Food Hydrocolloids 104 (2020) 105755

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Food Hydrocolloids
journal homepage: http://www.elsevier.com/locate/foodhyd

Whey protein films added with galactooligosaccharide

and xylooligosaccharide
Leonardo M. Fernandes a, Jonas T. Guimara ~es b, Ramon Silva a, b, Ramon S. Rocha a, b,
Natha�lia M. Coutinho , Celso F. Balthazar b, Rodrigo N. Calvalcanti c, Carlos W. Piler d,
b

Tatiana C. Pimentel e, Roberto P.C. Neto f, Maria In^es B. Tavares f, Erick A. Esmerino b,
Mo^nica Q. Freitas b, Marcia C. Silva a, Adriano G. Cruz a, *
a
Instituto Federal de Educaç~
ao, Ci^encia e Tecnologia do Rio de Janeiro (IFRJ), Departamento de Alimentos, 20270-021, Rio de Janeiro, Brazil
b
Universidade Federal Fluminense (UFF), Faculdade de Medicina Veterin� aria, 24230-340, Niter�
oi, Rio de Janeiro, Brazil
c
Universidade Estadual de Campinas (UNICAMP), Faculdade de Engenharia de Alimentos (FEA), 13083-862, Campinas, S~ ao Paulo, Brazil
d
Embrapa Agroindústria de Alimentos, Avenida das Am�ericas 29501, Guaratiba, 23020-470, Rio de Janeiro, Brazil
e
Instituto Federal do Paran�
a, Campus Paranavaí, 87703-536, Paranavaí, Brazil
f
Universidade Federal do Rio de Janeiro (UFRJ), Instituto de Macromol�eculas Professora Eloisa Mano (IMA), 21941-598, Rio de Janeiro, Brazil

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

Keywords: This study aimed to evaluate the effect of addition of xylooligosaccharide (XOS) and galactooligosaccharide
Xylooligosaccharide (GOS) to whey protein (WP) films produced by casting technique and using glycerol as a plasticizer. The films
Galactooligosaccharide were evaluated for thickness, scanning electron microscopy (SEM), differential scanning calorimetry (DSC),
Whey protein film
mechanical properties, water vapor permeability (WVP) and contact angle. No effect of the addition of prebiotic
Tensile strength
Scanning electron microscopy
components on thickness of the films was observed (0.13–0.14 mm, p > 0.05). XOS and GOS addition resulted in
Differential scanning calorimetry similar cross-sectional SEM images, presenting smaller and retracted laminated structures, with lower tensile
strength and higher elongation at break (3.8–1.7 MPa and 144–208%, respectively, p < 0.05); In addition, the
XOS and GOS addition reduced the WVP (1.09–0.63 g.mm.h 1.m 2.kPa 1, p < 0.05), despite the higher hy­
drophobicity evidenced by contact angle reduction (56.61–46.69� , p < 0.05). Finally, thermal analysis indicated
that the increased XOS and GOS concentration resulted in films with lower melting points (169.6–135.65 � C, p <
0.05). The possibility of using XOS and GOS to manufacture WP-films formulation provided interesting changes,
creating new forms to combine and add value to biopolymers, considering technological and functional aspects.

1. Introduction
Packaging is one of the most used methods to protect food from
adverse environmental conditions (Bersaneti, Mantovan, Magri, Mali, &
Celligoi, 2016). The development and use of renewable and environ­
mentally friendly materials of biological origin is one of the most studied
topics currently, which aim the reduction of environmental impact
caused by petroleum-based materials used in food packaging (Bakshi,
Selvakumar, Kadirvelu, & Kumar, 2019; Costa, Cerqueira, Ruiz, Foug­
nies, Richel, Vicente, 2015; Zhong, Godwin, Jin, & Xiao, 2019). Cheese
whey is a byproduct of cheese industry and the concentration and
isolation of its proteins can manufacture products and food ingredients
with high protein content (>90%), which can be used in the manufac­
ture of edible films. Whey protein-based films are characterized by their
transparency and lack of aroma and flavor, allowing a wide range of
applications (Dianin, Jrb, Pimentelc, Hernandesa, & Costaa, 2019).
However, they have some limitations regarding physical and mechanical
characteristics, requiring the use of materials with plasticizing proper­
ties to improve the resistance to moisture transfer and the flexibility of
the films (Castro, Domingues, Ohara, Okuro, dos Santos, Brexo, et al.,
2017). The plasticizer can act improving the mechanical properties of
edible films; however, some synthetic plasticizers may present some
toxicity problems, related to the migration of phthalates, which have
been avoided with the use of natural-based and biodegradable plasti­
cizers (Vieira, da Silva, dos Santos, & Beppu, 2011). Moreover, the
natural biopolymer edible films produced with the most common plas­
ticizers usually present low resistance (tensile strength) and high
moisture uptake, which may be improved using crosslinking techniques

* Corresponding author.
E-mail address: adriano.cruz@ifrj.edu.br (A.G. Cruz).

https://doi.org/10.1016/j.foodhyd.2020.105755
Received 29 September 2019; Received in revised form 4 February 2020; Accepted 9 February 2020
Available online 11 February 2020
0268-005X/© 2020 Elsevier Ltd. All rights reserved.
L.M. Fernandes et al.
to generate a stronger three-dimensional network and overcome the
inherent deficiencies in mechanical and barrier properties of bio­
polymers (Garavand, Rouhi, Razavi, Cacciotti, & Mohammadi, 2017).
In recent decades, there is growing interest in the development of
functional and active packaging (Bersaneti et al., 2016), mainly from
natural and biodegradable sources (Vahedikia, Garavand, Tajeddin,
Cacciotti, Jafari, Omidi, et al., 2019), which may be used as carrier
vehicles of antioxidants (Souza, Fernando, Pires, Rodrigues, Andreia &
Fernandes, 2017), antimicrobials (Hashemi and Khaneghah, 2017),
probiotics (Dianin et al., 2019) and prebiotic components (Bersaneti
et al., 2016). Prebiotics are food components selectively used by gut
microbiota, conferring health benefits (Gibson, Hutkins, Sanders, Pre­
scott, Reimer, Salminen, 2017). The incorporation of prebiotics in edible
packaging may increase the health claim of a food product, adding value
to it, also may help to increase the intake of those beneficial compounds
by population, which can be added directly to the food without affecting
the sensory characteristics of the products (Farias, Araújo, Neri-Numa, &
Pastore, 2019; Guimar~ aes, Balthazar, Silva, Rocha, Graça, Esmerino,
et al., 2020; Tang, Xie, Zhang, Zhu, Liu & Liu, 2015).
Xyloligosaccharides (XOS) are produced by the action of endox­
ylanases on the xylan, while galactooligosaccharides (GOS) are enzy­
matically produced in a kinetically controlled reaction of lactose
transgalactosylation catalyzed by different microbial strains (Vera,
Co�rdova, Aburto, Guerrero, Sua �rez & Illanes, 2016; Xu, Xia, Yuan, &
Sun, 2019). Both compounds can be used as a food ingredient to improve
bowel function, increase calcium absorption, and reduce the risk of
tooth decay. Given the excellent biological properties, the incorporation
of XOS and/or GOS into edible packaging films can be an effective
method for improving functional activity of films (Xu et al., 2019).
Previous studies have evaluated the incorporation of prebiotics into
films, including fructooligosaccharides (FOS, Bersaneti et al., 2016),
XOS (Xu et al., 2019), inulin (Tang et al., 2015), polydextrose (Soukoulis
et al., 2014), and arabioxyloligosaccharide (Costa et al., 2015). How­
ever, to the best of our knowledge, there is no study associating GOS and
XOS to whey protein-based films. Therefore, this study aimed to eval­
uate the effect of the inclusion of XOS and GOS on the physical-chemical
and mechanical properties of whey protein based edible films.
2. Materials and methods
2.1. Materials
Commercial whey protein isolate (Clean Whey, Glanbia Nutritional
Sanavita, Piracicaba, Brazil), XOS (powder, AIDP Incorporation, Cali­
fornia, USA), composed of 26% xylobiose (n ¼ 2), 21% xylolriose (n ¼
3), 12% xylotetraose (n ¼ 4), 16% other polymerized components and
5% mixed sugars (glucose, xylose, arabinose), GOS (Vicinal® GOS
Syrup, Friesland Campina Domo®, Borculo, Holland), composed of 38%
of disaccharides (n ¼ 1) and 59% of galactooligosaccharides (n ¼ 2 and
n ¼ 3), 3% others polymerized components (n > 3), analytical grade
glycerol (Vetec, Quimica Fina, Rio de Janeiro), sodium chloride (Vetec,
Quimica Fina, Rio de Janeiro), analytical grade sodium hydroxide
(Dinamica, Diadema, SP) and polystyrene Petri plates, 8.4 cm diameter,
were used in the experiments.
2.2. Preparations of edible films
The concentrations and combinations of the components used in this
study were established according to Hassannia-kolaee, Khodaiyan,
Pourahmad & Shahabi-ghahfarrokhi, (2016) with modifications ac­
cording to preliminary tests, to obtain the best properties of the films
and to ensure the film-forming ability and characterization. To obtain
the plasticizing effect, the glycerol concentration was established at
30g/100g for all films. Four prebiotic concentrations were incorporated
into the WP-based films, as follows: 0, 10, 20, and 30g/100g, and the
films were named according to their nature (W– – WP, X ¼ XOS, and G ¼
2
Food Hydrocolloids 104 (2020) 105755
GOS), as follows: W100, W90X10, W80X20, and W70X30 corresponding
to the samples containing XOS, and W100, W90G10, W80G20, and
W70G30 corresponding to the samples containing GOS.
A preliminary test was carried to verify the film-forming capacity of
the formulation. It was observed that using pH lower than 7.0 in ho­
mogenization step was not possible to make stable films due to changes
in denaturation and interactions between proteins, which is influenced
by pH, temperature and concentration. Then, the pH was increased (7.5)
to improve the properties of the films, since it prevent the protein pre­
cipitation due to denaturation, favoring the homogenization of the fil­
mogenic solution (Schmid & Müller, 2019, pp. 407–437). The
processing temperature of the film-forming solutions (FFS) was 90 � C,
because the denaturation of whey proteins in pH near neutral occur
efficiently from temperatures of 64 and 85 � C for beta-lactoglobulin and
alfa-lactoalbumin, similar methods were used by other authors
(Gagliarini, Diosma, Garrote, Abraham, & Piermaria, 2019; Ozdemir &
Floros, 2008).
The film-forming solutions (FFS) were prepared by diluting the solids
in distilled water until a total solid concentration of 10%. The FFS was
homogenized using a magnetic stirrer at room temperature for 10 min,
and the pH was adjusted to 7.5 using sodium hydroxide. After, the so­
lutions were heated to 90 � C for 20 min under constant stirring on a
Brabender viscoamilograph (Duisburg, Germany). The heated FFS was
cooled to 70 � C, and 10 mL aliquots were poured into Petri plates (8.4
cm internal diameter) and incubated at 27 � C in a forced convection
incubator (ELKA, Germany) for 24 h. After drying, the films were
removed manually from the plates and stored for 48 h in hermetic
chambers, under vacuum and 75% relative humidity before analysis.
2.3. Film thickness
The film thickness was measured using a Fowler IP 54 digital
micrometer (Fowler, Newton, USA), with a sensitivity of �0.001 mm, at
ten random points in different parts of the film. The final thickness was
considered as the arithmetic mean of 10 measurements.
2.4. Scanning electron microscopy (SEM)
The microstructure analysis of the films was performed using a TM
3000 scanning electron microscope SEM (Hitachi, Tokyo, Japan), being
the samples previously dried in a circulating oven at 60 � C for 24 h.
Following this, they were cut with the aid of a metallic blade, in a
rectangular form of about 3–4 mm, placed in appropriate support using
double sided adhesive tape and coated with a thin layer of gold for 15
min in vacuum (Piccirilli, Soazo, P�
erez, Delorenzi, & Verdini, 2019). The
superficial images (magnification of 3000x) were obtained using the
whole film and cross-sectional images (magnification of 400x) were
obtained after transversal cut using scalpel blades.
2.5. Thermal analysis
The analysis was performed by differential scanning calorimetry (DSC)
using Q200 equipment (TA Instruments, New Castle, USA). For that,
0.03 mg of sample was placed in hermetically sealed aluminum pan,
heated at 10 � C/min in the range of 5–180 � C, cooled using Nitrogen
50.0 ml/min, to 20 � C, and reheated to 180 � C. All analyses were carried
out in triplicate.
2.6. Mechanical properties
The mechanical properties tensile strength at break (MPa) and
elongation at break (%) were determined based on the standard guide­
lines of the American Society for Testing and Materials D 882-83 (ASTM,
1995) with some modifications to adapt to the characteristics of our
samples, using a TA XT Plus texture analyzer (Stable Microsystems,
Surrey, England). For the tests, the films were cut in specimens of 50 mm
L.M. Fernandes et al. Food Hydrocolloids 104 (2020) 105755

long and 20 mm wide and stored for 48 h at 25 � C and 75% RH. The tests Table 1
were performed with a clamp speed of 1 mm/s and initial clamp distance Thickness and peak temperature of the WP-based films.
of 10 mm. Five repetitions were performed for each treatment. Treatments Thickness (mm) Peak temperature (oC)
a
W100 0.13 � 0.01 169.6 � 0.92 a
2.7. Water vapor permeability W90G10 0.13 � 0.02 a 160.79 � 1.07 b
W80G20 0.13 � 0.01 a 153.75 � 0.78 c
The water vapor permeability was determined gravimetrically, ac­ W70G30 0.13 � 0.02 a 135.65 � 0.99 d
cording to the method E96-80 proposed by the American Society for W90X10 0.14 � 0.00 a 160.76 � 1.73 b
W80X20 0.14 � 0.00 a 150.37 � 0.65 c
Testing and Materials (ASTM, 2001) at 25 � C. The edible films were cut W70X30 0.13 � 0.00 a 136.19 � 0.84 d
into circular format (40 mm in diameter), placed inside the permeation
cells filled with distilled water, and stored in desiccators containing blue *The values are expressed as mean � standard deviation. Different letters at the
same column indicate statistical difference according the Tukey test (p < 0.05).
silica. The weight of cells and films was monitored at 24-h intervals for 5
n ¼ 10 for thickness and n ¼ 3 for peak temperature. W100 ¼ 100% whey
days, aimed to determine the weight changes throughout the period.
protein, no prebiotics added. W90X10, W80X20, and W70X30 ¼ the first and
Water vapor permeability was determined according to Equation (1). second number are linked to the amount of whey protein and xylooligo­
� g � x saccharide added at the film formulation; W90G10, W80G20, and W70G30 ¼
WVP ¼ � (1)
t � A ΔP the first and second number are linked to the amount of whey protein and gal­
actooligosaccharide added to the edible film formulation.
where WVP is water vapor permeability (g.mm.h 1.m 2.kPa 1); g is the
weight gain (g); t is the total time, in hours; A is the permeation area; x is prebiotic components on the surface microstructure of the films, which
the mean film thickness (mm); and ΔP is the vapor pressure difference presented smooth and homogeneous structures, with no granules, par­
between the surface of desiccant (silica gel; kPa at 25 � C) and pure water ticles, and bubbles. In the cross-section images, there was no indication
(3.167 kPa at 25 � C). of separation of phases, suggesting a good intermolecular interaction
between whey proteins and the prebiotics XOS and GOS. After the cut
2.8. Contact angle using scalpel blade, the cross-sectional surfaces of the films presented
laminated structures with a peeling behavior, and these laminated
The contact angle of the liquid drop was measured at room tem­ structures were larger in the samples without the prebiotics, indicating a
perature, as described by Silva, Pereira, Carvalho, and Ferrua (2007), higher force of interaction and a more rigid structure, using only whey
using a CAM 101 contact angle meter (KSV, City, Finland), according to protein. The addition of both oligosaccharides resulted in similar cross-
the sessile drop method at the time of 20 s, using the image processing sectional images, which presented smaller and retracted laminated
software. For that, the film samples (50 � 20 mm) were fixed to a glass structures, probably due to the lower interactions between the oligo­
slide by double-sided adhesive tape, placed on the base of the apparatus, saccharides and whey protein chains and an increased flexibility or
and the measurements of the right and left angle of three drops were ductility provided by the carbohydrates (Almond, 2005; Xu et al., 2019).
performed. A 0.1 mL drop of water was placed onto the sample surface Moreover, the images of the films added of 20% and 30% of XOS pre­
with the aid of a syringe, and the droplet image was captured by a digital sented the smallest and most retracted laminated structures, which may
camera for 60 s at 1s intervals. be related to the highest values obtained for elongation at break of these
samples, indicating the more ductility provided by the XOS addition.
2.9. Statistical analysis

The processing was repeated three times, being the analysis per­
formed at least in triplicate. The results were presented as mean �
standard deviation and statistical analysis was carried using analysis of
variance (ANOVA) and Fisher’s test (p � 0.05), using XLSTAT 2019.1
software (Adinsoft, Paris, France).

3. Results and discussion

3.1. Thickness

The results of the film thickness are presented in Table 1. There was
no effect of the prebiotic ingredient (GOS or XOS) on the film thickness
(p > 0.05). The films were between 0.13 and 0.14 mm thick, corrobo­
rating previous studies with whey protein-based films (Gagliarini et al.,
2019; Soazo, P� erez, Piccirilli, Delorenzi, & Verdini, 2016). The low
variability is of great importance to investigate the effect of the pre­
biotics on the film properties, since film thickness can greatly affect the
responses. The maintenance of film thickness after the addition of pre­
biotic components to the formulations indicates good solubility of the
components in the WP based film-forming solution, with no formation of
insoluble particles, evidencing a good interaction between the prebiotics
and the three-dimensional structure of whey proteins (Bersaneti et al.,
Fig. 1. Scanning electron microscopy (SEM, Superficial images) at magnifica­
2016).
tion of 3000x. W100 ¼ 100% whey protein, no prebiotics added. W90X10,
W80X20, and W70X30 ¼ the first and second number are linked to the amount
3.2. Scanning electron microscopy (SEM) of whey protein and xylooligosaccharide added at the film formulation;
W90G10, W80G20, and W70G30 ¼ the first and second number are linked to
SEM micrographs were obtained for film surfaces (Fig. 1) and cross- the amount of whey protein and galactooligosaccharide added at the edible film
sectional surfaces (Fig. 2). There was no significant effect of the formulation.

3
L.M. Fernandes et al. Food Hydrocolloids 104 (2020) 105755

Table 2
Mechanical properties, Water Vapor permeability and contact angle values of
the WP- based films.
Treatments Tensile Elongation at Water Vapor Contact
strength at break (%) Permeability (g. angle
break (Mpa) mm.h 1.m 2. (degrees)
kPa 1)

W100 3.80 � 0.08 144.03 � 1.09 � 0.18 a 56.61 �

a
2.72 d 0.39 a
b
W90G10 3.17 � 0.08 149.41 � 0.78 � 0.10 49.55 �
b
4.79 cd 4.04 b
W80G20 2.70 � 0.13 161.64 � 0.76 � 0.03 b 50.93 �
c
6.83 c 3.49 b
W70G30 1.73 � 0.31 189.55 � 0.69 � 0.03 b 51.66 �
d
6.59 b 5.04 b
W90X10 3.64 � 0.15 151.99 � 0.74 � 0.05 b 46.75 �
a
2.33 cd 1.49 b
W80X20 2.65 � 0.13 181.51 � 0.71 � 0.08 b 46.97 �
c
3.65 b 1.18 b
W70X30 1.89 � 0.06 208.22 � 0.63 � 0.06 b 46.69 �
d
4.71 a 1.82 b

The values are expressed as mean � standard deviation. Analysis were per­
formed at least in triplicate. Different letters at the same column indicate sta­
tistical difference according the Tukey test (p < 0.05). W100 ¼ 100% whey
protein, no prebiotics added. W90X10, W80X20, and W70X30 ¼ the first and
second number are linked to the amount of whey protein and xylooligo­
saccharide added at the film formulation; W90G10, W80G20, and W70G30 ¼
the first and second number are linked to the amount of whey protein and gal­
actooligosaccharide added at the edible film formulation.

made with 10g/100g XOS (p > 0.05).

Fig. 2. Scanning electron microscopy (SEM, cross section images) at magnifi­
cation of 400x. W100 ¼ 100% whey protein, no prebiotics added. W90X10,
W80X20, and W70X30 ¼ the first and second number are linked to the amount
of whey protein and xylooligosaccharide added at the film formulation;
W90G10, W80G20, and W70G30 ¼ the first and second number are linked to
the amount of whey protein and galactooligosaccharide added at the edible film
formulation.
3.3. Thermal analysis
The results of the DSC analysis are shown in Table 1. The thermal
properties of films are important variables for the application in in­
dustry, since packaging materials often undergo heating processes dur­
ing the manufacture, storage and consumption of the products (Wang,
Liu, Ye, Wang, & Li, 2015).
The use of higher concentrations of prebiotic and lower of WPI
resulted in a decrease in endothermic peak temperatures (Tp, p < 0.05),
probably because the addition of XOS and GOS weakened the in­
teractions between whey protein chains (e.g. hydrogen bonds and
electrostatic interactions), reducing the resistance to mobility of the
polymer chains, thus, resulting in lower Tp values (Xu et al., 2019). The
addition of prebiotic ingredients formed less dense structures (Fig. 2)
due to the branched characteristic of the oligosaccharides (Almond,
2005), producing more ductile films, which require less energy to break
the interchain and oriented-peptide bonds, resulting in a lower peak
temperature (Wang et al., 2015).
3.4. Mechanical properties
The decrease in tensile strength and increase in elongation in films
added of XOS and GOS, may be related to the lower formation of strong
protein-protein interactions (e.g. hydrogen bonds and electrostatic in­
teractions) between whey protein chains (Xu et al., 2019). The addition
of oligosaccharides (high volumes to their molecular weight, sugar and
hydroxyl molecules) to the whey protein films, induce complex in­
teractions between carbohydrates, proteins and water, forming large
and branched structures, which gives to these structures more flexibility
(Almond, 2005). Wihodo and Moraru, (2013) have reported that more
heterogeneous films are associated to more flexible materials, while
films with smooth microstructures are related to more resistant and
brittle materials. The addition of prebiotic oligosaccharides resulted in
more heterogeneous films (smaller and more laminated structures)
(Fig. 2). Despite the low molecular weight of the oligosaccharides, their
branched structure compared to the globular structure of the whey
proteins may have developed an intermolecular spacing effect, similar to
that observed when plasticizers are used (Tang et al., 2015). Therefore,
there was a reduction in tensile strength and an increase in elongation of
the films, since the prebiotic oligosaccharides decreased the structure
density, increasing the mobility of the polymeric chains, thus forming
less resistant but more ductile films (Castro et al., 2017). Films with
lower concentrations of prebiotic components may be used in foods
requiring greater mechanical resistance, while films with higher prebi­
otic concentrations can be used for other purposes (Xu et al., 2019).
However, the tensile strength of films used food packaging, as PVC
(Polyvinyl chloride) films, are usually greater than 20 MPa, in order to
be used without rupturing (Coltro, Pitta, & Madaleno, 2013), then, the
low TS presented by the studied samples indicates a difficulty of using it
as an external packaging material, but it may have other interesting
applications like the use for separation of cheese slices (Cruz-Diaz,
Cobos, Ferna �ndez-Valle, Díaz, & Cambero, 2019).

The results of the mechanical properties of the films are shown in

Table 2. In general, the addition of prebiotic components at concentra­
tions greater than 20 g/100g to the films led to a significant decrease in
tensile strength and an increase in elongation at break (p < 0.05). No
significant changes were observed for elongation of the films made with
10g/100g GOS, and for both elongation and tensile strength of the films
3.5. Water vapor permeability
Whey protein-based films usually present relatively low oxygen
permeability, due to the formation of strong intermolecular covalent
bonds (e.g disulphide bonds) between denatured whey proteins, which

4
L.M. Fernandes et al.
result in the creation of a three-dimensional network increasing the
structural cohesion (Schmid, Reichert, Hammann, & Sta €bler, 2015).
However, these films also present poor humidity barriers due to the
general intrinsic protein hydrophilicity, which limit their application
(Schmid & Müller, 2019, pp. 407–437).
The water vapor permeability of the studied films ranged from 0.63
� 0.06 to 1.019 � 0.18 (g.mm.h 1.m 2.kPa 1) (Table 2). The addition
of XOS and GOS associated to the lower WPI content decreased the WVP,
regardless of the type and concentration of the prebiotics (p < 0.05). The
increase in the tortuous path for water vapor molecules to pass through
the prebiotic film (Fig. 2) may have resulted in slower diffusion and
lower permeability (Xu et al., 2019). In addition, the molecular char­
acteristic of the oligosaccharides (Wang, Zheng, Wang, Tang, Liu & Li,
2020) may have also induced the interaction with water, forming strong
interactions between water and hydroxyl groups (Nakamura, Hata­
keyama, & Hatakeyama, 1983), which may decrease free water in the
system, resulting in less water diffusivity throughout the film matrix,
and decreasing WVP (Bersaneti et al., 2016). Water vapor transfer in
films is also strongly related to the particle size distribution, thus the
smaller particle size of the prebiotic components and the creation of a
differentiated structure can be related to the lower WVP of the prebiotic
films (Galus and Kadzin � ska, 2016). In this context, the incorporation of
oligosaccharide components changed the properties of the WPI films,
which are moisture sensitive. The WVP is usually reduced by addition of
hydrophobic compounds, like lipids and waxes, however, in this study,
the addition of XOS and GOS could also decrease the film permeability
to water vapor. Finally, the prebiotic edible films may serve as semi­
permeable barriers against moisture in foods, including fresh fruits and
vegetables or bakery products (Ferna �ndez, de Apodaca, Cebria �n,
Villar�
an, & Mat� e, 2007), in which is not desirable the water vapor
condensation due to the microbial spoilage risk.
3.6. Contact angle
The measurement of the water contact angle (CA) is an effective tool
to determine the hydrophobic and hydrophilic characteristics of the
films. Contact angle values higher than 90� characterize hydrophobic
surfaces, while CA values lower than 90� characterize the hydrophilic
surfaces (Xu et al., 2019).
The films of the present study presented contact angles (CA) with
water ranging from 46.69 to 56.61� . The samples with prebiotics addi­
tion, regardless of the type and concentration of prebiotics, presented
lower contact angles in comparison to the film without prebiotic (p <
0.05) (Table 2). The decreased contact angles indicate that the prebiotic
addition increased the hydrophilicity or decreased the hydrophobicity
of the film, which confirm the results observed for WVP, since a film
with higher hydrophilicity interact more with water, resulting in less
water diffusivity throughout the film. These effects may be related to the
hydrophilic and hygroscopic characteristics of some prebiotics, like ol­
igosaccharides, including XOS and GOS (Soukoulis et al., 2014; Wang
et al., 2020), therefore, lower CA of prebiotic films may be proportio­
nated by the hydrophilic nature of the prebiotic components (Hashemi
and Khaneghah, 2017).
The characteristics of a packaging film depends on the type of food
you want to protect and the desired functionalities, then, despite the
changes caused by XOS and GOS to the edible WPI- based film, like low
tensile strength, making it difficult to use as an external packaging
material, it may have other interesting applications. Further studies may
be necessary to achieve the improvement of the mechanical properties,
like the utilization of crosslinking techniques. At first view, our findings
are not too much relevant if compared to the conventional synthetic and
petroleum-based plastics, but the possibility of using XOS and GOS to
produce edible films create new forms to combine and add value to
biopolymers, contributing to the technological development and func­
tional characteristics of edible WP-based films.
5
Food Hydrocolloids 104 (2020) 105755
4. Conclusion
This study demonstrated that the addition of prebiotic components
(GOS or XOS) to WP films induced significant changes in their me­
chanical properties, reducing the tensile strength at break (3.8–1.7
MPa), increasing the elongation at break (144–208%) and thickness
values (0.13–0.14 nm) and reducing the water droplet contact angle
(56.61–46.69� ). Despite the increased hydrophilic characteristic of the
WP-film, the permeability to water vapor was reduced (1.09–0.63 g.mm.
h 1.m 2.kPa 1), which is desired in most of the film applications. In
addition, the thermal analysis indicated that increasing the concentra­
tion of oligosaccharides resulted in lower melting points (169.6–135.65
�
C), decreasing its resistance to heat.
Overall, interesting changes were noted by addition of XOS and GOS
at the WP-film formulation, to combine and add value to biopolymers,
considering technological and functional aspects.
Author contribution
All the authors contribute in a similar way in all the steps of the
manuscript.
Declaration of competing interest
None.
Acknowledgement
The authors are grateful to the Rio de Janeiro State Research Support
Foundation (FAPERJ), National Council for Scientific and Technological
Development (CNPQ) and Higher Education Personnel Improvement
Coordination (CAPES) and Federal Institute of Science and Technology
of Rio de Janeiro (IFRJ) for the financial support.
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