Food Packaging and Shelf Life 26 (2020) 100577

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Food Packaging and Shelf Life

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Development of polyethylene films coated with gelatin and mango peel

extract and the effect on the quality of margarine
A. Nor Adilah a, M.A. Noranizan a, B. Jamilah a, Z.A. Nur Hanani a, b, *
a
Department of Food Technology, Faculty of Food Science and Technology, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor, Malaysia
b
Halal Products Research Institute, Universiti Putra Malaysia, 43400, UPM Serdang, Selangor, Malaysia

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

Keywords: Polyethylene (PE) films coated with an active layer of gelatin and mango peel extract (MPE) were developed for
Active packaging margarine product. MPE as an antioxidant source was incorporated into a fish gelatin-based film-forming so­
Bilayer film lution (FFS). The FFS was coated onto PE films with different thicknesses (10, 20, 40, and 60 μm) to form
Shelf life
polyethylene/gelatin bilayer films (PE/G). The physical and antioxidant properties of the PE/G films were
Mango peel
Antioxidant
determined. Thicker coatings produced coloured films, which improved light barrier properties and increased
DPPH radical scavenging values. Scanning electron microscopy (SEM) analysis showed the bilayer films were
compatible with one another and produced compacted film integrity. Also, the PE/G60 film improved the
oxidation stability of margarine up to 28 days of storage period at 4 ◦ C. The results suggest that bilayer films have
potentials to be used as active packaging materials for delaying lipid oxidation.

1. Introduction gelatin-based films (Nor Adilah et al., 2018). Therefore, active bilayer
films fabricated by coating an active biopolymer onto a synthetic
An approach that combines synthetic materials with other bio­ polymer film may be advantageous to enhance the functionality of
polymers has been increasingly adopted to gain an extra function from synthetic packaging materials.
conventional packaging in the form of active packaging (antioxidants, Oxidation is a major cause for food nutritional and quality deterio­
antimicrobials, etc.). Furthermore, the incorporation of active com­ ration. Factors such as temperature, moisture, and light could accelerate
pounds during the production of synthetic polymers may degrade the the lipid oxidation process in food products (Carrizo et al., 2016). Lipid
functionality of active compounds due to the high temperature used oxidation could lead to the formation of hydroperoxides, a primary
during processing. Biopolymers can be carriers of bioactive compounds oxidation product which are the precursors to the secondary oxidation
for active packaging films (Rahmani et al., 2017). Among biopolymers, products. The secondary oxidation products will impart undesirable
gelatin is a good example of a protein-based polymer that has been odour and flavour which is known as rancidity (Carrizo et al., 2016).
extensively used owing to its excellent film-forming and gas barrier Generally, food products with a high composition of fats and oils are
properties (Nur Hanani et al., 2014). more susceptible to lipid oxidation. Margarine is a type of fluid emulsion
Mango peel is a by-product of fruit processing and contributes of edible fat or oil which contains no less than 80 % oils and due to the
approximately 15–20 % from the whole fruit weight (Rudra et al., high composition of the lipid/fat, the product is prone to lipid oxidation.
2015). Mango peels are also rich in valuable components such as The traditional way to inhibit the lipid oxidation is to incorporate
phenolic compounds, fibres and minerals (Jahurul et al., 2015). Bioac­ antioxidants during the margarine-making process. Synthetic antioxi­
tive compounds that have been identified in mango peels include xan­ dants are usually used in the production of commercial margarine but
thones, flavonoids, benzophenones, gallates, gallotannins, gallic acid due to health concerns, researchers are shifting their focus on the use of
and its derivatives (Dorta et al., 2014), which contribute to the antiox­ natural antioxidants to retard lipid oxidation process (Chen et al., 2014;
idant ability of the mango peels. Our previous study revealed that mango Inanc & Maskan, 2012). However, incorporating natural extracts into
peel has the potential as an antioxidant component in the production of margarine formulation may impart undesired flavour and sensory

* Corresponding author at: Department of Food Technology, Faculty of Food Science and Technology, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor,
Malaysia.
E-mail address: [email protected] (Z.A. Nur Hanani).

https://doi.org/10.1016/j.fpsl.2020.100577
Received 24 April 2020; Received in revised form 20 August 2020; Accepted 30 September 2020
Available online 18 October 2020
2214-2894/© 2020 Elsevier Ltd. All rights reserved.
A. Nor Adilah et al. Food Packaging and Shelf Life 26 (2020) 100577

qualities, thus affecting consumer preferences towards the product. ± 2 ◦ C with 50 ± 5% relative humidity (RH) for 2 days before further
Therefore, incorporating active compounds into the food packaging analysis.
materials could be a promising alternative to maximize the potential of
their antioxidant ability (Licciardello et al., 2015; Marcos et al., 2014).
2.5. Preparation of margarine and its packaging for storage
Previous studies revealed that the overall acceptability of the food
products packed with natural extracts active packaging had satisfactory
Margarine was prepared according to the method as described by
acceptance although some sensory qualities were affected by the pro­
Pande et al. (2013) with slight modifications. The margarine produced
long shelf life conditions (Han Lyn et al., 2019; Pateiro et al., 2019;
was free from preservatives, adulteration and colourant to reduce the
Mehdizadeh & Langroodi, 2019; Siripatrawan & Noipha, 2012).
limitations that might influence the antioxidant efficiency of the bilayer
Film thickness is one of the crucial parameters in the production of
films. The lipid phase (82 %) was prepared by blending the oils (81.5 %)
packaging material, as it defines specific functional parameters such as
and liquid soy lecithin (0.5 %) together. Aqueous phase (18 %) consisted
permeability to UV light (Ha et al., 2016) and oxygen (Maalihan &
of water (16 %) and salt (2%) were prepared. Then, the lipid phase and
Pajarito, 2016), resistance to insects (Stejskal et al., 2017), permeation
the aqueous phase were mixed and heated at 60 ◦ C for 3 min with
and diffusivity (Delgado et al., 2018) or migration rate of migrants
continuous stirring. After that, the mixtures were vigorously emulsified
(Wagner et al., 2018). Therefore, this study aimed to evaluate the effect
by using a tabletop blender (Tefal blendforce maxi, Tefal, UK) for 5 min.
of active layer thickness (gelatin with mango peel extract) on the
The mixtures were crystallized in an ice bath and then refrigerated
physical and antioxidant properties of PE bilayer films. The effect of
overnight. Next, the margarine was tempered for 4 h and smoothens by
bilayer films on the quality of margarine was also determined.
using a hand mixer. Finally, about 15 g of margarine was packed in
packets (10 × 10 cm) of polyethylene (PE) and polyethylene/gelatin
2. Materials and method
bilayer films (PE/G). The packed samples were stored at 4 ± 3 ◦ C and 25
± 3 ◦ C for 28 days.
2.1. Materials

Polyethylene (PE) plastic (thickness: 98 μm; size: 90 × 120 cm2) was 2.6. Analyses of film
purchased from a local store, and Chokanan mango peels were collected
from a fruit stall in Serdang, Selangor, Malaysia. Fish gelatin from 2.6.1. Film thickness
Tilapia fish skin (~ 240 bloom) was purchased from Custom Collagen The thickness of the films was measured by obtaining average values
(Addison, IL, USA). Absolute ethanol (99.8 %) and 2,2-diphenyl-1-pic­ from five different random positions on the films by using a hand-held
rylhydrazyl (DPPH) were obtained from Sigma Chemical Co. (St. digital micrometer (Mitutoyo, Tester Sangyo Co. Ltd., Tokyo, Japan).
Louis, MO, USA), whereas Folin-Ciocalteu reagent, gallic acid, glycerol
(99.5 % purity) and sodium carbonate were purchased from Merck 2.6.2. Colour measurement
(Darmstadt, Germany). All reagents used were of analytical grade. The colour of the film samples was measured using a Hunter Lab
Ultrascan PRO spectrocolourimeter (Model A60− 1012-402, VA, USA).
2.2. Preparation of mango peels A white tile was used for instrument calibration before the measurement
was taken at 5 random positions on the films. The values that indicate
Chokanan mango peels were collected from stall markets in Serdang, the films lightness (L-value), greenness/redness (a-value), and blueness/
Selangor, Malaysia. The peels were cleaned with tap water before yellowness (b-value) were recorded.
removing excess dirt and undesired parts on the peels. Then, the peels
were rinsed with distilled water and dried for 24 h in a 35 ◦ C oven 2.6.3. Transparency
(Memmert model UF110, Germany). Dried peels were ground into The transparency of the films was measured at the wavelength of 280
powder by using an electrical blender (Panasonic model MX-J210PN, nm (UV) and 660 nm (visible) by using a UV–vis spectrophotometer
Japan). (Shimadzu UV–vis 1601, Japan) as described by Wang and Rhim (2015).
The amount of UV-light and visible light that was able to pass through
2.3. Extraction of mango peels the bilayer films was expressed as the percentage of transmittance (%).

The mango peel powder was macerated in absolute ethanol (1:10 w/ 2.6.4. Water vapour permeability
v) as in a previous study by Sultana et al. (2012). The filtrate was The water vapour permeability (WVP) was measured according to a
concentrated using a vacuum rotary evaporator at 45 ◦ C. Then, the modified ASTM E-96 standard method (ASTM 1990) by Nur Hanani
mango peel extract (MPE) was kept at − 18 ◦ C and away from light et al. (2012). Approximately 6 mL of distilled water was filled into the
exposure until used. test cup before the film sample was tightly fixed over the opening with a
rubber gasket. After that, the cups were placed under controlled RH and
2.4. Preparation of bilayer films temperature at 50 ± 5% and 23 ± 2 ◦ C, respectively. Then, the weight of
the test cups was recorded every hour for duration of 9 h. The WVP was
The film-forming solution (FFS) was prepared by dissolving 4% fish calculated using Eq. (1) below:
gelatin (w/v) in distilled water for 30 min at 45 ◦ C as described by
WVP = (Δm/Δt) ⋅L/(A Δpw) (1)
Hosseini et al. (2015) with slight modifications. Glycerol (30 % w/w
based on gelatin), which acts as a plasticizer, was added to the solution. where (Δm/Δt) is the slope of a linear regression of weight loss of cup
Then, the dispersion was stirred by using a magnetic stirrer and versus time (g/s), L is the film thickness (mm), A is the film area (m2)
continuously heated for another 15 min at a constant temperature. Then, and Δpw is the difference in water vapor pressure (kPa).
5% MPE based on w/w of gelatin was added to the solution and stirred
for another 60 min. Last, the FFS was cast onto PE films, and different 2.6.5. Determination of total phenolic content (TPC)
application volumes were adjusted by the film applicator to obtain The extraction of active bilayer films was performed by soaking 25
gelatin thicknesses of 10 μm (PE/G10), 20 μm (PE/G20), 40 μm mg of film in 3 mL of ethanol. The total phenolic content (TPC) of films
(PE/G40), and 60 μm (PE/G60). The polyethylene/gelatin bilayer films was determined by mixing 0.3 mL of film extract with 2.5 mL of 10 %
(PE/G) were dried at 25 ± 2 ◦ C overnight. PE without a gelatin layer was Folin-Ciocalteu reagent and 2 mL of 7.5 % sodium carbonate solution
prepared as a control. The films were conditioned at a temperature of 25 according to Ruiz-Navajas et al. (2013). The mixture was incubated at

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A. Nor Adilah et al. Food Packaging and Shelf Life 26 (2020) 100577

Table 1
The physical and antioxidant properties of polyethylene (PE) and polyethylene/gelatin bilayer films (PE/G).
Films Total thickness (μm) Expected thickness (μm) WVP TPC DPPH
10
(×10− g.mm/m2.s.kPa) (GAE mg/g film) (%)

PE 98.00 ± 0.02e – 2.3 ± 0.4a – –

PE/G10 107.40 ± 0.04d 108.00 3.8 ± 0.1b 8.6 ± 0.5a 68 ± 1d
PE/G20 120.20 ± 0.04c 118.00 4.4 ± 0.1b 5.4 ± 0.3b 74 ± 1c
PE/G40 131.20 ± 0.01b 138.00 5.0 ± 0.2c 4.7 ± 0.1b 77 ± 1b
PE/G60 155.80 ± 0.02a 158.00 7.2 ± 0.5d 2.8 ± 0.0c 81 ± 1a

Values are given as mean ± standard deviation (n = 3). Means in the same column with different superscript letters are significantly different (p ≤ 0.05). Lowercase
letters indicate comparison between different types of films. PE/G10, PE/G20, PE/G40, and PE/G 60 represents the bilayer films with 10, 20, 40, and 60 μm gelatin
thicknesses, respectively.

50 ◦ C for 5 min before being measured using a spectrophotometer 2.7. Oxidative stability of product
(Shimadzu UV–vis 1601, Japan) at 760 nm. The TPC for the control film
(PE) was not evaluated, as there was no antioxidant added in the PE film. 2.7.1. Peroxide value
The primary products of oxidation was evaluated according to the
2.6.6. DPPH radical scavenging activity (DPPH) method described by Santos et al. (2014). About 5 g of margarine was
The antioxidant activity of films was evaluated by using the method weighed and mixed with acetic acid-chloroform solution (3:2 v/v).
of mixing 3 mL of film extract with 1 mL of a 0.1 mM ethanolic solution Then, 1 mL of potassium iodide solution and 1 mL of 1% starch solution
of 2,2-diphenyl-1-picrylhydrazyl (DPPH) and allowing the mixture to were added before titrated with 0.01 N sodium thiosulphate standard
stand in the dark for 30 min (Siripatrawan & Harte, 2010). The extracts solutions. Values obtained were expressed as milliequivalents of active
of the films were obtained the same as TPC. The mixture was measured oxygen per kilogram of sample (meq/kg).
at 517 nm by using a spectrophotometer (Shimadzu UV–vis 1601,
Japan), and the percentage of DPPH scavenging activity was determined 2.7.2. Thiobarbituric acid reactive substances (TBARS)
using Eq. (2) below: TBARS of margarine were evaluated according to the method as
described by Tananuwong & Tewaruth (2010). The sample was pre­
AbsDPPH–Absextract
DPPHscavengingactivity(%) = × 100 (2) pared by mixing 50 mg of margarine with 1-butanol and was marked up
AbsDPPH
until 25 mL in a volumetric flask. Then, 5 mL of the solution was added
where the absorbance of the ethanolic DPPH solution is denoted as Abs with 0.2 % of TBA in 1-butanol. The mixture was incubated at 95 ◦ C of
DPPH and Abs extract represents the absorbance of the sample extract. water bath for 2 h. Finally, the absorbance was read at 532 nm and the
The DPPH for the control film (PE) was not evaluated, as there was no reaction was calculated by the following equation:
antioxidant added in the PE film.
TBARS = [50 × (Asample – Areagent blank)] / m (3)

2.6.7. Scanning electron microscopy (SEM) whereby, m denoted as mass of sample (mg) and the TBARS value was
The morphology of the surface area and cross-sections of the films expressed as (mg− 1).
was visualized at up to 1500× magnification by using scanning electron
microscopy (JSM 6400, Jeol, Tokyo, Japan). Pre-conditioned film 2.7.3. Colour measurement for margarine
samples were cut into 1 × 1 cm by using a blade cutter at room tem­ The colour of margarine was evaluated by Hunter Lab Ultrascan PRO
perature. The exposed edges of the film were mounted onto stubs spectrocolourimeter (Model A60− 1012-402, VA, USA). White tile was
vertically to obtain the visualization of the cross-section of the film. The used for calibration and the sample was defined by whiteness (L value),
flat surface of the film was mounted onto the stub for the visualization of green to red (a value) and blue to yellow (b value).
the surface area. Then, the stubbed samples were sputtered with gold by
using a sputter coater SCD 005 (BAL-TEC AG, Balzers, Liechtenstein) 2.7.4. pH of margarine
before visualization. The pH of margarine was determined using a pH meter (pH 700,
Eutech Instruments, Singapore) after being standardized with pH 4 and
pH 7 buffers.

Table 2
Colour properties and transparency of polyethylene (PE) and polyethylene/ 2.8. Statistical analysis
gelatin bilayer films (PE/G) films.
%T Statistical analysis was performed using one-way analysis of variance
Films L a b (ANOVA) in Minitab (Version 17, Minitab, Pennsylvania, USA), and the
T280 T660
differences between means were compared using Tukey’s test method of
PE 89.3 ± 0.6a − 1.2 ± 0.0a 1.6 ± 0.0e 0.02 ± 0.00a 55.6 ± 0.3c
comparison at a 95 % significance level.
PE/ 87.2 ± 0.5b − 1.7 ± 0.0b 4.7 ± 0.2d 0.01 ± 56.2 ±
G10 0.01ab 0.9cb
PE/ 86.7 ± − 1.8 ± 5.60 ± 0.01 ± 56.7 ± 3. Results and discussion
G20 0.3bc 0.1bc 0.1c 0.01bc 0.4cb
PE/ 86.0 ± − 1.8 ± 0.0c 7.3 ± 0.3b 0.01 ± 57.1 ± 0.6b
G40 0.0cd 0.01cd
3.1. Film thickness
PE/ 85.6 ± 0.2d − 2.0 ± 0.1d 9.4 ± 0.3a 0.01 ± 0.00d 59.5 ± 0.4a
G60 Table 1 shows the total thicknesses of the bilayer films. The expected
Values are given as mean ± standard deviation (n = 3). Means in the same values of film thicknesses were expressed as the total thickness of PE
column with different superscript letters are significantly different (p ≤ 0.05). single layer film with the initial thickness of casted gelatin layer (10, 20,
Lowercase letters indicate comparison between different types of films. PE/G10, 40 & 60 μm) onto the PE film. Whereas, the total measured thickness
PE/G20, PE/G40, and PE/G 60 represents the bilayer films with 10, 20, 40, and values were obtained after the bilayer films were dried and conditioned.
60 μm gelatin thicknesses, respectively. The thicknesses of the bilayer films were significantly (p ≤ 0.05)

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A. Nor Adilah et al. Food Packaging and Shelf Life 26 (2020) 100577

Fig. 1. SEM micrographs and the images of the polyethylene (control) and the polyethylene/gelatin bilayer films (PE/G) at different thicknesses.

different from those of single PE films. The average thicknesses were the bilayer films were more yellow than the control. The yellow tint of
slightly different from the expected values; however, the thicknesses the bilayer films (as shown in Fig. 1) could be due to the presence of MPE
were still within an acceptable range (±5 μm). The differences in total in the gelatin coating. The MPE contained pigmented compounds called
thicknesses could be due to the drying of the films. The uneven drying carotenoids (Maldonado-Celis et al., 2019), which gave the mango peels
rate could have caused some parts of the films to be thicker than the colours ranging from orange to yellow. The colour intensified as the
others. The total thickness of polyethylene/gelatin bilayer films at 20 μm mangoes ripened due to the high levels of carotenoids produced (Haque
(PE/G20) was slightly higher compared to its expected thickness, et al., 2015).
probably due to the non-uniform dispersion of the film-forming solution The transparencies of the PE and polyethylene/gelatin bilayer films
onto the PE single layer. Therefore, multiple random sites were (PE/G) were recorded as the % of transmittance at 280 nm (UV-light)
measured to obtain the average values. In addition, the rearrangement and 660 nm (visible light). An increase in the thickness of the films up to
of the protein structures in the gelatin matrix due to the evaporation of 155.80 μm showed a significant (p ≤ 0.05) difference in transmittance
water molecules could have reduced the thickness of the coating. compared to that of the control film. Additionally, the increase in
thickness resulted in a decrease in transmittance at 280 nm. A very low
3.2. Colour and transparency of bilayer films transmission (0.02 to 0.01 %) at 280 nm denoted excellent functionality
as a UV barrier, as only a low amount of light could pass through the
Table 2 shows the colour and transparency measurements of bilayer bilayer films. The prevention of UV light transmission could be attrib­
films. The results showed that the addition of a gelatin layer of various uted to the presence of phenolic compounds in the gelatin matrix. This
thicknesses on PE significantly (p ≤ 0.05) affected the colour of the result is in agreement with those of the studies by Wang & Rhim (2015)
films. Gelatin coatings of 10–60 μm significantly (p ≤ 0.05) decreased and Wu et al. (2013). In addition, the high content of aromatic amino
the L- and a-values of the bilayer films compared to those of the control. acids content in the protein-based films also acted as UV-absorbers,
However, a further increase in the thickness significantly (p ≤ 0.05) thereby providing the films with good UV barrier properties (Jiang
increased the b-value of the bilayer films. High b-values suggested that et al., 2010; Mohajer et al., 2017). This result indicated that these films

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Fig. 2. Peroxide values of margarine in polyethylene (PE) and polyethylene/gelatin bilayer films (PE/G) films stored at 4 ◦ C and 25 ◦ C.

can potentially protect UV-sensitive food from deterioration. Generally, released TPC when the thickness of the gelatin layer was increased from
the visible light (660 nm) transmittance of all films was in the range of 10–60 μm. The reduction in the released TPC values could have been
55.6%–59.5%. Data also showed an increase in the light transmittance caused by the low diffusivity of phenolic compounds from the gelatin
at 660 nm, with a significant (p ≤ 0.05) finding between the PE and layer to the extracting solvent. An increase in the thickness of the gelatin
bilayer films with gelatin thickness of 60 μm (PE/G60). This result layer led to the creation of a greater protein network. More protein-
showed that all the bilayer films were suitable for use as transparent phenolic compound interactions occurred within the gelatin matrix,
packaging materials because their UV protection effect could prevent and the resultant reduction in the free movement of phenolic com­
the oxidation of packaged foods (Martins et al., 2012; Wang & Rhim, pounds in the medium reduced their reaction with the Folin-Ciocalteu
2015). reagent. It can be suggested that thicker films slowed down the release
of phenolic compounds into the medium. This result was in agreement
3.3. WVP with Rossi-Marquéz et al. (2009), whereby thinner films increased the
rate of antimicrobial release, as the compounds only needed to pass
The WVP of the bilayer films was significantly (p ≤ 0.05) higher than through a short distance of film to reach the aqueous solution. This slow
that of the control (Table 1). An increase in the thickness of the coating release of phenolic compounds is favourable if active packaging aims to
from 10–60 μm led to a WVP increase from 3.8 × 10− 10 to 7.2 × 10− 10 g. prolong the shelf lives of food products over a long period.
mm/m2.s.kPa. The increase in thickness of the coatings resulted in a Also, DPPH radical scavenging activity (DPPH) of the bilayer films
greater number of polar groups, causing the films to be more hydrophilic was significantly (p ≤ 0.05) different from that of the control film.
(Kokoszka et al., 2010; Rahmani et al., 2017). Gelatin is known to have a (Table 1). The bilayer films exhibited a gradual increase in DPPH when
great affinity for water molecules (Nur Hanani et al., 2012) due to the their thickness increased. The DPPH increased as the TPC decreased.
presence of hydrophilic amino acids in the gelatin structure (Mohajer Maryam Adilah and Nur Hanani (2016) and Yang et al. (2016) have
et al., 2017). reported that the content of the phenolic compound in the extracts in­
Furthermore, the compounds in the MPE that formed hydrogen fluences their antioxidant activities. In this study, the DPPH of the films
bonds with the gelatin molecules reduced the availability of free gelatin did not correlate with the amount of phenolic compounds present. It can
molecules for binding with water molecules. Therefore, thick coatings be suggested that the DPPH of the films was attributed to the peptide
with a large gelatin matrix favoured the binding of water with free fragments of the gelatin layer. Amino acids such as glycine and proline
gelatin molecules over binding with MPE compounds. Hu et al. (2016) that were present in the peptide chain were responsible for the antiox­
stated that the polar molecules of phenolic compounds could also affect idant function (Tongnuanchan et al., 2014). As the thickness of the
the WVP of bilayer films through their binding with water molecules. gelatin layer was increased, a greater cross-sectional area was available
The phenolic compounds in the MPE contained various compounds with for free peptide fragments to react with free radicals. The subsequent
different aromatic phenyl rings and hydroxyl groups. When the thick­ formation of a stable end product increased the DPPH capabilities of the
ness of the gelatin coatings increased, hydroxyl groups of the phenolic films.
compounds combined with water molecules and subsequently intensi­ In addition, the antioxidant function of gelatin can also be influenced
fied the adherence of water to the coatings. Hence, higher WVP values by other factors, such as the molecular weight of the gelatin, confor­
were observed in bilayer films than in PE films. mations and positions of amino acids in the peptide sequence, the type of
Moreover, the WVP was also influenced by the hydrophobic nature hydrolysis (acidic, alkaline, or enzymatic), and protease specificity
of the PE films, which reduced the number of water molecules released (Alemán et al., 2011; da Trindade Alfaro et al., 2015). Although pure
to the outer layer of the bilayer films. This resulted in the trapping of gelatin films have been reported to exhibit antioxidant activity (Biten­
water molecules within the hydrophilic inner coating, much like a court et al., 2014; Gómez-Estaca et al., 2009; Jridi et al., 2014), the
‘reservoir’. Therefore, an increase in the thickness of the gelatin layer up mechanism behind this reaction has not been studied.
to 60 μm could increase the binding of water molecules to the gelatin
layer, increasing the adsorption of water vapour to the inner layer of the 3.5. Film microstructure
PE films.
The surface and cross-sectional morphologies of the bilayer films are
3.4. Released TPC and DPPH of bilayer films represented in Fig. 1. It can be observed that PE films were smooth, non-
porous, and had no agglomeration surfaces. Conversely, some bilayer
The released total phenolic content (TPC) of the bilayer films is films with gelatin thickness of 20 μm (PE/G20), 40 μm (PE/G40), and 60
shown in Table 1. The results demonstrated a decreasing trend in the μm (PE/G60) had a few grainy structures on their surfaces, unlike the

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Fig. 3. TBARS of margarine in polyethylene (PE) and polyethylene/gelatin bilayer films (PE/G) films stored at 4 ◦ C and 25 ◦ C.

other films (Fig. 1c, 1d and 1e). The grain-like structures on the surfaces et al. (2014) also showed a reduction in the peroxide value of butter
of the bilayer films could have arisen due to conformational changes in when it was packed in a nanocellulose starch-based film with propolis
the gelatin sequence when the gelatin-phenolic compound interactions compared to low-density polyethylene (LDPE) film. This suggests that
resulted in the development of protruded structures on the film matrices. gelatin coatings incorporated with MPE provides an additional gas or
In addition, the agglomeration of MPE on the gelatin layer during drying light barrier on the PE film, which impacts the oxidation process of the
may have been another factor in the formation of these grain-like margarine. Besides, delay in the oxidation process of margarine could
structures. However, all of the films were free from any visible voids also occur because of the radical scavenging antioxidant compounds
or cracks on their surfaces. present in MPE as observed from the previous DPPH scavenging activity.
Through analysis of the cross-section, it was observed that all films Mahdi et al. (2015) and Pawar et al. (2012) implied that the addition of
were dense, compact, and continuous. The PE films, which were derived fennel seed extract and ethanolic herb extract as the source of antioxi­
from polymerized monomers, were closely packed, forming linear-like dant could slow down the PV during storage of margarine and ghee,
PE chains that subsequently gave rise to a crystalline network. Simi­ respectively. Furthermore, the addition or concentration of mango
larly, the active gelatin layer on the PE also showed a homogenous and kernel oil in films also helped the oxidation stability of butter oil
ordered matrix structure due to the linear structure of the polypeptide (Nadeem et al., 2017).
chains. The incorporation of MPE also maintained the integrity of the Supposedly, the active gelatin layer is effective as an antioxidant to
biopolymers without disrupting the protein-protein interactions. In inhibit lipid oxidation but margarine in PE/G stored at 25 ◦ C was an
addition, an increase in the thickness of the gelatin layer up to 60 μm exception. It produced significantly (p ≤ 0.05) higher amount of PV as
increased the number of gelatin networks available for binding with compared to margarine in PE/G stored at 4 ◦ C. This showed that
phenolic compounds via hydrogen bonding. Moreover, no distinct film oxidation of margarine could be affected by the temperature. It could be
separation or gaps were observed in the bilayer films. This result re­ due to the greater formation rate of oxidative molecules from the un­
flected the good adhesion compatibility of both hydrophobic and hy­ saturated fatty acid from the soybean oil used in margarine making,
drophilic components of the PE and gelatin layers. which is more susceptible to oxidation at room temperature compared to
4 ◦ C. Subsequently, degradation of the unsaturated oil could influence
the increase in the PV of the margarine at 25 ◦ C. This difference was also
3.6. Peroxide value of margarine observed by Rudzińska et al. (2014), where margarine stored at 20 ◦ C
showed about 81 % higher PV value compared to margarine stored at 4
The purpose of antioxidant active packaging is to improve the ◦
C. Likewise, the rise in PV at different storage temperatures was studied
oxidation stability of the food product. The primary oxidation products by Nadeem et al. (2017).
of margarine can be measured as peroxide value (PV). Oxidation of
margarine during storage for 28 days at 4 ◦ C and 25 ◦ C is represented in
Fig. 2. The result showed that all samples increased in PV and reached a 3.7. TBARS
maximum value after 28 days of storage. At the end of storage, marga­
rine packed in polyethylene/gelatin bilayer films (PE/G) and stored at 4 The formation of secondary oxidation products (aldehydes and
◦
C showed the lowest PV compared to margarine packed in PE and carbonyl compounds) which triggers the off-flavor attribute of a food
stored at 4 ◦ C and 25 ◦ C. After 7 days of storage, the PV of margarine product was measured by TBARS test (Santos et al., 2014). The changes
packed in PE/G and stored at 4 ◦ C was able to be slowed down up to 56 of TBARS values for margarine packed in PE and polyethylene/gelatin
% until the 21st day. This may be due to the antioxidant activity of the bilayer films (PE/G) during storage at different temperatures are pre­
phenolic compounds present in the MPE from the active gelatin layer, in sented in Fig. 3. Margarine packed in PE and stored at 25 ◦ C exhibited
which its maximum oxidation inhibition of the margarine sample was the highest increment of TBARS up to 78 % on the 28th day of storage
observed on day 21. In contrast, an increase in PV up to 74 % was compared to day 0, followed by margarine in PE/G stored at 25 ◦ C, PE at
observed from day 7 to day 28 for margarine in PE/G stored at 25 ◦ C. An 4 ◦ C, and PE/G at 4 ◦ C with 52 %, 50 %, and 30 % increase in TBARS
increase in the PV of margarine in PE at 4 ◦ C and 25 ◦ C starting from day value on the last day of storage, respectively. Also, margarine packed in
7 to day 28 was seen, with the increments being 60 % and 47.5 %, PE without coating had higher TBARS value compared to PE/Gpacked
respectively. margarine, regardless of temperature. The presence of MPE within the
PV is influenced by several factors such as the type of oil, free fatty inner layer of the packaging material improved the lipid oxidation for
acid content, degree of saturation, packaging materials, pH, tempera­ margarine packed in PE/G stored at both 4 ◦ C and 25 ◦ C.
ture, light, and storage conditions (Hu et al., 2016). Notably, packing Previous evaluation on the scavenging activity showed that PE/G
margarine in PE/G and storing at 4 ◦ C was a more effective strategy to films exhibited DPPH after the films were immersed in ethanol, which
control lipid oxidation compared to packing in a PE. A study by Costa acted as a medium to release the MPE compounds for inhibiting DPPH

6
A. Nor Adilah et al. Food Packaging and Shelf Life 26 (2020) 100577

Fig. 4. pH changes of margarine in polyethylene (PE) and polyethylene/gelatin bilayer films (PE/G) films stored at 4 ◦ C and 25 ◦ C.

and PE/G-packed margarine stored at 25 ◦ C, with 0.48 and 0.22 mg− 1

Table 3
respectively. This result coincides with the ones obtained by Matumo­
Colour measurement of margarine packaged in polyethylene (PE) and poly­
to-Pintro et al. (2017) who stated that storage temperature also affected
ethylene/gelatin bilayer films (PE/G) films stored at 4 ◦ C and 25 ◦ C.
the lipid oxidation of food sample.
4 ◦C 25 ◦ C
Days
PE PE/G PE PE/G 3.8. pH of margarine
L value
0 72.0 ± 0.8aA 72.0 ± 0.8aA 72.0 ± 0.8aA 72.0 ± 0.8aA Value of pH is the measurement of free acid or hydrogen ions within
3 69.6 ± 0.8aA 64.1 ± 1.0cB 66.1 ± 0.6bB 66.5 ± 1.5bB
a product. Usually, it is defined as the negative log of hydrogen ions. The
7 70.8 ± 1.0aA 66.5 ± 0.4bB 58.0 ± 0.6cC 57.9 ± 0.2cC
10 66.2 ± 1.3bA 66.1 ± 0.6bA 50.6 ± 0.8dB 51.0 ± 0.5dB pH values of margarine at both 25 ◦ C and 4 ◦ C are presented in Fig. 4.
14 62.6 ± 0.3cA 61.2 ± 0.6dA 48.4 ± 0.6eB 49.0 ± 0.7dB The pH of all samples ranged from 4.43 to 5.16. The lowest pH value
18 57.5 ± 0.8dB 63.3 ± 0.1cA 47.2 ± 0.5efD 49.2 ± 1.2dC observed at the end of storage period was for margarine in PE stored at
21 58.5 ± 0.2dB 60.5 ± 0.4dA 45.8 ± 0.5fC 43.5 ± 0.4eD 25 ◦ C, with the pH of 4.43 and 14 % reduction from the control (day 0).
28 55.8 ± 2.0dA 52.2 ± 0.5eB 40.0 ± 0.5gC 38.4 ± 1.2fC
Meanwhile, margarine packed in polyethylene/gelatin bilayer films
a value
0 − 2.8 ± 0.2fA − 2.8 ± 0.2fA − 2.8 ± 0.2gA − 2.8 ± 0.2gA (PE/G) and stored at 4 ◦ C had a lower reduction in pH, 9%. Notably, all
3 − 2.4 ± 0.1eC − 2.0 ± 0.0eB − 1.8 ± 0.1fA − 2.3 ± 0.1fC margarine showed a significant decrease (p ≤ 0.05) in pH at the end of
7 − 1.8 ± 0.0dB − 1.9 ± 0.0eC − 1.6 ± 0.0efA − 2.1 ± 0.0eD storage period as compared to day 0. This pH changes may be due to the
10 1.7 ± 0.0cdB 1.7 0.1deB − 1.4 ± 0.0deA − 1.6 ± 0.0dAB
− − ±
formation of oxidation by-products as previously discussed in terms of
14 − 1.6 ± 0.0cC − 1.5 ± 0.0cdB − 1.3 ± 0.0cdA − 1.6 ± 0.0dC
18 − 1.5 ± 0.0cC − 1.3 ± 0.1bcB − 1.1 ± 0.0bcA − 1.2 ± 0.1cAB
PV and TBARS values. The oxidation by-products consists of various
21 − 1.3 ± 0.0bB − 1.0 ± 0.2bA − 1.0 ± 0.0bA − 0.8 ± 0.0bA mixtures which includes volatile, non-volatile and polymeric products
28 − 0.4 ± 0.1aC − 0.5 ± 0.1aC 1.4 ± 0.1aA 0.3 ± 0.0aB such as aldehydes, ketones, alcohols, hydrocarbons, epoxy compounds
b value and organic acids (Khanum & Thevanayagam, 2017). Moreover, the
0 20.3 ± 0.8aA 20.3 ± 0.8aA 20.3 ± 0.8aA 20.3 ± 0.8aA
changes in pH of margarine could be caused by the hydrolysis reaction of
3 19.6 ± 0.5abA 19.2 ± 0.1abA 20.0 ± 0.3aA 19.4 ± 0.3aA
7 18.9 ± 0.2bcA 18.7 ± 0.5abcA 17.2 ± 0.4bB 16.7 ± 0.1bB the blended oils used to form free fatty acids.
10 18.1 ± 0.4cdA 18.2 ± 0.1abcdA 17.3 ± 0.1bA 15.8 ± 0.6bB
14 18.2 ± 0.1cdA 17.4 ± 0.3bcdAB 16.9 ± 0.1bcB 15.9 ± 0.6bC
3.9. Colour of margarine
18 17.6 ± 0.3dA 17.3 ± 0.9bcdA 15.9 ± 0.1cdB 15.5 ± 0.3bcB
21 17.6 ± 0.2dA 16.6 ± 0.3cdA 14.9 ± 0.4deB 14.0 ± 0.8cdB
28 16.0 ± 0.3eA 16.2 ± 1.7dA 14.8 ± 0.2eAB 13.1 ± 1.0dB The whiteness, green/redness, and blue/yellowness of margarine are
represented as L, a, and b values, respectively. Colour measurements of
Values are given as mean ± standard deviation (n = 3). a–g: different letters
indicate significant difference (p ≤ 0.05) in the same column. A-D: different
margarine during 28 days of storage at 4 ◦ C and 25 ◦ C are shown in
letters indicate significant difference (p ≤ 0.05) in the same row. PE/G10, PE/ Table 3. The whiteness of packed margarine decreased after 28 days of
G20, PE/G40, and PE/G 60 represents the bilayer films with 10, 20, 40, and 60 storage, regardless of their temperature or packaging type. Both PE- and
μm gelatin thicknesses, respectively. polyethylene/gelatin bilayer films (PE/G)-packed margarine stored at
25 ◦ C were significantly different (p ≤ 0.05) compared to the ones stored
free radicals. Therefore, it can be assumed that MPE compounds were at 4 ◦ C on day 28. Margarine in PE/G stored at 25 ◦ C on day 28 was 47 %
released into the margarine and subsequently retard the lipid oxidation darker compared to day 0. This may be due to the migration of MPE from
during the 28 days of storage. Migration or slow release mechanism of the active coating into the margarine, imparting a darker colour.
antioxidant towards food sample may be the reason for the antioxidant Also, an increase (p ≤ 0.05) in a-values was observed for all samples
compounds to suppress oxidation process over time (Bolumar et al., on the 28th day. Margarine packed in PE and stored at 25 ◦ C on day 28
2016; Bolumar et al., 2011). The antioxidant activity was contributed by had the most positive rise of a-value from -2.8 (day 0) to 1.4. This in­
the phenolic compounds present in MPE, which acted as electron or dicates that margarine stored at 25 ◦ C is more prone to redness
hydrogen donors by slowing the production of secondary products and compared to margarine stored at 4 ◦ C. Initially, the margarine produced
conjugating dienes as well as decreasing the formation of hydroperox­ in this study was whitish in colour (Fig. 5) which differed from com­
ides (El-Shourbagy & El-Zahar, 2014). mercial margarine due to the absence of colourant in the margarine-
In this study, margarine packed in PE/G stored at 4 ◦ C showed the making process. The colour changes may be caused by the oxidation
lowest TBARS value (0.07 mg− 1) at the end of storage period than PE- of the samples, which can be expressed by their PV and TBARS value.
Esmaeilifard et al. (2016) stated that the redness of margarine was

7
A. Nor Adilah et al. Food Packaging and Shelf Life 26 (2020) 100577

Fig. 5. Packed margarine in polyethylene (PE) and polyethylene/gelatin bilayer films (PE/G) at day 0 and day 28 stored at 4 ◦ C and 25 ◦ C.

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Declaration of Competing Interest 100451.
Haque, S., Begum, P., Khatun, M., & Islam, S. N. (2015). Total carotenoid content in some
mango (Mangifera indica) varieties of Bangladesh. International Journal of
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