Accepted Manuscript

Native and modified Sorghum starches as wall materials in

microencapsulation of nutmeg oleoresin

Hira Arshad, Tahira Mohsin Ali, Abid Hasnain

PII: S0141-8130(17)32895-7
DOI: doi:10.1016/j.ijbiomac.2018.03.082
Reference: BIOMAC 9304
To appear in:
Received date: 4 August 2017
Revised date: 21 February 2018
Accepted date: 16 March 2018

Please cite this article as: Hira Arshad, Tahira Mohsin Ali, Abid Hasnain , Native and
modified Sorghum starches as wall materials in microencapsulation of nutmeg oleoresin.
The address for the corresponding author was captured as affiliation for all authors. Please
check if appropriate. Biomac(2017), doi:10.1016/j.ijbiomac.2018.03.082

This is a PDF file of an unedited manuscript that has been accepted for publication. As
a service to our customers we are providing this early version of the manuscript. The
manuscript will undergo copyediting, typesetting, and review of the resulting proof before
it is published in its final form. Please note that during the production process errors may
be discovered which could affect the content, and all legal disclaimers that apply to the
journal pertain.
 ACCEPTED MANUSCRIPT

Native and modified Sorghum starches as wall materials in microencapsulation of Nutmeg

oleoresin

Hira Arshada,x, Tahira Mohsin Alia, Abid Hasnaina

a
Department of Food Science and Technology, University of Karachi, 75270, Karachi, Pakistan

T
x
Corresponding author email (hira_fst@hotmail.com)

IP
CR
US
AN
M
ED
PT
CE
AC

1
 ACCEPTED MANUSCRIPT

Abstract

The effect of the partial or total substitution of gum arabic (GA) with native (NA), octenyl

succinic anhydride (OSA) and succinylated (SUC) sorghum starches on microencapsulation of

nutmeg oleoresin was studied using spray drying technique. The oleoresin with 10% load is

emulsified by using three different combinations of GA along with native and modified sorghum

T
IP
starches. The proportion of GA and sorghum starch was fixed at 75:25, 50:50, and 25:75. Most

CR
of the feed emulsions were having good emulsion stability and lower emulsion viscosity. The

highest oil retention of 95% with 84.07% encapsulation efficiency was achieved when GA: NA

US
starch was used in the fraction of 25:75. The highest encapsulation efficiency of 95.38% was

obtained by GA: OSA in a ratio of 75:25. Results obtained suggested that both NA and OSA
AN
starches could be considered as a good alternative to gum arabic for microencapsulation.
M

Keywords

Microencapsulation; Nutmeg Oleoresin; Spray Drying; Sorghum Starch

ED
PT
CE
AC

2
 ACCEPTED MANUSCRIPT

1. Introduction

Spices are derivatives of aromatic plants used to enhance the flavor and aroma profile of food

and possess a significant position in the field of food industry. Common spices include clove,

cinnamon, mace, nutmeg, black pepper, cumin etc. Spices could be used directly in the form of

dried powder or in the form of its oleoresin. Spice oleoresin represents the aroma profile similar

T
to that of original spice from which it has been extracted [1]. Oleoresins are the solvent extract of

IP
spices that exhibit volatile as well as non volatile constituents of spices. Rather than ground

CR
powder, oleoresins are more preferred because of their balanced, reliable and quantifiable nature

[2]. Oleoresins are easily accessible throughout the year with guaranteed storage stability in the

US
final product and also free from microbial contamination. As oleoresins are sensitive to light, air,
AN
moisture and elevated temperature, they can easily degrade [3]. Microencapsulation offers an

alternative method to limit the aroma and flavor loss during storage and processing.
M

Microencapsulation is the process of making enveloped capsule enveloping guest molecule in a

ED

micron range [4]. Simply, microencapsulation is a technique to protect targeted particle in a

coating material to give capsules of micron size ranging from one micron to several hundred
PT

microns [5]. These protected particles remain inert in capsules for specific period of time and
CE

release when needed for its specific function. Solid, liquid or even gaseous particles can be

encapsulated for uncountable reasons [3].The material within the capsule is often refer to as core
AC

or fill whereas the wall material refers as coating or shell material [6]. Core material may be in

solid material as an active constituent, diluents, stabilizers, excipients or release rate accelerators

and as a liquid core could include dispersed or dissolved material [7]. Microencapsulation is an

important technique to provide coating of bioactive compounds into food system and their

3
 ACCEPTED MANUSCRIPT

successful release to gastrointestinal tract such as essential oils, vitamins, lycopene, minerals,

essential fatty acids, probiotics, phytosterols, plant extracts, antioxidants etc.

Numerous methods are reported for microencapsulation of spice oleoresin, but the most accepted

technique employed in the industry is spray drying. Spray drying is an appropriate method for

microencapsulation of oils and oleoresins [8], [9]. Carbohydrates such as hydrolyzed starches

T
IP
(SHPs), modified starches, emulsifying starches and gums (especially gum acacia) are the most

CR
common carrier materials [10]. Gums are also used for secondary effect such as stabilization of

emulsion, encapsulation, and film formation. Being hydrophilic in nature, gum arabic and native

US
starches have little affinity for hydrophobic flavor oils. Their hydrophilic nature can be altered

by modifying them with octenyl succinic anhydride (n-OSA). N-OSA treated starch contains
AN
hydrophobic octenyl side chains, which impart emulsifying ability to the starches. These wall
M

materials have excellent emulsification properties [11]. However, emulsifying starches have
ED

some limitations. In addition, problems associated with the use of gum arabic in

microencapsulation are high cost and limited supply and they exhibit poor flavor protection
PT

against oxidation and have off flavor [10]. Krishnan [1] studied the effectiveness of succinylated

waxy maize starch, maltodextrin and gum arabic as wall materials for encapsulation of
CE

cardamom oleoresin by spray drying.

AC

White sorghum (Sorghum bicolor) is a non-gluten cereal crop with major storage form of

carbohydrate is starch that ranges from 55.6 to 77% based on kernel weight [12]. Sorghum starch

is very similar to commercially important corn starch in many of its functional properties,

whereas in terms of agronomic properties it is even better than corn. Nevertheless, low cost of

sorghum combined with significant agronomic properties make sorghum an ideal crop for

4
 ACCEPTED MANUSCRIPT

isolation of starch especially for a country like Pakistan facing heightened water shortage.

Secondly, with increased use of corn and potato in preparation of breakfast cereals and snacks,

their accessibility is warning. Therefore, sorghum could be foreseen as a potential commercial

source for isolation of starch [13].

The present work deals with microencapsulation of nutmeg oleoresin by spray drying. The

T
objective of this research was to study suitability of native and modified sorghum starches (OSA

IP
and Succinylated) in combination with gum Arabic in different ratios as wall material. Emulsion

CR
characteristics, encapsulation efficiency, physiochemical properties of spray dried

microcapsules; retention and stability of the main flavor oil in microcapsules during storage were

studied.
US
AN
2. Material and methods

White sorghum grains were provided by Pakistan Agriculture Research Council (PARC) and
M

stored at room temperature after fumigation. Nutmeg seeds were purchased from local market in
ED

Karachi and stored at 4⁰C prior to extraction of oleoresin. Gum Arabic, succinic anhydride, n-

octenyl succinic anhydride, sodium metabisulphite, ethanol, sodium hydroxide, hydrochloric

PT

acid and n-hexane were purchased from Merck (Darmstadt, Germany). All chemicals utilized
CE

were of analytical grade.

2.1. Extraction of nutmeg oleoresin

AC

Nutmeg oleoresin was obtained from nutmeg seeds (Myristica fragrans houtt) by direct

maceration method according to the procedure described by Assagaf et al. [14].

2.2. Isolation of sorghum starch

Isolation of starch from sorghum grains was carried out by using the method described by

Mehboob et al. [13].

5
 ACCEPTED MANUSCRIPT

2.2.1. Succinylation of sorghum starch

Succinylation of sorghum starch was done by the method of Moin et al. [15].

2.2.2. Degree of substitution (DS) of succinylated starch

Molar degree of substitution (DS) is the average number of hydroxyl groups substituted per

glucose unit of starch. The method described by Wurzburg [16] was adopted to calculate the

T
IP
degree of substitution for succinylated starch.

CR
2.2.3. Octenyl succinic anhydride (OSA) modification of sorghum starch

The method of Bhosale and Singhal [17] was used for octenyl succinic anhydride modification of

US
sorghum starch with few modifications.
AN
2.2.4 Degree of substitution of OSA modified starch
M

The determination of octenyl succinylation level of modified sorghum starch was done by

titrimetric method described by Bhosale and Singhal [17].

ED

2.2.5. Particle size analysis of starch (native and modified)

PT

For native and modified sorghum starches, the particle size distribution of each sample was
CE

analyzed by using public domain software Image (J v1.36b). The result was obtained by

measuring the diameter of 100 particles of starch (native and modified) with the help of SEM
AC

images (1000x) through software. The particle size of starches (native and modified) were

expressed as the mean volumetric size d43 (De Brouckere mean diameter) of sphere having same

volume [20].

2.3. Emulsion preparation

The wall material used in the current study was gum arabic, native and modified (succinylated

and octenyl succinylated) sorghum starches and nutmeg oleoresin was used as core material.

6
 ACCEPTED MANUSCRIPT

About 30% (w/w) solution of gum Arabic (GA) and sorghum starches (ST) (native and

modified) in the proportion of 75:25, 50:50 and 25:75 on dry weight bases were unified in

500mL distilled water with constant stirring at ambient temperature. While the forth emulsion

comprised of starch only. The blends were kept in refrigerator for rehydration for about 24 hours

at 10⁰C. Nutmeg oleoresin was added slowly in a proportion of 10% (w/v) with respect to wall

T
material concentration. The blend was then homogenized at 9000 rpm for 15 min by using T.K

IP
Homo Mixer 2 (Model A94506X, Osaka, Japan).

CR
2.3.1. Emulsion stability

US
Emulsion stability or creaming stability was estimated using the method of Park et al., [18] based

on the emulsion stability index (ESI).

AN
2.3.2. Emulsion viscosity

Emulsion viscosity of emulsion was determined by Haake Visco tester 6 L at 30 rpm (HAAKE,
M

TYP 3870001, and SPAIN) by using spindle L2 at 25 .

ED

2.3.3. Emulsion droplet size

PT

The particle droplet size of emulsions was determined by the method described by Frascareli

[19].
CE

2.4. Encapsulation of nutmeg oleoresin

AC

The homogenized emulsion was spray dried in Eyela spray dryer SD-1 (Tokyo Rikakikai Co.,

Ltd Japan) equipped with twin fluid nozzle operating co currently at air pressure of 0.6 kg/cm2

with flow rate of 400 mL/h using the method of Frascareli et al., [19].

7
 ACCEPTED MANUSCRIPT

2.5. Analysis of spray dried microcapsules

2.5.1. Moisture content

The moisture content of spray dried microcapsules was determined according to the method of

Fernandes et al., [20] by drying 0.5g powdered sample gravimetrically in hot air oven at 103

until constant weight.

T
IP
2.5.2. Cold Water Solubility

CR
Cold water solubility of spray dried powder was determined using the method of Singh and

Singh [21].

US
2.5.3. Hygroscopicity
AN
Hygroscopicity of the spray dried powdered samples were analyzed using the method of Cai and

Corke [22] with some modifications. One gram of each sample was placed in a dessicator
M

containing saturated brine solution of relative humidity 75.3% for 7 days. The weight of the
ED

samples was taken after one week and hygroscopicity of samples were determined by the amount

of adsorbed moisture per 100g of powder sample.

PT

2.5.4. Powder wettability

CE

Powder wettability of spray dried microcapsules was determined by the method of Fernandes et

al., [20].
AC

2.5.5. Flowing properties of microcapsules

The bulk densities (ρB) and tapped densities (ρT) were determined in 25ml graduated glass

cylinders described by Xue et al., [23]. About 3g of sample (mo) was poured into graduated

cylinder. The volume of the sample (v0) was read directly from the cylinder and used to calculate

the bulk density (ρB= mo/vo). For tapped density, the cylinder was tapped until a constant volume.

8
 ACCEPTED MANUSCRIPT

The flow ability of samples was observed by Carr’s index and the Hausner Ratio by using

formula C= 100*( ρT -ρB )/ ρT and HR = ρT/ ρB.

2.5.6. Retention of nutmeg oleoresin in microcapsules

Oil retention for nutmeg microcapsules was estimated by calculating the oil concentration before

and after spray drying with respect to wall material concentration.

T
IP
2.5.7. Surface oil content on microcapsules

CR
The amount of oil present on the surface of microcapsules represents the non encapsulated or

free oil and was determined by the method of Tan et al., [24].

US
2.5.8. Estimation of total oil in microcapsules

Extraction and measurement of the total oleoresin present in the spray dried powder was
AN
determined by using soxhlet method illustrated in Wrolstad [25].
M

2.5.9. Encapsulation efficiency

ED

Encapsulation efficiency (EE %) was determined by the fraction of encapsulated oil over the

total oil in the spray dried microcapsules.

PT

2.5.10. Oxidative stability of oleoresin in microcapsules

CE

To determine the oxidative stability of encapsulated oil, the spray dried powder samples as well

as pure nutmeg oleoresin were stored at 7 and 25 in air tight plastic containers for 6 weeks.
AC

Samples were examined from first week to sixth week with respect to lipid oxidation by

evaluating the peroxide index of samples. To determine the Peroxide value, the oil was extracted

by the method of Partanen et al., [26]. The result was calculated as peroxide value meqv/ kg of

encapsulated oil.

9
 ACCEPTED MANUSCRIPT

2.5.11. Lipid oxidation

Peroxide values were determined according to IDF standard method described by Frascareli et

al., [19] with some modifications. The portions of 400µl of extracted sample were incorporated

to 9.6 ml of chloroform/methanol (7:3) mixture and then add 50 ml of 3.94M thiocyanate

solution and 50 ml of Fe+2 solutions. The sample was reacted in the dark and absorbance was

T
measured at 500nm before 10 min. By using Fe+3 standard curves with iron concentration

IP
ranging from 1 to 25 µg, the hydroperoxide concentrations were evaluated.

CR
2.5.12. Powder morphology and Particle size analysis of microcapsules

US
Morphological properties of microcapsules were observed by scanning electron microscopy

(JSM, 6380A, Jeol Japan) operating at an accelerating voltage of 10 kv. The powder sample was
AN
fixed on stub and coated with gold layer in a vacuum evaporator. The images of all
M

microcapsules were studied at 2000x magnification. For spray dried microcapsules, the particle

size distribution of each sample was analyzed by using public domain software Image J (v1.36b).
ED

The particle size of microcapsules were calculated as the mean volumetric size d43 (De
PT

Brouckere mean diameter) of sphere having same volume by measuring the diameter of 100

particles of microcapsules with the help of SEM images (1000x) through software [20]. The
CE

results were expressed in graph (particle size in µm vs. % volume).

AC

2.5.13. Statistical analysis

All measurements were carried out in triplicate. The results were statistically analyzed using

software statistical package for social sciences (SPSS). Analysis of variance (ANOVA) was

performed using the Duncan’s multiple range tests to compare treatments means (n≥3). Whereas

for comparing significant difference at p<0.05 for two samples (n=2), t-test was used employing

SPSS (version 20, SPSS, Inc, USA).

10
 ACCEPTED MANUSCRIPT

3. Results and discussion

3.1. Degree of substitution (DS) and Particle size analysis of starches

Starch is a naturally occurring, low cost biopolymer with comprehensive applications in food

industry due to its safety, biodegradability, inexpensiveness, and specific technological

characteristics such as gelling property, thickening, film forming, fat mimicking, etc [28]. Native

T
starch is hydrophilic in nature and their hydrophilicity is further altered by esterification with

IP
hydrophobic groups or negatively charged groups. OSA modification gives a specific surface

CR
activity to starch by incorporating hydrophobic alkenyl groups from OSA into the hydrophilic

starch molecule which disturbed the linearity of amylose chain and ramified portion of

US
amylopectin. Therefore, OSA starches are characterized by a decreased in gelatinization
AN
temperature and increase in paste viscosity. Octenyl succinic starches are used as emulsion

stabilizers, texturizing agents in many food-systems and for flavor encapsulation. Succinylation
M

of starch leads to addition of hydrophilic negatively charged succinyl groups which in turn gives
ED

a hydrophilic character to starch. Succinic groups weaken the internal bonding in starch granules

and facilitate starch solubilization even in cold water [28]. The degrees of substitution for
PT

modified starches are presented in Table 1. All sorghum starch samples were treated with 3%
CE

succinic anhydride. The DS of 0.0709 was observed for succinylated sorghum starch. The

difference in chemical substitution between starches of varying botanical sources is due to the
AC

difference in packaging of amylose in amorphous region together with the packaging of both

amylose and amylopectin within the granule. Degree of substitution of 0.023 was achieved for

OSA sorghum starch. The present result is quite similar to that reported by [17] having a DS of

0.021 for waxy corn starch treated with 3% OSA under the same conditions. In the current study,

the modifications of starches were done at a level of 3% which is the approved limit for

11
 ACCEPTED MANUSCRIPT

modification of starches by Food and drug administration (FDA). The mean particle size of

native, OSA modified and succinylated starches are presented in Table 1. The mean particle

diameter for native sorghum starch was observed as 12.56µm, whereas 13.65µm for OSA and

12.41µm for succinylated sorghum starch. There is no significant difference in mean particle size

of native and succinylated starch while OSA starch showed slight increase in particle size as

T
compared to both native and succinylated starch.

IP
CR
3.2. Emulsion stability and emulsion viscosity and oil droplet size

According to kinetic stability, emulsions are thermolabile systems which can be rapidly or

US
slowly divided into two immiscible phases [27]. Emulsion stability has been reported to have an

impact on microencapsulation efficiency, stability and properties of spray dried oil powders in
AN
terms of flocculation, coalescence or phase separation [24]. The emulsion stability and emulsion
M

viscosity are presented in Table 2. Most of the samples consisting of high proportion of gum

Arabic with starch had excellent emulsion stability which ranged from 0.80-1.0. Samples
ED

comprised of 100% starch (native and both OSA and Succinylated modified) showed slight
PT

phase separation after 24 hours. The emulsion stability for 100% OSA modified sample was

found to be 0.63, 0.73 for 100% native and 0.77 for 100% succinylated starch sample. The
CE

sample containing the fractions 25:75 (GA:SUC) also resulted in low emulsion stability 0.63, as
AC

succinylated starches have more hydrophilic characteristic which resulted in low emulsion

stability as compare to both native and OSA modified starches . In current study, spray drying

process took 45-55 minutes for one batch after emulsion preparation. Minor flocculation during

this process had been observed in all samples comprising of 100% starch. Emulsions consisting

of high portion of gum Arabic had high viscosity values as compared to the samples comprising

of high portion of starch either native or modified. The highest value of 48.67m.Pa.s was

12
 ACCEPTED MANUSCRIPT

observed for the sample comprising of 75% gum Arabic along with 25% OSA starch.

Additionally, the samples containing OSA modified starch with or without gum arabic had

slightly high values of emulsion viscosities as compare to native and succinylated. This is due to

the fact that hydrophobically modified polymers such as OSA starches are also called associative

thickeners due to interactions with other polymers and surfactants in aqueous solutions. The

T
viscosity of OSA starches is generally higher than that of other substituted derivatives. This

IP
observable fact may be caused by an associative effect of the hydrophobic chains [28]. Due to

CR
the greater molecular structure of gum Arabic, emulsions comprising of high proportion of gum

arabic led to an increase in high viscosity and vice versa [29]. Whereas, the samples consisting of

US
greater proportion of starch had lowest viscosities. Results described by Chanamai and
AN
McClements [30] proposed that the rheology of concentrated emulsions (viscosity) is fairly

dependent on droplet concentration, size and shear rate, in addition to the electrostatic repulsion
M

between droplets.
ED

The emulsion droplet size is an important factor for retention of encapsulated material in spray

dried process and enhanced by reducing the mean emulsion droplet diameter. The mean diameter
PT

of the emulsions is presented in Table 2. The lowest mean diameter was observed in the sample
CE

GA: NAT (25:75) i.e. 2.36µm and highest value was observed in sample GA: SUCCI (0:100)

which is 4.88 µm. The replacement of gum arabic with starch in different samples and the
AC

modification of starch (both OSA and succi) did not make any remarkable changes in mean oil

droplet size of emulsions.

3.3. Flowing properties of spray dried microcapsules

Besides microencapsulation efficiency, flowing properties are measured in term of bulk density,

hausner ratio and carr’s index [23]. The bulk density values for the reported spray dried samples

13
 ACCEPTED MANUSCRIPT

ranged from 0.30-0.418g/ml. These values were close to those as previously observed for

microencapsulation of rosemary essential oil prepared using gum arabic as the wall material

(0.25-0.36g/ml) and for microencapsulation of rosemary essential oil using gum

arabic/starch/maltodextrin/inulin as wall materials (0.23-0.35g/ml) [21]. The hausner ratio and

Carr’s index can influence powder properties during processing and storage conditions.

T
According to the categorization (Table 2.) for flowing property of powder, all spray dried

IP
microcapsules had poor powder flowing property. The different ratios of gum arabic with native

CR
and modified sorghum starch showed little influence on Hausner and Carr’s index. However, as

compared to native and OSA starch, combinations of gum arabic with succinylated sorghum

US
starch showed little improvement in Hausner and Carr’s index. It was observed that
AN
modification of starch did not affect the flowing ability of microcapsules.
M

3.4. Moisture content

Moisture content depends on the physical and chemical properties of the wall material and core
ED

material, method of encapsulation and operating conditions thus affects the shelf life of
PT

microcapsules [22]. The moisture content of under studied microcapsules ranged from 1.85%-

3.20% as given in the Table 3. There was no significant difference (p<0.05) between the samples
CE

constituting of native and modified starches along with the gum arabic. . Therefore, the obtained
AC

results were in accordance with the results reported by B.Cuq et al., [32] who found out that in

spray drying process, higher inlet and outlet temperatures accelerated the drying rate of droplets

and resulted in low moisture content in final spray dried powder.

3.5. Hygroscopicity

Hygroscopicity is a capability of substance to absorb or adsorb and retain moisture from

surrounding. In microencapsules, the presence of moisture can affect many parameters such as

14
 ACCEPTED MANUSCRIPT

lipid oxidation, flowing property, solubility etc. The results obtained confer an idea about the

hygroscopic nature of gum Arabic and sorghum starch. As mentioned in the Table 3, the

hygroscopicity values of all the samples were in the range of 4.57%-12.80%. These results

showed that the spray dried powders can be handled with ease and feasible for storage. The

highest values were observed for the compositions comprising of high proportion of gum Arabic

T
and low proportion of sorghum starch (native and modified) and vice versa. These values of the

IP
hygroscopicity were observed due to the changes in gum Arabic content [17]. The

CR
hygroscopicity of samples consisting of native starch is lower than the samples comprising of

modified starches. These changes can be attributed to the different polarities of the wall material

US
used, highly branched structure of gum Arabic which makes the polar interactions with water
AN
easy by hydrogen bonding, amphiphilic nature of OSA and hydrophilic nature of succinylated

starches.
M

3.6. Cold Water Solubility

ED

Water solubility of the nutmeg microcapsules varied from 2.72%-75.20% with the highest values
PT

observed for the samples having high percentage of gum arabic (Table 3). With the increase in

starch proportion in all samples, the percent water solubility decreases and least value was
CE

observed for the samples consisting of 100% native, OSA and succinylated starches. Sample A
AC

constituting of 75% gum Acacia with 25% native and 25% modified starches (OSA and

succinylated) had the highest values for water solubility. This is due to the fact that gum arabic is

a complex hydrocolloid with brilliant water soluble attribute and consists of highly branched

arrangement of the simple sugars galactose, arabinose, rhamnose, and glucuronic acids [7].On

the other hand, native starch granules are insoluble in cold water due to the hydrogen bonds and

crystallinity of the molecule. On commercial basis, the level of monosubstitution in starch

15
 ACCEPTED MANUSCRIPT

polymer is in low range; consequently, it doesn't influence the overall hydrophilicity of starch

granules that’s why very slight variation in water solubility was observed among native and

modified starch samples.

3.7. Powder wettability

The capability of spray dried microcapsules to combine with water is one of the most important

T
IP
physical characteristics associated with reconstitution with water. In fact, powder rehydration is a

CR
quality determining aspect and it is directly affected by the molecular interaction between two

phases [32]. In current study, the time taken for spray dried powders to become fully wet and

US
disappearance from the surface was used to evaluate the extent of wettability [20]. Powder

wettability of spray dried microcapsules ranged from 3sec-688sec (Table 3). The powder
AN
samples comprising of high proportion of gum Arabic took more time to disappear from surface
M

while samples consisting of sorghum starch (native or modified) as a whole, settled immediately.

This is due to the fact that starch samples (native and modified) had high density as compared to
ED

gum Arabic .Powder Wettability depends on powder particle size, type of wall materials, density,
PT

porosity, surface activity and hydrophilic nature of wall materials [33]. In present study, powder

wettability was affected by difference in proportion of gum Arabic and sorghum starch rather
CE

than type of modification of starch.

AC

3.8. Encapsulation efficiency of nutmeg microcapsules

Microencapsulation efficiency and oil retention are most important quality parameters for the

encapsulation of essential oil and is mainly determined by the content of oil retained in the dried

capsule and total oil captured inside the matrix. The amount of surface oil and entrapped oil was

first determined to estimate the EE%. The quantity of surface oil in spray dried powder is critical

16
 ACCEPTED MANUSCRIPT

for storage stability of microcapsule. This is due to the fact that surface oil can easily be oxidized

resulting in inappropriate off flavors. In obtained results (Table 4), the quantity of surface oil

ranged from 0.24-1.51g/100g of dried powder. These results revealed that the quantity of wall

materials used were sufficient for encapsulation of bulk oil. The mixtures comprising of gum

arabic and native sorghum starch showed high values of surface oil as compare to gum arabic

T
with modified starches. On the other hand, the sample containing purely native sorghum starch

IP
resulted in high surface oil as compared to sample containing of OSA and succinylated sorghum

CR
starch wholly. The amount of oil retention in obtained results ranged from 33.53-44.40% for the

mixtures containing succinylated sorghum starch, 42.10-71.40% for mixtures of OSA starch and

US
58.55-95% for native sorghum starch along with gum arabic. The sample GA: NAT (25:75)
AN
showed the highest value for oil retention i.e. 95% oil retention as compared to all other samples.

In this study, the substitution of sufficient amount of gum arabic by native and OSA modified
M

sorghum starch resulted in better oil retention. The lower values of oil retention were observed in
ED

sample comprising of 100% succinylated sorghum starch and mixture of gum arabic along with

succinylated starch. This is due to the fact that succinylation of starch leads to addition of
PT

hydrophilic negatively charged succinyl groups which gives hydrophilic nature to that starch
CE

[28]. The encapsulation efficiency for all the samples varied from 74.46-95.38%. On other hand,

50.52-83.60% EE was observed by Kausadikar [34] by using gum arabic, modified starch and
AC

maltodextrin for lemon oil. In current study, the sample containing GA: OSA starch resulted in

higher EE%, good retention of oil and lower surface oil in comparison with the samples

comprising of gum arabic with native sorghum starch that showed a high encapsulation and oil

retention but also resulted in slightly higher values for surface oil then previous samples and

native compared to insignificantly differ from succinylated starch

17
 ACCEPTED MANUSCRIPT

3.9. Peroxide value

The oxidative stability of nutmeg oleoresin encapsulated in different combinations of binary wall

system comprising of gum arabic and sorghum starch at 4⁰C and 25⁰C was calculated by their

peroxide values (PV). The results are shown in fig 1, for oxidative stability of microcapsules

correspond to native, OSA and SUC starch as wall material with gum arabic. The peroxide value

T
IP
of bulk oil at both temperatures in comparison to encapsulated oil was evaluated for 6 weeks. At

1st day, the bulk oil at both temperature had the starting PV of 0.0766 meqv kg-1 and 0.0805

CR
meqv kg-1 respectively while all the encapsulated samples showed the PV lower than bulk oil

US
ranged from 1.21x10-4 meqv kg-1 for the sample GA: NA (25:75) and 7.5x10-4 meqv kg-1 for the

sample comprising of native starch only. The most elevated value for bulk oil at 4⁰C for PV was
AN
observed on 3rd week that was 2.3229 meqv kg-1 while for 25⁰C; the elevated value observed
M

was 1.992 meqv kg-1 on 4th week. All the encapsulated samples showed that there is no
ED

significant increase in the PV in all the samples during six weeks of study. The results showed

that encapsulated samples were stable during six weeks of storage at ambient and refrigerated
PT

temperatures. The peroxide value was slightly decreased in bulk oil sample after 3 rd and 4th week
CE

at both refrigerated and ambient temperatures. This implies that all the different combinations of

gum arabic with native and modified sorghum starch samples were more stable against oxidation
AC

than bulk oil. Similar to the present work Frascareli, et al., [19]; Bae and Lee [27] observed that

bulk and encapsulated coffee and avocado oil were stable during storage under refrigeration and

at room temperature as compare to oil samples stored at 60⁰C as peroxide index increased at

higher temperatures. Oxygen is of main concern in the formation of primary oxidation products

and controlling these reactions is important to avoid off flavor formation in foods. In bulk fats

and oils, mechanism of oxidations is well known as compared to the dispersed liquid phase

18
 ACCEPTED MANUSCRIPT

which is complicated due to different compositional and structural behavior. There are many

factors which affected the oxygen permeability of the wall matrix and determined the oxidative

stability of the core material. These factors include porosity of wall material, biopolymer

composition, moisture content and glass transition temperature of biopolymers [27], [36]. Pores

were not observed in the morphology of spray dried powders and microcapsules showed low

T
moisture content. Therefore, the permeability of oxygen is limited which in turn minimized the

IP
lipid oxidation. In carbohydrate glasses, such as starch, transportation of oxygen is minimized by

CR
solubility and diffusion of oxygen which in turn is affected by the amount of water content

present in carbohydrates. Considering all these facts, it can be concluded that the whole

US
encapsulating system has reduced the lipid oxidation by interrupting oxygen permeation.
AN
3.10. Powder morphology
M

It is important to characterize microstructure of spray dried powder because many properties of

microencapsulated systems for example flow properties, entrapment of core material and
ED

protection of core material from the surroundings depends upon their morphology. Fig 2a, 2b and
PT

2c shows the SEM microstructures (external) of microcapsules produced with different

combinations of gum arabic and sorghum starch (native and modified). All powder samples
CE

involved approximately sphere-shaped particles with a diameter in a range of 5-22μm. The

AC

powder samples showed spherical shape microgranules with various sizes which is the typical

characteristic of spray dried powder [19]. The microgranules have no apparent crack, holes and

fracture on external surfaces which concluded that capsules have lower permeability to gases,

enhanced protection and retention of core material. The samples comprising of 75% gum arabic

along with 25% native and modified starches (OSA and succinylated) showed spherical shape

with extensive dented surfaces while smoothness on the surface of powder samples improved as

19
 ACCEPTED MANUSCRIPT

the percentage of starch (native and modified) increased in each sample. Round and smooth

surfaces with no dents was observed in samples consisting of native and modified starches as a

whole. It is suggested that depressions are formed as a result of mechanical stress encouraged by

irregular drying at different parts of the liquid droplets produced during the early stages of spray

drying, to the transfer of moisture during the non saturated surface drying period and as a result

T
of surface tension-viscous flow [35]. The particle size distribution of spray dried microcapsules

IP
is shown in figure 3a, 3b and 3c. Most of the curves showed three distinct peaks while few

CR
presented bimodal behavior (two peaks). Most of the particles were observed to have first broad

peak corresponding to mean particle diameter of approximately 1-5µm. The samples comprised

US
of 100% starch (both native and modified) and showed broad peaks between 5-10µm. Similar
AN
results were also obtained by Fernandes et al., [20]. The author observed that the particle size

was significantly affected by the type of wall material and resulted in largest particle size when
M

starch was used [21].The particle size distribution for the spray dried microcapsules of samples
ED

GA: NAT (75:25), (50:50), (25:75) and (0:100) ranged from (2.8-14.3) µm, (2.2-19.8) µm, (2.0-

21.9) µm and (3.7-18.5) µm respectively. For the microcapsules comprising of OSA modified
PT

starch, the particle size for spray dried microcapsules of sample GA: OSA (75:25), (50:50),
CE

(25:75) and (0:100) ranged from (2.4-11.6) µm, (2.3-18.1) µm, (1.3-19.0) µm and (6.8-21.04)

µm respectively. The particle size distribution for the spray dried microcapsules of samples GA:
AC

SUCCI (75:25), (50:50), (25:75) and (0:100) ranged from (2.0-23.1) µm, (2.7-22.7) µm, (2.1-

30.6) µm and (2.6-19.4) µm, respectively.

Conclusion

In current study, it was possible to encapsulate nutmeg oleoresin by spray drying method using

gum arabic, native sorghum starch and modified sorghum starch (succinylated and OSA) as wall

20
 ACCEPTED MANUSCRIPT

materials. Most of the emulsion formulations showed better stability after 24 h except the blends

comprising of starch as a whole. The spray dried nutmeg microcapsules had poor flowing

properties but contained lower moisture content values. While hygroscopicity, cold water

solubility and powder wettability decreased as the ratio of gum arabic decreased. The spray dried

powder samples showed spherical shaped microgranules with various sizes with no apparent

T
crack, holes and fracture on external surfaces. The studied wall matrices comprising of 25%

IP
OSA sorghum starch with 75% gum arabic and 75% native sorghum starch along with 25% gum

CR
arabic resulted in high oil retention and encapsulation efficiency. Based on results, it could be

concluded that native sorghum starch and octenyl succinic anhydride (OSA) starch, in different

US
combinations with gum arabic, is a suitable wall material for the production of nutmeg capsule
AN
with functional claims and enhancing the potential of developing novel formulations of

encapsulants.
M
ED

References

[1] S. Krishnan, R. Bhosale, R.S. Singhal, Microencapsulation of cardamom oleoresin:

PT

Evaluation of blends of gum arabic, maltodextrin and a modified starch as wall materials,
CE

Carbohyd Polym. 61(1) (2005) 95-102.

[2] S. Vaidya, R. Bhosale, R.S. Singhal, Microencapsulation of cinnamon oleoresin by spray

AC

drying using different wall materials, Drying Tech. 24(8) (2006) 983-992.

[3] R. Baranauskiene, E. Bylaite, J. Zukauskaite, R.P. Venskutonis, Flavor retention of

peppermint (Mentha piperita L.) essential oil spray-dried in modified starches during

encapsulation and storage, J. agric & food Chem. 55(8) (2007) 3027-3036.

21
 ACCEPTED MANUSCRIPT

[4] A. Gharsallaoui, G. Roudaut, O. Chambin, A. Voilley, R. Saurel, Applications of spray-

drying in microencapsulation of food ingredients: An overview, Food Res. Intl. 40(9) (2007)

1107-1121.

[5] F. Nazzaro, P. Orlando, F. Fratianni, R. Coppola, Microencapsulation in food science and

biotechnology, Current Opinion in Biotech. 23(2) (2012) 182-186.

T
[6] H. Umer, H. Nigam, A.M. Tamboli, M.S.M. Nainar, Microencapsulation: Process, techniques

IP
and applications, Intl. J. Res. pharma. and biomed. Sci. 2(2) (2011) 474-481.

CR
[7] S. Bansode, S. Banarjee, D. Gaikwad, S. Jadhav, R. Thorat, Microencapsulation: a review,

Intl. J. Pharma. Sci. Review and Res. 1(2) (2010) 38-43.

US
[8] B. Raghavan, K. Abraham, M. Shankaranarayana, Encapsulation of spice and other flavour
AN
materials, Ind. Perfumer 34(1) (1990) 75-85.

[9] B. Sankarikutty, M. Sreekumar, C. Narayanan, A. Mathew, Studies on microencapsulation of

M

cardamom oil by spray drying technique, J. Food Sci. Tech. 25(6) (1988).
ED

[10] G.A. Reineccius, Spray-drying of food flavors, ACS Publications (1988).

[11] J. Loksuwan, Characteristics of microencapsulated β-carotene formed by spray drying with

PT

modified tapioca starch, native tapioca starch and maltodextrin, Food hydrocoll. 21(5) (2007)
CE

928-935.

[12] V.G. Reddy, H. Upadhyaya, C. Gowda, Current status of sorghum genetic resources at
AC

ICRISAT: their sharing and impacts, Intl. Sorghum and Millets Newsletter 47 (2006) 9-13.

[13] S. Mehboob, T.M. Ali, F. Alam, A. Hasnain, Dual modification of native white sorghum

(Sorghum bicolor) starch via acid hydrolysis and succinylation, LWT-Food Sci. Tech. 64(1)

(2015) 459-467.

22
 ACCEPTED MANUSCRIPT

[14] M. Assagaf, P. Hastuti, C. Hidayat, S. Yuliani, S. Supriyadi, Characteristics of

microencapsulated nutmeg oleoresin: determination of Encapsulant whey protein concentrate

(WPC) : maltodextrin (MD) ratio. J. Agritech, (2013) 33 (01).

[15] A. Moin, T.M. Ali, A. Hasnain, Effect of succinylation on functional and morphological

properties of starches from broken kernels of Pakistani Basmati and Irri rice cultivars, Food

T
Chem. 191 (2016) 52-58.

IP
[16] O. Wurzburg, Acetylation, Methods in carbohyd. Chem. 4 (1964) 286-288.

CR
[17] R. Bhosale, R. Singhal, Process optimization for the synthesis of octenyl succinyl derivative

of waxy corn and amaranth starches, Carbohyd. Polym. 66(4) (2006) 521-527.

US
[18] C.I. Park, W.-G. Cho, S.J. Lee, Emulsion stability of cosmetic creams based on water-in-oil
AN
high internal phase emulsions, Korea-Australia Rheology J. 15(3) (2003) 125-130.

[19] E. Frascareli, V. Silva, R. Tonon, M. Hubinger, Effect of process conditions on the

M

microencapsulation of coffee oil by spray drying, Food bioproducts processing 90(3) (2012) 413-
ED

424.

[20] R.V. de Barros Fernandes, S.V. Borges, D.A. Botrel, Gum arabic/starch/maltodextrin/inulin
PT

as wall materials on the microencapsulation of rosemary essential oil, Carbohyd. Polym. 101
CE

(2014) 524-532.

[21] J. Singh, N. Singh, Studies on the morphological and rheological properties of granular cold
AC

water soluble corn and potato starches, Food hydrocoll. 17(1) (2003) 63-72.

[22] Y. Cai, H. Corke, Production and Properties of Spray‐dried Amaranthus Betacyanin

Pigments, J. Food Sci. 65(7) (2000) 1248-1252.

[23] F. Xue, C. Li, Y. Liu, X. Zhu, S. Pan, L. Wang, Encapsulation of tomato oleoresin with zein

prepared from corn gluten meal, J. Food Eng. 119(3) (2013) 439-445.

23
 ACCEPTED MANUSCRIPT

[24] L. Tan, L. Chan, P. Heng, Effect of oil loading on microspheres produced by spray drying,

J. Microencapsulation 22(3) (2005) 253-259.

[25] R.E. Wrolstad, Current protocols in Food Analyt. Chem., Wiley2001.

[26] R. Partanen, J. Raula, R. SEPPAnen, J. Buchert, E. Kauppinen, P. Forssell, Effect of relative

humidity on oxidation of flaxseed oil in spray dried whey protein emulsions, J. Agri. Food

T
Chem. 56(14) (2008) 5717-5722.

IP
[27] E. Bae, S. Lee, Microencapsulation of avocado oil by spray drying using whey protein and

CR
maltodextrin, J. Microencapsulation 25(8) (2008) 549-560.

[28] D. Ackar, J. Babic, A. Jozinovic, B. Milicevic, S. Jokic, R. Milicevic, M. Rajic, D. Subaric,

US
Starch modification by organic acids and their derivatives: A Review, Molecules 20(10) (2015)
AN
19554-19570.

[29] C. Chranioti, C. Tzia, Arabic gum mixtures as encapsulating agents of freeze-dried fennel
M

oleoresin products, Food Bioprocess Tech. 7(4) (2014) 1057-1065.

ED

[30] R. Chanamai, D. McClements, Comparison of gum arabic, modified starch, and whey

protein isolate as emulsifiers: influence of pH, CaCl2 and temperature, J. Food Sci. 67(1) (2002)
PT

120-125.
CE

[31] S. Veprek, M. Haussmann, S. Reiprich, L. Shizhi, J. Dian, Novel thermodynamically stable

and oxidation resistant superhard coating materials, Surface Coatings Tech. 86 (1996) 394-401.
AC

[32] B. Cuq, E. Rondet, J. Abecassis, Food powders engineering, between knowhow and science:

constraints, stakes and opportunities, Powder Tech. 208(2) (2011) 244-251.

[33] C. Vega, Y. Roos, Invited review: spray-dried dairy and dairy-like emulsions—

compositional considerations, J. Dairy Sci. 89(2) (2006) 383-401.

24
 ACCEPTED MANUSCRIPT

[34] S. Kausadikar, A.D. Gadhave, J. Waghmare, Microencapsulation of lemon oil by spray

drying and its application in flavour tea, Adv. Appl. Sci. Res 6 (2015) 69-78.

[35] D. Moreau, M. Rosenberg, Microstructure and fat extractability in microcapsules based on

whey proteins or mixtures of whey proteins and lactose, Food Structure 12(4) (1993) 6.

T
IP
CR
US
AN
M
ED
PT
CE
AC

25
 ACCEPTED MANUSCRIPT

Figure caption

Fig. 1. Oxidation stability of bulk and encapsulated nutmeg oil in microcapsules at 4⁰C and

25⁰C. NAT A: gum arabic75% & native sorghum starch 25%; NAT B: gum Arabic 50% &

native sorghum starch 50%; NAT C: gum arabic 25% & native sorghum starch 75%; NAT D:

100% native sorghum starch; OSA A: gum arabic 75% & modified OSA starch 25%; OSA B:

T
gum arabic 50% & modified OSA sorghum starch 50%; OSA C: gum arabic 25% & modified

IP
OSA sorghum starch 75%; OSA D: 100% modified OSA sorghum starch; SUC A: gum

CR
arabic75% and modified succinylated sorghum starch 25%; SUC B: gum arabic 50% and

US
modified succinylated sorghum starch 50%; SUC C: gum Arabic 25% and modified succinylated

sorghum starch 75%; SUC D: 100% modified succinylated sorghum starch

AN
Fig. 2a. SEM of the nutmeg microcapsules prepared from (a) gum arabic 75% & native

sorghum starch 25% , (b) gum arabic 50% & native sorghum starch 50%, (c) gum arabic 25%
M

& native sorghum starch 75%, (d) 100% native sorghum starch.
ED

Fig. 2b. SEM of the microcapsules prepared from a) gum arabic 75% & modified OSA starch
PT

25%, (b) gum arabic 50% & modified OSA sorghum starch 50%, (c) gum arabic 25% &

modified OSA sorghum starch 75%, (d) 100% modified OSA sorghum starch
CE

Fig. 2c. SEM of the microcapsules prepared from a) gum arabic 75% & modified succinylated

sorghum starch 25%, (b) gum arabic 50% & modified succinylated sorghum starch 50%, (c) gum
AC

arabic 25% & modified succinylated sorghum starch 75%, (d) 100% modified succinylated

sorghum starch.

Fig. 3a. Particle size distribution of the nutmeg microcapsules prepared from (a) gum arabic

75% & native sorghum starch 25% , (b) gum arabic 50% & native sorghum starch 50%, (c)

gum arabic 25% & native sorghum starch 75%, (d) 100% native sorghum starch.

26
 ACCEPTED MANUSCRIPT

Fig. 3b. Particle size distribution of the microcapsules prepared from a) gum arabic 75% &

modified OSA starch 25%, (b) gum arabic 50% & modified OSA sorghum starch 50%, (c) gum

arabic 25% & modified OSA sorghum starch 75%, (d) 100% modified OSA sorghum starch

Fig. 3c. Particle size distribution of the microcapsules prepared from a) gum arabic 75% &

T
modified succinylated sorghum starch 25%, (b) gum arabic 50% & modified succinylated

IP
sorghum starch 50%, (c) gum arabic 25% & modified succinylated sorghum starch 75%, (d)

CR
100% modified succinylated sorghum starch

US
AN
M
ED
PT
CE
AC

27
 ACCEPTED MANUSCRIPT

Table 1

Degree of substitution of chemically modified white Sorghum starches and particle size analysis a

Starch Degree of substitution (DS) Particle size d4,3(µm)

Native sorghum starch ND* 12.56±0.07a

T
OSA sorghum starch 0.0232±0.00a 13.65±0.03b

IP
Succinylated sorghum starch 0.0709±0.08b 12.41±0.04a

CR
a
Values are the mean of three different replications. Different superscript letters within first column are significantly

different at p<0.05 by using T-test.

US
*Not Determined
AN
M
ED
PT
CE
AC

28
 ACCEPTED MANUSCRIPT

Table 2

Mean values and standard deviations for emulsion stability, viscosity, mean droplet size and flowing properties of nutmeg microcapsules a

Emulsion Emulsion Emulsion Bulk

P THausner Car’s index

Samples stability droplet size viscosity density

R I ratio

1.00±0.00d
d3,2(µm)

2.82±0.00d
(mPa.s)

44.67±9.29a,b
C
(gm/ml)

S
0.356±0.04d 1.67±0.023d 39.93±1.65d
GA:NAT(75:25)

GA:NAT(50:50) 0.90±0.00c 2.42±0.00b

N U
34.33±9.71b,c,d,e 0.358±0.04b 1.52±0.035b 34.13±1.47c

1.00±0.00d 2.36±0.00a A
32.00±2.00b,c,d 0.418±0.04d 1.65±0.035d 39.39±1.50d
GA:NAT(25:75)
M
GA:NAT(0:100) 0.73±0.06b 3.30±0.00h

E D 26.67±5.90a,b 0.398±0.04c 1.61±0.08c,d 38.67±2.7b,c

GA:OSA(75:25) 0.90±0.00c

0.80±0.00b P T
2.62±0.00c

3.63±0.00i
48.67±12.58e

44.00±9.64d,e
0.302±0.04c

0.331±0.04b
1.53±0.036b,c

1.68±0.03b,c
34.09±1.48c

40.78±1.28d
E
GA:OSA(50:50)

GA:OSA(25:75) 0.80±0.00b

C C 3.26±0.00f 42.00±10.44c,d,e 0.350±0.04b 1.55±0.062b,c 35.39±2.73c

GA:OSA(0:100)

GA:SUC(75:25)
A
0.63±0.15a

1.00±0.00d
4.31±0.00k

2.84±0.00e
30.67±5.13a,b,c,d

42.00±3.60c,d,e
0.324±0.04a

0.308±0.04d
1.48±0.046a,b

1.51±0.012b
32.36±2.22a,b,c

33.71±0.66b,c

GA:SUC(50:50) 1.00±0.00d 3.70±0.00j 34.33±4.04b,c,d,e 0.317±0.04d 1.55±0.025b,c 34.95±1.06c

29
 ACCEPTED MANUSCRIPT

GA:SUC(25:75) 0.63±0.58a 3.27±0.00g 28.67±4.75a,b,c 0.355±0.04a 1.42±0.042a 30.52±1.97a,b

GA:SUC(0:100) 0.77±0.58b 4.88±0.00l 17.00±5.20a 0.302±0.04b 1.42±0.040a 30.03±3.82a

a
Values are the mean of three different replications. Different superscript letters within each column are significantly different at p≤0.05.

GA: gum arabic; NAT: native sorghum starch; OSA: octenyl succinic anhydride sorghum starch; SUC: succinylated sorghum starch

P T
R I
S C
N U
A
M
E D
P T
C E
A C

30
 ACCEPTED MANUSCRIPT

Table 3

Mean values and standard deviations for moisture content, hygroscopicity, cold water

solubility and powder wettability of microcapsulesa

Samples Moisture Hygroscopicity Cold water Powder

content (%) (%) solubility (%) wettability

T
IP
(min)

CR
GA:NAT(75:25) 1.94±0.6a 11.06±0.82d,e 75.20±2.45f 8.14±0.91e,f

GA:NAT(50:50) 2.10±0.4a 9.80±1.15c,d,e 51.01±0.95d 5.43±0.51d

US
GA:NAT(25:75) 1.95±0.15a 5.64±1.01a 27.33±6.38b,c 3.48±0.67b
AN
GA:NAT(0:100) 1.85±0.61a 4.57±0.41a 2.72±0.67a 0.53±0.57a

GA:OSA(75:25) 2.4±0.11a 12.80±0.70g 76.79±2.19f 8.50±0.50f

M

GA:OSA(50:50) 2.6±0.28a 11.19±0.53e,f 55.90±1.67c 7.55±0.53e

ED

GA:OSA(25:75) 2.7±2.2a 9.92±0.70d,e 30.37±1.39c 4.27±0.94b,c

GA:OSA(0:100) 3.1±0.35a 8.44±1.04a,c 5.00±3.26a 0.03±0.01a

PT

GA:SUC(75:25) 3.2±0.21a 12.48±0.75f 74.44±0.97f 11.28±0.17h

CE

GA:SUC(50:50) 2.8±0.10a 10.38± 0.41d,e 53.04±1.40d,e 10.31±0.23g

GA:SUC(25:75) 2.9±0.18a 9.63±1.10c,d 24.75±1.04b 4.42±0.10c

AC

GA:SUC(0:100) 3.1±0.18a 8.14±0.10b 3.52±0.80a 0.17±0.14a

a
Values are the mean of three different replications. Different superscript letters within each column are significantly

different at p≤0.05.

GA: gum arabic; NAT: native sorghum starch; OSA: octenyl succinic anhydride sorghum starch; SUC: succinylated

sorghum starch

31
 ACCEPTED MANUSCRIPT

Table 4

Mean values for surface oil, total oil, retention of oil and encapsulation efficiency of the

Samples Surface oil Total oil Oil retention Encapsulation

(g/100g) (g/100g) (%) efficiency%

T
GA:NAT(75:25) 0.79±0.82d 6.89±0.00b 68.9±0.00d 88.51±0.91c,d

IP
GA:NAT(50:50) 0.48±0.79a,b,c 5.19±1.27a,b 58.55±7.07b,c,d 91.97±0.95d,e,f

CR
GA:NAT(25:75) 1.51±0.82f 9.50±0.71c 95±7.07e 84.07±2.07b

GA:NAT(0:100) 1.18±0.82e 6.81±2.56b 68.1±25.6d 74.46±5.53a

US
GA:OSA(75:25) 0.24±0.10a 5.21±0.28a,b 52.1±2.80a,b,c,d 95.38±0.00f
AN
GA:OSA(50:50) 0.29±0.00a 6.22±0.00a,b 62.30±0.02c,d 90.36±0.00c,d,e

GA:OSA(25:75) 0.76±0.01c,d 5.70±2.51a,b 71.4±1.98d 89.31±0.64c,d,e

M

GA:OSA(0:100) 0.635±0.10b,c,d 4.21±0.00a,b 42.10±0.00a,b 84.8±0.00b

ED

GA:SUC(75:25) 0.357±0.10a,b 4.29±0.00a,b 41.33±4.03a,b 91.68±0.96d,e,f

GA:SUC(50:50) 0.497±0.80a,b,c 3.87±0.03a 33.53±0.00a,b 87.34±1.74b,c

PT

GA:SUC(25:75) 0.375±0.82a,b 4.44±1.23a,b 44.40±12.33a,b,c 92.78±1.11e,f

CE

GA:SUC(0:100) 0.393±0.79a,b 3.7±1.06a 37.17±10.61a 90.72±0.26c,d,e

microcapsulesa
AC

a
Values are the mean of three different replications. Different superscript letters within each column are significantly

different at p≤0.05.

GA: gum arabic; NAT: native sorghum starch; OSA: octenyl succinic anhydride sorghum starch; SUC: succinylated

sorghum starch

32
 ACCEPTED MANUSCRIPT

Highlights

 Sorghum starches are considered as good alternative for microencapsulation.

 The combinations of gum arabic and OSA starch resulted in high oil retention.

 The samples were stable during six weeks of storage at 25⁰C.

T
IP
 The microgranules had no apparent crack, holes and fracture on external surfaces.

CR
US
AN
M
ED
PT
CE
AC

33
Figure 1
Figure 2a
Figure 2b
Figure 2c
Figure 3