubility. Moreover, the decline in the

degree of crystallinity results in a reduction in both the energy and temperature required for the

manifestation of phase transitions [23,24]. Conversely, the GMC/RW/CM composition exhibited

the most significant relative crystallinity at 46.53%. The results indicate that Pulicaria jaubertii

extract microcapsules were within the range of 34.03% to 46.52%, as reported by Al-Maqtari et al.

[23]. However, it is worth noting that the crystallinity of these microcapsules was more remarkable

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compared to the microcapsules (MDN, GMC, and WYN with CM) studied by Mahdi et al. [28],

which had a relative crystallinity of cinnamon essential oil at 28.69%. The degree of crystallinity

has been shown to impact the barrier qualities related to temperature resistance, hygroscopicity,

and rehydrability [48].

3.2.9. SEM

SEM images provide visual representations of the microstructure and morphology of

freeze-dried microcapsules. Figure 3 demonstrates a noticeable disparity in the CM microcapsule

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compositions of RW/CM. The microcapsules generally have an irregular particle morphology

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reminiscent of a fractured glass-like structure. This glassy characteristic is probably attributed to

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the milling process conducted after freeze-drying [22]. The WYN/RW/CM formulation exhibited
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lighter shred powder than the other capsules, markedly smooth edges, and a crack-free surface.

The varied groups (hydrophobic and hydrophilic) in the resulting WYN may facilitate the
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dissolution of the RW/CM in the emulsion, forming more uniform microcapsules [4,6]. The
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GMC/RW/CM microcapsules notably exhibited a varied structure with sharp edges and some

smooth surfaces. Conversely, the MDN/RW/CM microcapsule has numerous holes and cracks with
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irregular surfaces. According to [28], the stability of the encapsulated oil is connected to the limit
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of pores or fractures, which reduces the oxidation process.

3.2.10. Thermal properties

Figure 4 depicts the thermograms of TGA and DSC. The TGA findings demonstrated a

disparity in thermal stability among the various microcapsules, which may be due to the thermal

properties of the polymer used. Two distinct thermal change patterns exhibited encapsulated

behavior based on the TGA curves. The first trend corresponded to moisture loss, while the second

trend indicated the loss of volatiles and other components. Furthermore, the remaining mass

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residues for MDN/RW/CM, GMC/RW/CM, and WYN/RW/CM were determined to be 33.62%,

31.21%, and 37.78%, respectively. Studies by Mohammed et al. and Yang et al. [22,49] reported

the same trend for Citrus aurantium and pepper seed oil microcapsules. In addition, GMC/RW/CM,

MDN/RW/CM, and WYN/RW/CM experienced mass losses of 6.5%, 3.24%, and 3.21%,

respectively, when subjected to a temperature of 100 °C. The findings indicate that CM

microcapsules can be utilized in food products that undergoing pasteurization and sterilization

processes. This is supported by an earlier report that there was no significant weight loss (mass

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loss < 5%) observed at a temperature of 100 °C [24,33]. However, the GMC/RW/CM capsule

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exceeds a mass loss of 5%, perhaps indicating a correlation with factors such as the speed and

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length of material emulsion homogenization, the ratio of core-to-wall material, and the
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temperatures utilized during freeze-drying.

The DSC thermograms may exhibit three primary thermal transitions- a glass transition
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associated with the amorphous phase, a melting transition attributed to the crystalline phase, and
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a transition resulting from crystallization. The DSC thermograms of the various microcapsules

displayed exothermic peaks within the temperature ranges of (36.6 °C–188.9 °C), (57.3 °C–
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172.8 °C), and (32.02 °C–212.26 °C), which corresponded to the amorphous fraction of the
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microcapsules. Additionally, endothermic peaks were observed within the temperature ranges of

(262.9 °C–343.9 °C), (203.05 °C –306.18 °C), and (224.91°C–355.07 °C), indicating the transition

from the melting crystalline fraction associated with the GMC/RW/CM, MDN/RW/CM, and

WYN/RW/CM microcapsules, respectively. These discoveries were documented by Ozdemir et al.

[33] and Yang et al. [49]. Thus, it was discovered that the microcapsules displayed varying forms,

architectures, and molecular weights. The DSC study revealed that the glass transition temperature

(Tg) of the different microcapsule formulations had the lowest value of GMC/RW/CM (73.6 °C),

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followed by MDN/RW/CM (87.5 °C) and the highest value of WYN/RW/CM (96.2 °C). These

results indicate that utilizing RW increased thermal stability. Furthermore, Tg represents a critical

temperature at which there is a notable alteration in material characteristics [49]. Specifically, it

signifies that molecules cannot move at temperatures lower than Tg, transforming polymers into a

glassy and rigid state. Thermally stable materials generate more stable particles throughout

processing, minimizing their interactions with external factors and, more critically, during storage

[22]. Tg temperature levels above 22–28 °C, according to Ozdemir et al. [33], are crucial for

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retaining powder uniformity and quality throughout storage.

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3.3. Storage stability of microcapsules

3.3.1. Release of TPC

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The release of TPC from the microcapsules was observed during storage for 55 days at

4 °C and 25 °C, which indirectly defines the percentage of TPC in the capsules during storage
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(Figure 5. A, B). Before the release study, it was observed that the quantity of TPC in the
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microcapsules significantly varied, with 31.18 mg GAE g-1 in WYN/RW/CM, 30.67 mg GAE g-1

in GMC/RW/CM, and 24.21 mg GAE g-1 in MDN/RW/CM (Table 3). The findings of this study
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suggest that incorporating WYN in conjunction with RW in CM formulations has led to a

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considerable enhancement in phenolic chemical binding, which is consistent with the EE results.

Numerous studies have verified that WYN is a promising wall material that can facilitate the

binding of phenolic compounds in its chemical structure, thereby enhancing their stability [28,50].

During storage, there were noteworthy changes in the release of TPC from various CM

microcapsules at 4 °C and 25 °C. This release gradually increased with time, as illustrated in Figure

5. A, B. After 55 days at 4 °C, the highest release was observed with MDN/RW/CM (70.84%),

next GMC/RW/CM (62.65%), with the lowest release occurring in the case of WYN/RW/CM

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(47.48%). Likewise, at 25 °C after the same duration, MDN/RW/CM exhibited the highest release

(100%), followed by GMC/RW/CM (93.19%), while WYN/RW/CM had the lowest release

(75.53%). The results indicated that WYN/RW/CM was the most efficient carrier system for

preserving CM phenolics, followed by GMC/RW/CM and MDN/RW/CM during storage at 4 °C

and 25 °C. Furthermore, it was observed that samples stored at a lower temperature (4 °C) delayed

the release of TPC from capsules than those stored at 25 °C. The polymeric structure of wall

materials and their proper combinations in the capsules might be crucial role in controlling the

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release or preserving the TPC over the storage period.

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The study conducted by Al-Maqtari et al. [23] indicated that the effective slow-release

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characteristic of microcapsules is strongly associated with their uniform construction of materials.
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These factors are instrumental in regulating the release of bioactive compounds, as evidenced by

a 28-day storage study conducted at various temperatures. The research observed that the
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maximum release of these compounds was below 40%, which aligns with the findings of Kenari
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et al. [51], who investigated the release of TPC over 60 days and detected a similar trend with a

release rate of approximately 50%. In both cases, the controlled release of bioactive compounds
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appears to be influenced by the microstructure and compactness of the microcapsules.

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3.3.2. Release of antioxidant

The changes in the antioxidant activity of microcapsules were investigated throughout the

storage period of 55 days at temperatures of 4 °C and 25 °C (Figure 5C, D). According to Table 3,

the WYN/RW/CM microcapsules had a maximum DPPH free radical inhibition percentage

(86.96%), followed by the GMC/RW/CM (83.47%) and MDN/RW/CM (80.41%). The storage

study results showed that the MDN/RW/CM microcapsules exhibited a greater level of antioxidant

activity than other microcapsules after the first 5-day of storage at 4 °C and 25 °C, with values of

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3.74% and 6.3%, respectively. While the GMC/RW/CM microcapsules showed antioxidant

activity of 2.8% and 4.9% at the respective temperatures, and the WYN/RW/CM microcapsules

exhibited the lowest release level of antioxidant activity, with values of 1.9% and 3.5% at 4 °C and

25 °C, respectively. As storage time increased, the antioxidant activity of CM capsules gradually

increased. After 55 days of storage, the MDN/RW/CM microcapsules exhibited more significant

free radical scavenging activity of 63.9% and 82.29% at 4 °C and 25 °C, respectively. While, the

GMC/RW/CM microcapsules revealed antioxidant activity of 54.36% and 70.48%, and the

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WYN/RW/CM microcapsules displayed 51.9% and 66.3% at 4 °C and 25 °C, respectively. Similar

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to the TPC results, storage temperature had a significant effect on antioxidant activity. Studies

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verified that antioxidant activity is correlated with the presence of antioxidant molecules that can
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scavenge free radicals. Since several phenolics are potent antioxidants (e.g., gallic acid), their

release from the microcapsules might enhance the antioxidant activity. Studies also support that, a
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more significant release of antioxidant phenolics from capsules may increase the level of
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antioxidant activity. Therefore, the superior antioxidant activity observed in MDN/RW/CM

microcapsules could be attributed to a more significant release of phenolics. In contrast,

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WYN/RW/CM and GMC/RW/CM microcapsules preserved the bioactivity, which can be

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gradually revealed depending on the phenolic release profile. The observed phenomenon could be

attributed to the combination of WYN and RW, which resulted in enhanced homogeneity of

emulsion interactions involving the hydrophobic compounds [15,27] present in both materials.

This interaction led to forming a thicker wall surrounding the active substances [52], reducing the

active compound release rate compared to the GMC and MDN. However, the effectiveness and

stability of encapsulated materials are governed by several aspects, among which the porosity

structure plays a significant role. The porous structure of microcapsules allows for the quicker

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penetration of oxygen through the matrix, leading to chemical oxidation and consequently, a more

rapid release of bioactive substances.

3.3.3. Oxidative stability

The oxidative stability of encapsulated CM was evaluated by chemical degradation

(amount of hydroperoxide). Figure 6 shows the oxidative stability of CM in various capsules

during the storage of 55 days at 4 °C and 25 °C. At the start of the study (0 days), the composition

of microcapsules significantly affected CM's oxidative stability. The measured hydroperoxide

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levels were 0.239 mM, 0.267 mM, and 0.213 mM for the MDN/RW/CM, GMC/RW/CM, and

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WYN/RW/CM microcapsules, respectively. MDN/RW/CM microcapsule showed the lowest

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oxidative stability without substantially distinct changes compared to the other microcapsules. The

results also demonstrated that combining WYN and RW in the microcapsules improved the
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oxidative stability of CM. These results were consistent with whey protein isolate-based
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formulations that had more excellent oxidative stability than gum Arabic and maltodextrin-based
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formulations [24,53]. Furthermore, the results demonstrated that temperatures influenced CM's

oxidative stability. When CM formulations were kept at 4 °C, oxidative degradation was lower
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than when stored at 25 °C.

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Mohammed et al. [22] demonstrated that temperature plays a crucial role in influencing the

oxidative stability of microcapsules. Their study revealed that microcapsules stored at 5°C

demonstrated superior oxidative stability compared to those stored at 50°C. Additionally, these

findings indicated a correlated relationship with encapsulation efficiency, as formulations

exhibiting lower efficiency tended to display diminished stability. Additionally, the findings

emphasized that combining various wall materials in the formulation led to superior encapsulation

of essential oils compared to using them individually. In summary, CM's microencapsulation

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significantly enhanced the core materials' oxidative stability, with the most substantial

improvement observed when utilizing WYN/RW/CM.

3.4. Antibacterial Activity

Foodborne infections play a substantial role in compromising food quality. The

antibacterial activity of diverse microcapsules at varying concentrations (2%, 4%, and 8%)

targeting S. aureus and E. coli are shown in Fig. 7A, B, and C. Overall, the results indicated

significantly enhanced antibacterial activity of the microcapsules against both S. aureus and E.

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coli, and the inhibition capacity increased with increasing concentration. The findings indicated

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that among the formulations examined, WYN/RW/CM had the most notable effect on the assessed

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bacteria. WYN/RW/CM (8%) achieved the most significant inhibition zones, measuring 40.5 mm
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and 41.4 mm against S. aureus and E. coli, respectively. Barbosa et al. [1] found a comparable

outcome, noting that the cinnamon capsules demonstrated inhibitory halos spanning
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approximately 44 to 56 mm. Also, similar observations were documented in a study conducted by

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López-Miranda et al. [54], where they noted increased antimicrobial effectiveness against E. coli

and S. aureus by encapsulating the carvacrol and thymol. Furthermore, Gottardo et al. [29]
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illustrated that combining equal proportions of the essential oils of oregano and cinnamon led to a
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noteworthy inhibition zone. The antibacterial action of chemical components is commonly

attributed to their capacity to permeate the cell wall, disrupt the cytoplasmic membrane of

microorganisms, and release intracellular components [23]. However, the findings of this study

suggest that these capsules hold significant potential as additives to combat common

microorganisms responsible for food degradation.

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4. Conclusion

In conclusion, the stability and bioactivity efficiency of the CM core material was significantly

enhanced by encapsulating it with various wall materials, including berry wax, combined with

individual materials (WYN, MDN, and GMC). This encapsulation technique considerably

increased the efficiency, improving the material's physicochemical properties and thermal stability.

Additionally, it facilitated the controlled release of bioactive substances from the microcapsules,

especially under storage conditions at 4 °C and 25 °C. The noteworthy advancements achieved

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with the combined WYN/RW encapsulation strategy hold promise for optimizing the utilization

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of sensitive bioactive substances like essential oils. To maximize their utilization, further studies

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should investigate the efficiency of this proven combination (WYN/RW) as a wall material for
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encapsulating other bioactive compounds.
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Credit authorship contribution statement.

Sulafa B.H. Hashim: Writing – original draft, Conceptualization, Methodology, Software.

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Haroon Elrasheid Tahir: Conceptualization, Methodology, Software. Amer Ali Mahdi:

Software, Validation, Data curation. Qais Ali Al-Maqtari: Visualization, Investigation.

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Mohammad Rezaul Islam Shishir: Visualization, Investigation. Xiaodong Zhai: Formal

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analysis. Gustav Komla Mahunu: Writing – review & editing. Xiaodong Zhai: Formal analysis.

Halah Aalim: Visualization, Investigation. Suliman Khan: Writing – review & editing. Zou

Xiaobo: Validation, Resources, Data curation, Funding acquisition. Shi Jiyong: Validation,

Resources, Data curation, Funding acquisition.

Declaration of Competing Interest

The authors declare that they have no known competing financial interests or personal

relationships that could have appeared to influence the work reported in this paper.

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Data availability

The data that has been used is confidential.

Acknowledgments

This work was supported by the National Key Research and Development Program of

China (Grant No. 2022YFD2100603); the National Natural Science Foundation of China (Grant

No. 32350410402, 32272407); the Natural Science Foundation of Jiangsu Province (Grant No.

BK20220058, BE2022313, BK20200103, BK20220111); Foundation of Jiangsu Specially-

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Appointed Professor (Grant No. 202074); Priority Academic Program Development of Jiangsu

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Higher Education Institutions (PAPD).

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Conflict of Interest

Sulafa B.H. Hashim declares that she has no conflict of interest. Haroon Elrasheid Tahir declares

that he has no conflict of interest. Shi Jiyong declares that he has no conflict of interest. Zou Xiaobo

declares that he has no conflict of interest. Amer Ali Mahdi declares that she has no conflict of

interest. Qais Ali Al-Maqtari declares that she has no conflict of interest. Mohammad Rezaul Islam

Shishir declares that he has no conflict of interest. Xiaodong Zhai declares that he has no conflict

of interest. Gustav Komla Mahunu declares that she has no conflict of interest. Halah Aalim

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declares that she has no conflict of interest. Suliman Khan declares that he has no conflict of

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interest.

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Graphic Abstract

Figure. 1. FTIR spectra of cinnamon essential oil (CM), berry wax (RW), gum Arabic (GMC),
maltodextrin (MDN), whey protein (WYN), and the microocapsules.

Figure 2. Relative crystallinity (%) of various microcapsules prepared with different wall
materials.

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Figure 3. Morphology of the various microocapsules with different wall materials by scanning
electron microscopy (SEM).

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Figure 4. TGA and DSC curves of the various microcapsules.
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Figure. 5. (A) TPC at 4 °C, (B) TPC at 25 °C, (C) Antioxidant at 4°C, (D) Antioxidant at 25 °C,
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various microcapsules prepared with different wall materials during storage days. Different upper-
case letters (A, B, and C) indicate significant differences (P ≤ 0.05) between the various
microcapsule at the same time, and lower-case letters (a–l) indicate significant differences between
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the same micocapsule at various times.

Figure. 6. (a) Oxidation value at 4°C, (b) Oxidation value at 25°C, of various microcapsules
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prepared with different wall materials during storage days. Different upper-case letters (A, B, and
C) indicate significant differences (P ≤ 0.05) between the various microcapsules at the same time,
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and lower-case letters (a–l) indicate significant differences between the same microcapsule at
various times.

Figure.7. Inhibition zone at different concentrations (2%, 4%, and 8%) of microcapsules against
(A) E. coli, (B) S. aureus, and (C) antimicrobial inhibition zones at an 8% concentration of
microcapsules. Different upper-case letters (A, B, and C) indicate significant differences (P ≤ 0.05)
between the various microcapsules at the same time, and lower-case letters (a–c) indicate
significant differences between the same microcapsule at various times.

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Table 1. Design of the aqueous and lipid phase formulations of Nanoemulsions

Formulation Berry Wax + Whey Maltodextrin Gum Arabic Cinnamon

Code Sunflower oil protein + + distilled essential oil +
+ distilled
(1:2) ratio distilled water (1:2) Tween 80 (5:1)
water (1:2)
water (1:2)

WYN/RW/CM 15 300 6

MDN/RW/CM 15 300 6

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GMC/RW/CM 15 300 6

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Table 2. Droplet Size diameter, polydispersity index (PDI), and Zeta -potential of various materials in fresh emulsions

Emulsions Formation Droplet size diameter (nm) PDI Zeta-Potential (mV)

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WYN/RW/CM 456.12 ± 1.04a 0.25 ± 0.01ab -34.57 ± 0.25b

MDN/RW/CM 440.33 ± 11.48a 0.31 ± 0.01a -27.39 ± 1.51a
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GMC/RW/CM 265.46 ± 5.35b 0.24 ± 0.03b -23.80 ± 0.20a

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The data are shown as the mean ± SD (n = 3). In the same column, the different letters indicate that the
data is significantly different (p ≤ 0.05).
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Table 3. Physical and Physicochemical Properties of Various Microcapsules

Microcapsule properties WYN/RW/CM MDN/RW/CM GMC/RW/CM

Encapsulation efficiency (%) 93.40 ± 0.16a 81.25 ± 0.09c 88.50 ± 0.58b

Moisture content (%) 2.21 ± 0.12a 2.46 ± 0.13a 2.27 ± 0.10a

Water activity 0.02 ± 0.01b 0.03 ± 0.01a 0.03 ± 0.01a

Hygroscopicity (%) 8.38 ± 0.49b 11.53 ± 0.29a 10.51 ± 0.42a

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Wettability (min) 15.12 ± 0.18a 10.46 ± 0.09c 12.34 ± 0.08b

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Solubility (%) 72.64 ± 1.77c 78.41 ± 1.71b 78.41 ± 1.70b

Bulk density (g/cm3) 0.39 ± 0.01a 0.27 ± 0.02c 0.30 ± 0.00b

Tapped density (g/cm3) 0.51 ± 0.01a

-p 0.44 ± 0.00c 0.47 ± 0.01b
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Particle density (g/cm3) 1.99 ± 0.06a 1.69 ± 0.07b 1.73 ± 0.08b
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Carr’s index (CI) 23.05 ± 1.88b 39.38 ± 0.82a 36.12 ± 1.09a

1.30 ± 0.03c 1.65 ± 0.02a 1.57 ± 0.03b

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Hausner ratio (HR)

Flowability Passable Awful Very poor

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Color parameters
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Lightness (L*) 86.08 ± 0.67c 97.93 ± 0.54b 92.56 ± 1.41a

Redness (a*) 2.22 ± 0.16a -0.75 ± 0.06b -0.63 ± 0.17b

Yellowness (b*) 39.64 ± 0.37a 3.82 ± 0.40c 15.69 ± 0.80b

TPC (mg GAE g-1capsules) 31.18 ± 0.21a 24.21 ± 0.01c 30.67 ± 0.01b

DPPH inhibition (%) 86.96 ± 0.28a 80.41 ± 1.39c 83.47 ± 0.91b

The data are shown as the mean ± SD (n = 3). In the same raw, the different letters indicate that the data is
significantly different (p ≤ 0.05).

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Highlights:

- Cinnamon oil is encapsulated in berry wax with various wall material formulas.

- Wall materials control the encapsulation efficiency and physiochemical properties.

- Release stability and lipid oxidation were conducted at 4 °C and 25 °C for 55 days.

- Microcapsules offered excellent antimicrobial activity against E. coli and, S. aureus.

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