Food Chemistry 190 (2016) 1151–1158

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Food Chemistry
journal homepage: www.elsevier.com/locate/foodchem

Comparison of spray, freeze and oven drying as a means of reducing

bitter aftertaste of steviol glycosides (derived from Stevia rebaudiana
Bertoni plant) – Evaluation of the final products
Charikleia Chranioti, Sofia Chanioti, Constantina Tzia ⇑
Laboratory of Food Chemistry and Technology, School of Chemical Engineering, National Technical University of Athens, Greece

a r t i c l e i n f o a b s t r a c t

Article history: The aim of this study was to encapsulate the steviol glycosides (SGs) by spray, freeze and vacuum oven
Received 1 April 2015 drying in order to minimise the bitter aftertaste of the SGs, as well as to improve their properties.
Received in revised form 1 June 2015 Different ratios of maltodextrin to inulin as agents were examined, 80:20, 75:25, 70:30, 65:35 and
Accepted 23 June 2015
60:40, while the concentration of SGs in total solids was maintained constant at 2.5%. The obtained
Available online 27 June 2015
SGs products were evaluated by microencapsulation efficiency (MEE%), hygroscopicity, solubility, mois-
ture content, structure (SEM, XRD), FT-IR and sensory properties. Significant differences in MEE%, mois-
Keywords:
ture content, structure and solubility values were observed depending on the applied drying method. The
Steviol glycosides
Bitter aftertaste
reduced hygroscopicity values (20.26–26.67 g H2O/100 g dry weight) contribute to improved stability.
Spray drying The FT-IR technique confirmed that SGs maintained their chemical integrity during the applied drying
Freeze drying processes. The spray dried SGs products presented the best physicochemical characteristics and the most
Oven drying appealing sensorial ones.
XRD Ó 2015 Elsevier Ltd. All rights reserved.
FT-IR
SEM

1. Introduction
Recently, stevia-based sweeteners, containing steviol glycosides
derived from Stevia rebaudiana (Bert) Bertoni plant, have gained
great attention. In contrast to other synthetic sweeteners, such as
aspartame or saccharine, that are most commonly used and
regarded either as having a mineral aftertaste or as being associ-
ated with health concerns, steviol glycosides can be used as a nat-
ural alternative sweetener (Guggisberg, Piccinali, & Schreier, 2011;
Puri, Sharma, & Tiwari, 2011).
S. rebaudiana (Bert) Bertoni plant contains several glycosides,
stevioside, rebaudioside A, B, C, D, E and dulcoside A; these glyco-
sides are about 200–300 times sweeter than sucrose (Gardana,
Scaglianti, & Simonettia, 2010). Rebaudioside A is considered to
be superior in terms of both sweetness and quality of taste,
whereas stevioside is usually perceived with a significant bitter
aftertaste (Dacome et al., 2005; Lemus-Mondaca, Vega-Galvez,
Zura-Bravo, & Ah-Hen, 2012). Steviol glycosides (SGs) are consid-
ered as non-toxic, non-mutagenic, non-caloric, also being capable
of treating diseases, such as hypoglycaemia, candidiasis, high
blood pressure and skin abrasions (Alupului, Calinescu, & Lavric,
⇑ Corresponding author.
E-mail address: tzia@chemeng.ntua.gr (C. Tzia).
2009; Kim, Yang, Lee, & Kang, 2011). They can therefore be con-
sumed by patients suffering from diabetes and other diseases
related to disturbances in carbohydrate metabolism (Bondarev,
Reshetnyak, & Nosov, 2001; Lemus-Mondaca et al., 2012; Puri
et al., 2011).
Nevertheless, the inadequate use of steviol glycosides in food
applications, involving heating (such as baking) or a controlled
release of the sweet taste, could require the application of an
encapsulation technique. In particular, for sweetener products,
microencapsulation technique is usually applied in order to mask
off-flavours and control the release of the encapsulated com-
pounds under pre-established conditions (Shahidi & Han, 1993;
Sun-Waterhouse & Wadhwa, 2013). Moreover, it can increase the
stability of the products under adverse environmental conditions,
by reducing their hygroscopicity and reactivity and by offering
resistance to high temperatures (Favaro-Trindade, Santana,
Monterrey-Quintero, Trindade, & Netto, 2010; Rocha-Selmi,
Bozza, Thomazini, Bolini, & Fávaro-Trindade, 2013).
The microencapsulation process consists of the preparation of
the emulsion or dispersion that contains the agent and the core
material, which is then dried, commonly using spray or
freeze-drying techniques (Lim, Tan, Bakar, & Ng, 2011). Spray
drying is one of the most extensively used microencapsulation
methods, due to the wide availability of the equipment, low

http://dx.doi.org/10.1016/j.foodchem.2015.06.083
0308-8146/Ó 2015 Elsevier Ltd. All rights reserved.
1152 C. Chranioti et al. / Food Chemistry 190 (2016) 1151–1158
processing costs, large variety of materials used as encapsulating
agents and good stability obtained for the final products
(Dzondo-Gadet, Nzikou, Etoumongo, & Desobry, 2005; Ma
et al., 2014). Freeze drying, on the other hand, carried out at
low temperatures and at absence of air, is an attractive method
for extending the shelf life of food products that prevents pro-
duct deterioration caused by oxidation or chemical modification
(Anwar & Kunz, 2011).
The selection of a proper encapsulation agent is of high impor-
tance for an efficient encapsulation process. Among the available
materials, maltodextrins are widely used as encapsulation agents,
since they possess a good compromise between cost and effective-
ness (Apintanapong & Noomhorm, 2003). Inulin, a mixture of
oligo- and polysaccharides, is of great interest, since it is often used
as a bulking agent in the production of sugar-free products, while
having an additional advantage as a dietary fibre (Zahn, Forker,
Krügel, & Rohm, 2013). Due to aforementioned functional proper-
ties and its low price inulin has drawn attention in food applica-
tions (Saénz, Tapia, Chávez, & Robert, 2009).
In our previous work (Chranioti, Chanioti, & Tzia, 2015), it has
been found that the bitterness of steviol glycosides (SGs), as eval-
uated by sensory tests, diminished when encapsulated with mal-
todextrin and inulin, using the spray drying technique. Although
many studies, have tested the performance of different extraction
and purification methods for obtaining steviol glycosides (SGs)
extracts (Bondarev et al., 2001; Dacome et al., 2005; Gardana
et al., 2010; Lemus-Mondaca et al., 2012; Puri et al., 2011;
Tadhani, Patel, & Subhash, 2007), several have dealt with the use
of SGs in food applications (Garcia-Noguera, Weller, Oliveira,
Rodrigues, & Fernandes, 2010; Guggisberg et al., 2011). No reports
were found in the literature about research involving the use of
microencapsulation techniques in order to reduce/mask the bitter
aftertaste of steviol glycosides and further utilise their function as
sweetener.
Therefore, the aim of this study was to attenuate the bitter
aftertaste of steviol glycosides by applying spray, freeze and vac-
uum oven drying, and using maltodextrin (MD-19DE) and inulin
(IN) as the encapsulating agents. The above agents were examined
in different ratios (80–20, 75–25, 70–30, 65–35 and 60–40), while
the concentration of steviol glycosides in total solids was kept con-
stant at 2.5% (Chranioti et al., 2015). The final encapsulated prod-
ucts were evaluated in terms of hygroscopicity, solubility,
moisture content, microencapsulation efficiency and sensory prop-
erties in syrup form, while the viscosity, refractive index and tur-
bidity of the produced syrups were also tested. Furthermore, the
structure and morphology of the final products were investigated
by X-ray diffraction (XRD) and scanning electron microscopy
(SEM) analysis. Finally, through Fourier Transform Infrared spec-
troscopy (FT-IR) technique became possible the characterisation
of the changes in the molecular structure of the glycosides into
the system of the final products.
2. Materials and methods
2.1. Materials
The steviol glycosides (SGs), containing stevioside (57.12%) and
rebaudioside A (24.78%), were generously donated by NL⁄ Stevia
and used as the core material. Inulin, IN, (Fibrulose F97) and mal-
todextrin, MD, from Waxy Maize (19 DE), were obtained from
Astron Chemicals S.A. and Chemicotechnica S.A., respectively and
used as the encapsulating agents. Rebaudioside A, RA, (98% purity)
was provided by NL⁄ Stevia and used as a standard. All chemicals
used were of analytical reagent (AR) grade.
2.2. Production of the encapsulated SGs products
The production method of the encapsulated steviol glycoside
products by applying spray, freeze and oven drying is presented
in Fig. 1.
2.2.1. Dispersion preparation
Initially, the maltodextrin (19 DE) and inulin agents were dis-
persed at 65 °C for 15 min under constant stirring. Then, steviol
glycosides (SGs) were added and mixed, using an homogenizer
(Unidrive X 1000, CAT, Staufen, Germany) for 5 min at
10,000 rpm (Ortiz et al., 2009) at room temperature, until complete
dispersion of the solids was achieved. Three dispersion samples
were prepared and each of them was separately fed to a laboratory
spray, freeze dryer or to a vacuum oven. The prepared powders of
the final products were either tested immediately, or stored in
glass containers with silica gel at room temperature, until further
examination. Fifteen formulations with different ratios of mal-
todextrin to inulin (MD:IN) were examined (80:20, 75:25, 70:30,
65:35, 60:40), while the concentration of SGs in total solids was
maintained constant at 2.5% for all formulations.
2.2.2. Spray drying (SD)
The dispersion was fed to a laboratory spray dryer with a two
fluid nozzle (B-191, Büchi Mini Spray Drier, Flawil, Switzerland),
which was operated under the following conditions: inlet air tem-
perature (Tin): 160 °C, outlet air temperature (Tout): 88 °C, feed
temperature: 60 °C, air pressure: 5 bar, aspirator: 90%, pump:
40% and compressed air flow rate: 500 L/h.
2.2.3. Freeze drying (FD)
The dispersion in open Petri dishes (60 mm dish, ml of emul-
sion) was frozen overnight at 30 °C and lyophilized in a
freeze-dryer (Christ Alpha 1-4 LD Plus, Osterode, Germany) at
P = 0.017 mbar and T = 57 °C for 48 h (Chranioti & Tzia, 2013).
The dried dispersion was converted into powder using a pestle
and mortar.
2.2.4. Oven drying (OD)
The dispersion was dried in a vacuum oven (Heraeus
Instruments Vacutherm VT 6025, London, United Kingdom) for
2.5 h. The vacuum pressure was less than 20 mbar and the temper-
ature was maintained at 45 °C.
2.3. Analyses of encapsulated products
2.3.1. Moisture content
The moisture content of the encapsulated products, the agents
(maltodextrin and inulin), and the sweeteners, steviol glycosides
and sucrose, was determined gravimetrically by oven drying at
100 °C to a constant weight (AOAC, 1990).
2.3.2. Solubility
1 g of each sample was added to 100 ml of distilled water, and
stirred at 110 rpm for 30 min, before centrifuging at 4000 rpm for
5 min. Aliquots of each supernatant were then removed, trans-
ferred to previously weighed porcelain dishes, and dried to con-
stant weight in an incubator at 100 °C. The dishes were weighed
and the solubility was calculated from the difference in weight
(Cano-Chauca, Stringheta, Ramos, & Cal-Vidal, 2005).
2.3.3. Hygroscopicity
Approximately 1 g of each sample was placed in hermetic pots,
containing a saturated sodium sulphate solution (RH = 81%), and
weighed again after 7 days. The hermetic pots were kept at 25 °C
in an incubator, with controlled temperature. The hygroscopicity
 C. Chranioti et al. / Food Chemistry 190 (2016) 1151–1158
Maltodextrin from Waxy
Maize (19 DE)
Dispersion under constant
stirring
(65°C for 15 min)
Mixing in an homogenizer
for 5 min at 10,000 rpm
(Unidrive X 1000, CAT)
Freeze drying (FD) Spray Drying (SD)
Freezing: Tin= 160 °C, Tout= 88 °C
Tfeed= 60 °C,
24 h at = -30 °C
Air pressure = 5 bar
Freeze drying: Aspirator = 90 %
48 h at = -57 °C and Pump = 40 %
Compressed air flow rate = 500 L/h
P = 0.017 mbar
Fig. 1. Flow diagram of microencapsulation process of steviol glycosides (SGs) products.
was expressed as grams of water absorbed by 100 g of sample (Cai
& Corke, 2000).
2.3.4. Microencapsulation efficiency (MEE%)
The microencapsulation efficiency (MEE%) of the final products
was based on their rebaudioside A (RA) content and calculated
using HPLC analysis according to Rocha-Selmi, Theodoro,
Thomazini, Bolini, & Favaro-Trindade, 2013, as shown in Eq. (1).
MEE% ¼ ðRA in the final product=initially added RAÞ  100 ð1Þ
2.3.5. HPLC analysis
For the quantification of the rebaudioside A (RA), a HP 1100
Series gradient HPLC system (Agilent Technologies, USA) combined
with quaternary pump, diode array detector (Hewlett-Pachard,
Waldbronn, Germany) and data analysis software (ChemStation
for LC3D Software, Agilent Technologies, Waldbronn, Germany)
was employed. A column (250  4.6 mm) packed with 5 lm parti-
cles Hypersil C18 (MZ Analysentechnik, Mainz, Germany) was used
for the separation. The operating conditions for HPLC analysis were
as follows: ambient temperature, acetonitrile–water (80:20) as the
eluting solvent at a flow rate of 1 ml/min and wavelength of UV
detector, 210 nm. The standard curve of RA was prepared using
concentrations of RA between 0.05 and 0.3 mg/ml. The standard
curve was analysed using the linear least-squares regression equa-
tion derived from the peak area (regression equation
y = 5,000,000x + 93.27, r = 0.998 where y is the peak area and x
the concentration).
2.3.6. Sample preparation
To determine the encapsulated RA present in the products, 1 g
of the sample was placed in a 20 ml screw cap test tube and was
extracted by vortex mixing for 10 min, at ambient temperature,
with 10 ml of 1:1 ethanol/water. The tube was subsequently cen-
trifuged at 5000 rpm for 5 min and an aliquot of the supernatant
1153
Inulin
(Fibrulose F97)
Steviol glycosides (SGs)
Oven drying (OD)
2.5 h at = 45 °C and
P < 20 mbar
Final product
was filtered through a 0.45 lm PTFE filter and used for quantifica-
tion of the RA.
2.3.7. Fourier-transform infrared spectroscopy (FT-IR)
The final products of steviol glycosides (SGs) and a sample pre-
pared by mechanical mixing of the three solid constituents of mal-
todextrin, inulin and steviol glycosides at an equivalent
formulation (physical mixture, PM) were characterised by infrared
spectroscopy in the region from 4000 to 400 cm1, using a FT-IR
spectrometer (FT-IR 4000 JASCO, Tokyo, Japan).
2.3.8. Scanning electron microscopy (SEM)
To study the morphological properties of the final products of
steviol glycosides (SGs), a scanning electron microscope (Quanta
200, FEI with LFD Detector) was used. Particles were loaded onto
a specimen stub, coated with gold with a sputter coater.
Examinations were made at 200 magnification.
2.3.9. X-ray diffraction analysis (XRD)
The crystallinity structure of the final products was charac-
terised by X-ray diffractometry. The analysis was conducted using
an X-ray diffractometer (Bruker D8-Advance), in which X-ray
source was radiation CuKa (k = 1.5418 Å), with 20 kV and 10 mÅ,
measured at angle 2h, ranging between 2° and 100° with a scan-
ning rate of 0.1 °/s.
2.4. Aqueous solutions (syrups) analyses
Aqueous solutions (syrups) were prepared with the final SGs
products in water at 1% w/v. The prepared syrups were tested for
viscosity, refractive index and turbidity. Sensory evaluation was
also conducted.
2.4.1. Viscosity
Viscosities of the syrups were measured using Brookfield
DV-II + Pro viscometer at 25 °C, with a sample volume of 50 ml
1154 C. Chranioti et al. / Food Chemistry 190 (2016) 1151–1158

Table 1
Microencapsulation efficiency and properties of the steviol glycosides (SGs) products.

Sample MEE %a Moisture content % Solubility % Hygroscopicityb

Spray drying (SD)
SD80-20 82.46 ± 1.60 e 7.99 ± 0.04 h 97.50 ± 0.10 g 26.67 ± 0.18 f
SD75-25 78.40 ± 2.30 cde 6.89 ± 0.12 ab 97.33 ± 0.06 ig 24.25 ± 0.1 de
SD70-30 76.50 ± 1.28 bcde 7.03 ± 0.08 bc 96.83 ± 0.29 ig 27.78 ± 0.04 f
SD65-35 71.24 ± 1.43 abcd 7.45 ± 0.10 de 96.70 ± 0.17 hi 21.51 ± 1.6 ab
SD60-40 63.72 ± 8.71 a 6.72 ± 0.06 a 96.03 ± 0.02 gh 20.26 ± 0.12 a
Freeze drying (FD)
FD80-20 82.05 ± 6.53 e 6.78 ± 0.16 a 95.94 ± 0.02 g 20.33 ± 0.21 a
FD75-25 79.23 ± 3.46 de 7.36 ± 0.05 d 92.33 ± 0.31 f 23.33 ± 1.8 cde
FD70-30 77.23 ± 1.76 bcde 7.58 ± 0.13 ef 90.86 ± 0.08 e 24.18 ± 0.13 de
FD65-35 73.51 ± 2.23 bcde 7.69 ± 0.06 fg 90.18 ± 0.04 de 24.45 ± 0.06 e
FD60-40 68.98 ± 1.12 abc 7.84 ± 0.17 gh 89.56 ± 0.08 d 22.23 ± 0.1 bc
Oven drying (OD)
OD80-20 80.92 ± 0.53 de 7.17 ± 0.12 c 89.85 ± 0.07 d 23.06 ± 0.16 cde
OD75-25 78.69 ± 7.47 cde 7.61 ± 0.08 ef 88.73 ± 0.04 c 21.39 ± 0.22 ab
OD70-30 75.08 ± 11.94 bcde 7.69 ± 0.14 fg 87.08 ± 0.03 b 22.86 ± 0.24 cd
OD65-35 72.09 ± 4.03 abcd 7.73 ± 0.06 fg 87.03 ± 0.01 b 23.75 ± 0.14 de
OD60-40 68.23 ± 3.95 ab 8.21 ± 0.18 i 84.01 ± 1.53 a 24.17 ± 1.6 de
Raw material
MDc – 6.28 ± 0.03 88.21 ± 0.10 24.95 ± 0.09
INd – 19.9 ± 0.07 76.32 ± 0.08 53.06 ± 0.11
SGe – 41.5 ± 0.12 62.46 ± 0.09 89.22 ± 0.07

Means within the same column followed by different letters (a,b,c) are significantly different (P < 0.05).
a
MEE: microencapsulation efficiency.
b
g H2O/100 g dry weight.
c
MD: maltodextrin.
d
IN: inulin.
e
SG: steviol glycosides.

operating at 100 rpm using a spindle set of S61 (Kshirsagar, Yenge, intensity and 0 (minimum) – 10 (maximum) for bitter aftertaste
Sarkar, & Singhal, 2009). and overall acceptance, respectively.

2.4.2. Refractive index 2.5. Statistical analysis

The refractive index of the syrups was determined in visible
light, using a refractometer (BOE 32400 ABBE, Boeco, Germany)
range of measurement: 1.300–1.700, accuracy: ±0.0002. The mea-
surements were carried out at ambient temperature.
2.4.3. Turbidity
The turbidity of the syrups was measured by a Turbimeter
(Hach 2100 N, Loveland, Co, USA). For the measurement, 20 ml of
the samples were poured into a glass cell, while the temperature
was set at 25 °C. The values of turbidity are given in NTU
(Nephelometric Turbidity Units) which are the most common tur-
bidity units.
2.4.4. Sensory evaluation
The sensory evaluation of the encapsulated SGs products, in the
form of syrups, was carried out in the accredited (ISO 17025) sen-
sory laboratory of NTUA, which is equipped with individual booths.
The panellists had been trained in sensory analysis and had former
experience in accessing sweetener samples. The evaluation of the
final products was carried out according to the literature
(Pangborn, 1963; Parpinello, Versari, Castellari, & Galassi, 2001;
Ye et al., 2013) with some modifications. In particular, the samples
of the SGs products were dissolved in drinking water and diluted to
a concentration of 1 g/100 ml, while sucrose, as well as SGs, were
prepared at concentrations of 10 and 1 g/100 ml, respectively,
and used as controls. The samples were served as 100 ml aliquots,
in 300 ml odour-free paper cups, at room temperature (25 °C) and
analyses were performed in individual tasting booths under nor-
mal lighting conditions. Panellists were instructed to rinse their
palates between samples. The evaluated parameters were sweet
intensity, bitter aftertaste and overall acceptance while the score
scale applied was: 0 (minimum) – 5 (maximum) for sweet
The experiments were carried out in triplicate. The resulting
data was assessed by analysis of variance (ANOVA) using
STATISTICA 7 (Statsoft Inc., Tulsa, USA). Duncan’s test was used
for significant differences at the probability level P < 0.05.
3. Results and discussion
3.1. Evaluation of microencapsulation efficiency (MEE%)
The microencapsulation efficiency (MEE%) of the final steviol
glycosides (SGs) products was estimated based on their content
in glycoside rebaudioside A (RA). According to the obtained results
(Table 1), the microencapsulation efficiency varied from 63.72% to
82.46%, regardless of the drying method used. It was observed that
the MEE was significantly influenced by the ratio of the agents
used (P < 0.05) and not by the applied drying method. In particular,
the ratio of 80–20 resulted in the highest recorded MEE values of
82.46%, 82.05% and 80.92% for spray, freeze and oven dried sam-
ples, respectively.
3.2. Study of the steviol glycosides (SGs) products’ properties
Among the studied properties of the steviol glycosides (SGs)
products, the moisture content presented values within the
expected range for sweetener powdered products (Rocha-Selmi
and Theodoro et al., 2013; Rocha-Selmi and Bozza et al., 2013),
ranging from 6.72 to 8.21 for SD60-40 and OD60-40 samples, respec-
tively (Table 1). The moisture content was significantly affected
only by the applied drying method (P < 0.05), with oven drying
exhibiting the highest average moisture content value of 7.68%.
Regarding hygroscopicity, its values ranged from between 20.26
 C. Chranioti et al. / Food Chemistry 190 (2016) 1151–1158 1155

Table 2
Physicochemical and sensory properties of aqueous solutions (syrups) of SGs products.

Sample Viscosity (mPas) Turbidity (NTU) Intensity of sweetness Bitter aftertaste Overall acceptance
Spray drying (SD)
SD80-20 3.02 ± 0.13 a 2.67 ± 0.58 a 4.33 ± 0.29 cd 3.50 ± 0.00 abce 8.67 ± 0.29 g
SD75-25 3.34 ± 0.03 ab 4.00 ± 1.73 a 4.33 ± 0.58 cd 3.43 ± 0.06 abc 8.63 ± 0.15 g
SD70-30 3.26 ± 0.19 ab 4.33 ± 0.58 a 4.50 ± 0.50 d 3.47 ± 0.42 abc 8.50 ± 0.00 fg
SD65-35 3.04 ± 0.03 a 5.00 ± 0.00 a 4.17 ± 0.29 bcd 3.30 ± 0.26 ab 8.53 ± 0.12 fg
SD60-40 3.12 ± 0.01 ab 4.67 ± 0.58 a 4.00 ± 0.00 abcd 3.17 ± 0.29 a 8.17 ± 0.29 ef
Freeze drying (FD)
FD80-20 3.08 ± 0.09 a 287.50 ± 3.54 d 3.90 ± 0.66 abcd 4.10 ± 0.36 df 7.97 ± 0.40 de
FD75-25 3.70 ± 0.30 bcd 411.50 ± 2.12 g 3.90 ± 0.36 abcd 4.00 ± 0.00 df 7.77 ± 0.25 cde
FD70-30 4.08 ± 0.75 d 441.50 ± 0.71 i 3.67 ± 0.12 abc 3.77 ± 0.25 bcde 7.67 ± 0.12 cd
FD65-35 3.22 ± 0.24 ab 432.00 ± 0.00 h 3.60 ± 0.17 abc 3.70 ± 0.26 bcde 7.50 ± 0.00 bcd
FD60-40 3.24 ± 0.00 ab 241.50 ± 2.12 b 3.50 ± 0.00 ab 3.50 ± 0.00 abce 7.33 ± 0.29 abc
Oven drying (OD)
OD80-20 3.36 ± 0.16 ab 299.50 ± 0.71 e 3.50 ± 0.50 ab 4.33 ± 0.29 f 7.67 ± 0.29 cd
OD75-25 3.50 ± 0.46 abc 385.50 ± 0.71 f 3.37 ± 0.51 ab 4.17 ± 0.29 df 7.50 ± 0.50 bcd
OD70-30 3.32 ± 0.24 ab 474.50 ± 0.71 J 3.43 ± 0.60 ab 4.00 ± 0.50 df 7.43 ± 0.15 abc
OD65-35 4.00 ± 0.61 cd 533.00 ± 5.66 k 3.27 ± 0.64 a 3.87 ± 0.12 cdef 7.17 ± 0.29 ab
OD60-40 3.62 ± 0.15 abcd 271.00 ± 2.82 c 3.17 ± 0.29 a 4.00 ± 0.00 df 7.00 ± 0.00 a
Controls
SGs – – 10 10 5
Sucrose – – 5 0 10

Means within the same column followed by different letters (a,b,c) are significantly different (P < 0.05).

and 26.67 g H2O/100 g dry weight for SD60-40 and SD80-20 samples,
respectively, while not been significantly affected by the applied
drying method and the ratio of the agents used. However, it is
worth noting that the hygroscopicity of the SGs encapsulated prod-
ucts was reduced compared to the non-encapsulated SGs (Table 1).
Moreover, maltodextrin (MD) which was the major component in
the studied formulations proved to be the less hygroscopic agent,
leading thus to products with similar properties. This can further
result in enhancing the stability of the final products. Finally, con-
cerning the solubility of the products, it proved to be significantly
affected by the drying method (P < 0.05), with the spray dried
products presenting the highest solubility (average value of
96.87%). Comparatively, the solubility of the final products was
reinforced, ranging from 84.01–97.50 for OD60-40 and SD80-20 sam-
ples, respectively, while non-encapsulated SGs solubility value was
62.64%. Similar observation regarding the enhancement of solubil-
ity of steviol glycoside (Rebaudioside D) using spray drying was
also reported by Pang, Ma, Zhang, and He (2015).
3.3. Properties of the aqueous solutions (syrups) of the encapsulated
SGs products
The aqueous solutions (syrups) prepared with the encapsulated
SGs products in water, at 1% w/v, were evaluated in terms of appar-
ent viscosity and turbidity, properties which are of great interest in
food applications involving the replacement of sucrose solutions
with steviol glycosides ones (Table 2). It was observed that the
apparent viscosity did not differ statistically with respect to the
type of the applied drying method and the ratio of the agents used.
On the other hand, the turbidity of the solutions was significantly
influenced only by the type of the drying method; the spray dried
products in particular, afforded aqueous solutions of low turbidity
values (average value of 4.13 NTU) while those produced by freeze
and oven dried products gave aqueous solutions with high turbid-
ity values (mean values of 362.8 and 392.7 NTU, respectively).
overall acceptance) were significantly influenced by the applied
drying method (P < 0.05) and not by the ratio of the encapsulating
agents used. In particular, the spray dried products showed the
highest values of sweetness intensity and overall acceptance
(mean values of 4.26 and 8.50, respectively). Concerning the bitter
aftertaste, the lowest values were recorded for the spray dried
products (mean value of 3.37), followed by the freeze and oven
dried products (mean values of 3.81 and 4.07, respectively).
Among the studied formulations, the SD80-20 sample was perceived
as the most appealing sweetener product, since it presented the
highest overall acceptance (8.67) accompanied simultaneously by
the greatest sweetness intensity (4.33) without overcoming the
acceptable limit value of bitter aftertaste (5.0) (Table 2).
3.5. Study of SGs products using the FT-IR technique
The FT-IR technique allows the characterisation of changes in
the molecular structure of the encapsulated substances, also pro-
viding information about chemical bonds between the substances
and the agents used. Based on the obtained FT-IR spectra, the
applied drying methods led to a similar band profile for the studied
SGs encapsulated products. Therefore, the spectra of the represen-
tative SD80-20 (Fig. 2iv), FD80-20 (Fig. 2vii) and OD80-20 (Fig. 2v) are

3.4. Sensory evaluation of the aqueous solutions (syrups) of the

encapsulated SGs products

Based on the results of sensory evaluation (Table 2) of the

encapsulated steviol glycosides products, the sensory characteris- Fig. 2. FT-IR spectra of: MD (i), SGs (ii), IN (iii), SD80-20 (iv), OD80-20 (v), PM (vi), and
tics of the syrups (intensity of sweetness, bitter aftertaste and FD80-20 (vii) samples, respectively.
1156 C. Chranioti et al. / Food Chemistry 190 (2016) 1151–1158
(a)
(c)
Fig. 3. Structures of representative SD80-20 (a), FD80-20 (b), OD80-20 (c) samples (magnification 200).
presented. Particularly, the intense and wide band that was formed
at 3440 cm1 (3200–3550 cm1) corresponds to the stretching
vibration of the OH bond (AOH stretching) and is associated with
the presence of hydrogen bond (He, Rodriguez-Saona, & Giusti,
2007; Socrates, 2001), while the band at 2925 cm1 is characteris-
tic of the stretching vibration of the CH bond of the methyl groups
(CH sp3 stretching) (2850–3000 cm1) (Coates, 2000). The low
intensity band, which was recorded at 172,598 cm1, is assigned
to the stretching vibration of the AC@O bond (AC@O stretching)
and is due to the presence of steviol glycosides, whose is also the
characteristic band (Fig. 2ii). The band around 1645 cm1 is also
assigned to the stretching vibration of the AC@O bond (AC@O
stretching). Furthermore, the bands at 1424.17 cm1 and
1387.53 cm1 correspond to the bending vibration of the CH bond
(1470–1350 cm1). The FT-IR spectra of the representative samples
showed also principal bands at 1154, 1080 and 1024 cm1, which
are characteristic absorption bands of the glycosidic bond (De
Oliveira, Paula, & De Paula, 2014), derived mainly from maltodex-
trin (Fig. 2i) and steviol glycosides (Fig. 2ii). Finally, the bands at
929 cm1 and 856 cm1 are attributed to bending vibration of
the @CH (@CH bending) and @CH2 (@CH2 bending) bonds, respec-
tively (Krishnaiah, Sarbatly, & Nithyanandam, 2012).
Comparing the spectra of the representative encapsulated
SD80-20, FD80-20 and OD80-20 samples with the spectrum (Fig. 2vi)
of the sample occurring by physical mixing of the components
(physical mixture, PM) an identical profile was observed confirm-
ing that the steviol glycosides maintained their chemical integrity
after the application of the drying processes. Also, due to the non
appearance of new bands or shifts of the already existing ones in
the PM spectrum in the spectra of the representative encapsulated
samples, it is likely that no chemical reaction between SGs and
agents took place during the drying processes. Therefore, this could
support further evidence of the encapsulation of SGs in the agents
by intermolecular interaction.
(b)
3.6. Structure characterisation of the SGs encapsulated products
3.6.1. Morphology – SEM analysis
The morphology of the steviol glycosides encapsulated prod-
ucts was investigated using scanning electron microscopy
(Fig. 3). It is clear that the structure of the products varied sig-
nificantly depending on the applied drying method. Specifically,
the spherical type microcapsules (Fig. 3a) and the sponge-like
appearance (Fig. 3b) are characteristics of a spray and freeze
dried (Ma et al., 2014) product, respectively, while the structure
of the oven dried product is an indicative structure of such type
(Fig. 3c).
3.6.2. Crystallinity – XRD analysis
The degree of crystallinity of the steviol glycosides products
was also investigated using X-ray diffraction spectroscopy
(Fig. 4). X-ray diffraction was used in this study to demonstrate
the presence of amorphous material as opposed to a material
with a crystalline structure. It is well-known that the width of
X-ray diffraction peak is related to the size of crystallite – the
broadened peak usually results from an imperfect crystal
(Hosseini, Zandi, Rezae, & Farahmandghavi, 2013). The diagrams
obtained are characteristic to amorphous compounds (Rutz
et al., 2012). However, the type of drying method applied as
encapsulation technique appeared to differentiate the structure
of the final products. Specifically, with the use of freeze drying
technique a small tendency of crystallisation was observed
(Fig. 4b) which became more pronounced in the case of vacuum
drying oven application. This produced morphology (Fig. 4c)
may present particular technological interest in the production
of sweetener products based on steviol glycosides where crys-
talline sweetener products imitating sugar’s properties can be
produced.
 C. Chranioti et al. / Food Chemistry 190 (2016) 1151–1158
Fig. 4. XRD spectra of representative SD80-20 (a), FD80-20 (b), OD80-20 (c) samples.
4. Conclusions
Finally, based on the results, the application of spray drying
with maltodextrin and inulin as encapsulating agents, could be
proved efficient in reducing the bitter aftertaste of steviol glyco-
sides. MEE% ranged between 63.72% to 82.46% and the resulted
products presented different properties, with the spray dried SGs
products giving the best physicochemical characteristics and the
most appealing sensorial ones. Moreover, the reduced hygroscopic-
ity values (20.26–26.67 g H2O/100 g dry weight) achieved through
encapsulation by means of drying methods contributes to products
with improved stability. The structure of the SGs encapsulated
products was affected by the applied drying method with vacuum
oven produced structure showing a small degree of crystallinity.
Considering the overall evaluation of the obtained sweeteners
(SD, OD, FD), they can be used in specific purposes based on their
physicochemical, sensorial and textural characteristics (e.g. OD
products rather imitate sugar’s crystallinity whereas SD ones
favour in sensorial attributes). Even though all the formulations
studied in this research can be found potential food application,
further studies should be carried out in order to evaluate their
functionality in certain food products.
1157
Acknowledgment
Charikleia Chranioti is grateful to the State Scholarships
Foundation of Greece (IKY) for financial support.
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