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International Journal of Biological Macromolecules 236 (2023) 124042

Contents lists available at ScienceDirect

International Journal of Biological Macromolecules


journal homepage: www.elsevier.com/locate/ijbiomac

Sodium alginate edible coating to reduce oil absorption of French fries with
maintaining overall acceptability: Based on a water
replacement mechanism
Ying Li , Xue Bai , Mengna Zhao , Hui Wang , Jia Feng , Xiufang Xia *, Qian Liu *
College of Food Science, Northeast Agricultural University, Harbin, Heilongjiang 150030, China

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

Keywords: The effect of sodium alginate (SA) coating on the oil content and quality of fries was evaluated, and the
French fries inhibitory mechanism of SA on oil absorption was analyzed based on the water replacement theory. Compared to
Sodium alginate coating uncoated samples, the penetrated surface oil (PSO), structure oil (STO), and total oil (TO) contents, a*, and b* of
Water migration
coated fries decreased, whereas moisture content, L* and hardness increased with no significant difference
Oil absorption
Food quality
revealed by sensory evaluation of all samples. The water contact angle of the films correlated negatively with the
Oil content water content and hardness of the fries. In contrast, it correlated positively with PSO, STO, and TO contents. The
TO content of fries with 1 % SA film which had a compact microstructure, was the lowest, reduced by 52.5 %
compared to the control sample. SA coating reduces the pores and roughness on the fries' surface, which inhibits
the oil from penetrating into the samples. SA coating decreased the T21, T22, and pores of the starch, and
increased the P2b, P21, relative crystallinity, and ΔH significantly (P < 0.05). Therefore, SA coating inhibits the
oil absorption in fries by reducing water evaporation which is attributed to the increase in double helices and
crystallinity of starch.

1. Introduction uptake in fried food including water replacement [1]: (1) the water in
fried food evaporates to form channels which oil penetrates; (2) the
With their golden color, crispy taste, and typical frying flavors, cooling-phase effect: the oil is sucked into the cracks in the crust of fried
French fries cater to the contemporary fast-paced, low-priced mass food during the cooling phase due to a “vacuum effect”; (3) surface-
consumption habits, being a popular fast food worldwide. In Europe, active agents: the oil undergoes a hydrolysis reaction during frying,
potato supply reached 1,964,759 t in 2019, and frozen potatoes which reduces the interfacial tension between oil and food. The jury is
accounted for 50 % of the total supply of potatoes, most of which are still out on which of these three mechanisms is the dominant one.
used for manufacturing French fries (FAO, 2019). Texture accounts for Studying the main oil absorption mechanism of fried food can signifi­
30 % of the quality score of French fries [1], and their crispy texture and cantly help in exploring more effective measurements in oil reduction.
crunching sound bring a pleasant feeling to consumers. The excellent Current studies related to oil content reduction focus on monitoring
sensory qualities of fries are attributed to starch gelatinization [2], frying conditions [5], frying technology development [6], pre-treatment
Maillard reaction [3], and changes in the surface microstructure [4], [7], and food surface modification [8]. Some researchers analyzed the
resulting from heat and mass transfer (moisture loss and oil uptake) changes in the oil content of potato strips fried with different oils or at
during frying. In addition to imparting a crispy texture to the fries, the different temperatures and frying times. Still, the found effect on oil
porous structure of the fries is also a major channel for the migration of reduction was not noteworthy [5,9]. Innovative frying technologies and
moisture and oils. During frying, the removal of water forms empty pre-treatment methods, such as air frying [6], electric field frying [7],
spaces for oil to enter, resulting in up to 35 % oil content in the food [4], and hot-air pre-drying [6], positively affect oil reduction, but, regret­
which leads to an increased incidence of obesity, heart diseases, and tably, are time-consuming and energy-intensive [10]. Compared with
certain cancers for consumers who prefer deep-fried food [1]. these methods, using an edible coating to inhibit the oil uptake in fried
Three possible mechanisms have been proposed to explain the oil food has the advantages of being low-cost, wide sources of materials,

* Corresponding authors.
E-mail addresses: xiaxiufang@neau.edu.cn (X. Xia), liuqian@neau.edu.cn (Q. Liu).

https://doi.org/10.1016/j.ijbiomac.2023.124042
Received 26 December 2022; Received in revised form 6 March 2023; Accepted 10 March 2023
Available online 15 March 2023
0141-8130/© 2023 Elsevier B.V. All rights reserved.
Y. Li et al. International Journal of Biological Macromolecules 236 (2023) 124042

convenient operation, and so on. Nowadays, some natural poly­ 2.5.2. Water contact angle (WCA)
saccharide coatings such as pectin [3] and guar gum [10] have been The hydrophilicity of the coating films was assessed by WCA mea­
used to inhibit oil absorption in fried food, reducing the potato chips' oil surements using a contact angle meter (Data Physics, Germany). Milli-Q
content by 31.0 % and 26.9 %, respectively. Polysaccharide coatings purified water (3 μL) was dropped on the film surface, and an angle
reduce water loss and change the surface structure by forming barrier image was taken with a digital camera.
coatings on the food surface [11]. However, pectin treatment adversely
affects the overall acceptability of samples [3]. Meanwhile, guar gum is 2.5.3. Thickness and viscosity
generated from guar beans at a high cost [10]. Sodium alginate (SA), a The thickness of the films was measured by a digimatic micrometer
by-product sourced from brown algae [12], is edible, highly hydrophilic (YHT127, Guangdong, China). Ten values obtained at different positions
[13], flexible [14], and low-permeable to oil [15], and has already been of each sample were used to calculate the average thickness.
used as a coating for food packaging and preservation [16]. In contrast, The viscosity of the coatings was evaluated using a viscometer
its applications for oil reduction have been few. (*DVS+, China). The test was performed in triplicates.
Therefore, the purpose of this study is to use a natural, environ­
mentally friendly, and low cost edible coating to reduce the oil uptake 2.5.4. Mechanical properties
and improve the quality of French fries, and provide insights into the The films' tensile strength (TS) and elongation at break (EB) were
water replacement mechanism by studying (1) the effect of SA coating tested on a texture analyzer (TA.XT Plus C, Stable Microsystems, UK).
on the water content, oil fraction content, and quality of samples; (2) the The films were cut into 10 × 50 mm rectangular strips according to Zhao
relation between the films' properties and the water content, oil content, et al. [17].
and quality of the French fries; (3) the effect of SA coating on the
macroscope and microscope oil distribution, and surface microstructure 2.5.5. Water vapor transition rate
of fries; (4) the effect of SA coating on the crystallinity and double he­ The water vapor transition rate (WVTR) of the films was evaluated
lices of starch in fries. following the ASTM E-96 procedure (2016). Distilled water was placed
in a 50 mL centrifuge tube, and the distance from the water surface to
2. Materials and methods the tube mouth was kept at 2–3 cm. The film was sealed to the tube
mouth and closed tightly. The tube was then weighed and placed into a
2.1. Materials constant-temperature-humidity chamber (BPS-50CL, Shanghai, China)
set at 25 ◦ C with 75 % relative humidity. The tube was weighed once
SA was supplied by Qingdao Bright Moon Seaweed Group Co., Ltd. every 24 h until the weight reduction reached equilibrium. All samples
(Qingdao, China). The frozen potato strips were obtained from Lamb were tested in triplicates, and the WVTR and water vapor permeability
Weston Potato Industry Co., Ltd. (Inner Mongolia, China), cut into 10 × (WVP) were calculated according to Eqs. (1) and (2):
10 × 50 mm strips, and stored at − 18 ◦ C. The soybean oil for the ( )/
WVTR = Δm × Tf A × t (1)
experiment was obtained from the local market (Harbin, China).
( )/
WVP = Δm × Tf (A × t × Δp) (2)
2.2. Preparation of coating solutions and films
where Δm (g) is the difference in tube weight, Tf (mm) is the thickness of
The SA was added to distilled water to prepare polymeric solutions of the film, A (m2) is the effective area of the films, t (d) is the time interval,
0.5, 1.0, 1.5, and 2.0 % (w/v). Ultrasound was used to remove air and Δp is the saturation vapor pressure of water (Pa) at 25 ◦ C (1754 Pa).
bubbles from the film-forming solution. The solutions were then poured
into disposable Petri dishes and dried at 30 ◦ C for 36 h [17]. Finally, the 2.5.6. Oil resistance
SA films (SAFs) were peeled off the Petri dishes. The oil resistance of the films was determined as per the TAPPI T559
cm-12 standard (1996).

2.3. Preparation of coated French fries


2.6. Moisture content and oil fraction contents
The pre-fried frozen potato strips were immersed into the respective
SA solutions (0.5, 1.0, 1.5, and 2.0 %) for 5 s. After draining off the The moisture content of fries was evaluated according to the
excess liquid, the coated strips were then fried in soybean oil at 170 ◦ C methods of AOAC (2000).
for 3 min using a thermostatically temperature-controlled fryer (DF25A, The oil fraction contents (g/100 g db) of fries were measured ac­
Guangzhou, China) (uncoated potato strips were used as control sam­ cording to the method described by Li et al. [18]. The French fries were
ples). After frying, the samples were subsequently shaken in an quickly taken out of the fryer and immersed into a constant-weight
aluminum basket to drain off excess oil for 30 s. Then, all samples were aluminum box containing 30 mL petroleum ether for 1 to 2 s. The oil
allowed for further analysis. content dissolved in petroleum ether was computed as the sum of the
surface oil (SO) and penetrated surface oil (PSO) contents. The same
measurement was carried out after the fries had been removed from the
2.4. Extraction of potato starch frying oil for 20 min, and the result was classified as the SO content. The
measurements were repeated six times. After removing SO and PSO, the
The starch of the unfried potato strips, uncoated French fries, and SA- fries were freeze-dried (Pilot3-6 M, Beijing, China), and the remaining
coated fries was extracted, according to Li et al. [18]. oil was extracted by the Soxhlet extraction method. This oil fraction was
classified as structure oil (STO). The total oil (TO) content was expressed
2.5. Analysis of coating films as the sum of SO, PSO, and STO contents. The TO content was measured
by Soxhlet extraction.
2.5.1. Microstructure
The SA films were fixed on the metal sample stage. The cross-sections 2.7. Quality of French fries
were examined with a scanning electron microscope (SEM) (TM-5570,
Hitachi High-Technologies Corp., Tokyo, Japan) at 2500× 2.7.1. Color
magnification. The skin color of the French fries was measured using a ZE-6000

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Y. Li et al. International Journal of Biological Macromolecules 236 (2023) 124042

Fig. 1. The preparation process of SA film (a); effect of sodium alginate concentrations on the microstructure (b1, b2, b3, b4), water contact angle (c), thickness and
viscosity (d), mechanical properties (e), and barrier properties (f) of films.
SAF-0.5, SAF-1.0, SAF-1.5, SAF-2.0 indicates 0.5 % SA films, 1 % SA films, 1.5 % SA films, 2.0 % SA films. The results are expressed as the mean ± standard error.
Different lower-case letters (a-d) denote significant differences within different samples (P < 0.05).

colorimeter (Juki Corp, Tokyo, Japan). The test was repeated three et al. [21] and Yang et al. [22], with little modification. A 1-mm dried
times. Color difference (ΔE) and Browning Index (BI) were expressed as sample section was observed at a 10× magnification using a 514 nm
follows [18]: laser. The obtained images were processed using the Lecia confocal
√̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅ software (Lecia Microsystems, Germany).
ΔE = (L* − L0 * )2 + (a* − a0 * )2 + (b* − b0 * )2 (3)
2.9. Microstructure
BI = (100 × (x − 0.31) )/0.17 (4)
The microstructure of the French fries was observed using an SEM
x = (a* + 1.75L* )/(5.645L* + a0 * − 3.012b* ) (5) (TM 5570, Hitachi High-Technologies Corp., Tokyo, Japan). The de-
oiled and freeze-dried surface slices of the fries were fixed on the
where L0*, a0*, and b0*: the color of unfried fries; L*, a*, and b*: the metal sample stage. Surface microstructure images were acquired at an
color of fried fries. accelerating voltage of 5 kV and 160× magnification.

2.7.2. Texture 2.10. Water states


The texture of the samples was measured by a puncture test using a
TA.XT Plus C texture analyzer (Stable Microsystems, UK) by the methods The water proton signal of unfried, control, and SA-coated samples
of Li et al. [18] and Zhang et al. [19]. was determined using a magnetic resonance imager [23] (MRI,
MesoMR23-060H-I analyzer, Newmart Analytical Instruments Co., Ltd.,
2.7.3. Sensory evaluation Suzhou, China) following the methods of Li et al. [18].
The freshly fried samples were placed in disposable meal boxes with
random 3-digit numbers and served to 20 trained panelists, which were
2.11. Starch solubility and swelling power
divided into 2 groups of 10 people. The panelists evaluated five sensory
attributes: color, texture, flavor, oiliness, and overall acceptability (on a
The starch solubility and swelling power of samples were determined
1–9 scale).
by the methods of Li et al. [18].

2.8. Water and oil distribution, oil distribution 2.12. X-ray diffraction

The macroscopic water and oil distribution of the fries were observed The relative crystallinity of the samples was analyzed using an X'Pert
by a magnetic resonance imager (MRI, MesoMR23-060H-I analyzer, Pro diffractometer (PA 148 Nalytical B.V., The Netherlands) at 2θ in the
Newmart Analytical Instruments Co., Ltd., Suzhou, China) according to 4◦ to 40◦ range.
Wang et al. [20]. The Spin-echo (SE) sequence parameters were: 23.312
MHz resonance frequency, 0.5 T magnet strength, 20 ms echo time (TE), 2.13. Differential scanning calorimetry (DSC)
and 500 ms repetition time.
The microscopic oil distribution was evaluated using a confocal laser The changes in double helices of the starch in the fries were char­
scanning microscope (CLSM, TCS SP8, Leica, Germany) according to Bai acterized using a DSC (DSC 250, TA instruments Waters Inc., America)

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Y. Li et al. International Journal of Biological Macromolecules 236 (2023) 124042

a 70 b SO PSO STO TO
a
Water content 40 a ab
60 a a
a a b
30 b
b
Water content (%)

50 b

Oil Content (%)


b
c
20 c
40 d
a
30 6
5 b
4 b
20 bc
3
10 2 c
a a a a a
1
0 0
Control SA0.5 SA1.0 SA1.5 SA2.0 Control SA0.5 SA1.0 SA1.5 SA2.0
c 110 d 40
SO PSO STO
a ab ab
ab b
Oil fraction percentage (%)

100 35

Oil Content (%)


y= -0.8822x + 76.2664
90 30 Pearson's r= -0.7086
a
20 b b 25
b
b
10 20
abc a ab
c bc
0 15
Control SA0.5 SA1.0 SA1.5 SA2.0 44 46 48 50 52 54 56 58 60 62
Water content (%)

Fig. 2. Effect of sodium alginate coatings on the water content (a), oil content (b), oil fraction percentage (c) and the correlation between water and oil content (d) of
French fries.
SA0.5, SA1.0, SA1.5, SA2.0 indicates the fried potato strips with 0.5 g/100 g, 1.0 g/100 g, 1.5 g/100 g, 2.0 g/100 g SA coatings. The results are expressed as the mean
± standard error. Different lower-case letters (a-d) denote significant differences within different samples (P < 0.05).

according to the methods of Gao et al. [24]. The changes in the microstructure of SA films are related to inter­
molecular interactions in the film solution [15]. Hydrogen bonds be­
tween SA molecules and hydration between SA-H2O are formed less at
2.14. Statistical analysis the early stage (Fig. 1a). Then, a dynamic equilibrium between these two
interactions is obtained in the 1 % SA solution, which allows the
All experiments in this study were conducted at least three times, and hydrogen bonds between the SA chains to arrange regularly, improving
the results were presented as the mean values ± standard error by using the compactness of the film structure. However, the excessive addition
the Statistix 8.1 software (Analytical Software, St. Paul, MN, USA). of SA induces more interaction between SA molecules than between SA
Graphs were generated by using Origin 8.5, and the significance level and H2O, resulting in a random agglomeration of the SA molecular
was set to P < 0.05. chains and, thus, the formation of a coarse and loose structure.

3. Results and discussion 3.1.2. Water contact angle


The water contact angle (WCA) is an essential parameter to measure
3.1. SA films' properties the surface hydrophilicity of films. A hydrophilic coating material is
preferable for fried food rather than a hydrophobic one because it can
The effectiveness of edible coatings in oil reduction in fried food form an effective barrier and thus inhibit the escape of water vapor [11].
depends on the film-forming properties such as thickness, mechanical The WCAs of all films were below 90◦ , which indicates that the SA
properties, barrier properties, and microstructure. coatings are hydrophilic (Fig. 1c). With an increase in SA concentration,
the WCAs of the films decreased significantly and then gradually
3.1.1. Cross-section microstructure increased. The minimum value was obtained in SAF-1.0. The results can
The edible coating can create a three-dimensional network structure be explained by the fact that the increased SA-SA interaction led to the
on the food surface and change its properties, so it is vital to observe the formation of high-molecular-weight aggregation, partially burying hy­
microstructure of the films [11]. Fig. 1b shows the cross-section drophilic groups [18].
microstructure of SA films. It is intuitive that the film thickness gradu­
ally increases with the increasing SA concentration. In the case of SAF- 3.1.3. Viscosity and thickness
0.5, some fractures and cracks were observed on the films. Meanwhile, The changes in viscosity and thickness of SA coatings with increasing
the surface was uneven. SAF-1.0 had a homogeneous and smooth cross- concentration are shown in Fig. 1d. The viscosity and thickness grow
section without structural defects. In the SAF-1.5 and SAF-2.0 cross- with increasing SA concentration (P < 0.05), which corresponds well
sections, there were faults and more cracks.

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Y. Li et al. International Journal of Biological Macromolecules 236 (2023) 124042

Fig. 3. Effect of sodium alginate coatings on the color (a, b), texture (c, d), sensory evaluation (e) and appearance (f) of French fries.
The results are expressed as the mean ± standard error. Different letters (a-e) in the same column indicate statistically significant differences (P < 0.05).

with the results in Fig. 1b, mainly because of the increase in solid con­ increase in TS is an increased number of hydrogen bonds and aggregates
tent and SA swelling. between SA chains at higher SA concentrations, which reduces the dis­
tances between the molecular chains in the network structure of the SA
3.1.4. Mechanical and barrier properties films. Thus, more force is required to break the film under strain [25].
Mechanical and barrier properties are crucial parameters to evaluate Naeeji, Shahbazi, & Shavisir [26] also reported that the increasing TS of
the effectiveness of edible coatings in water retention and oil reduction the films is likely related to the presence of high intermolecular in­
[11]. The mechanical properties, including TS and EB, can be illustrated teractions between the polymers in the films. Besides, Comaposada,
by the maximum mechanical resistance and the ability to extend in the Gou, Marcos, & Arnau [27] reported that the maximum force in the
longitudinal direction in the tensile test. The changes in TS, EB, WVTR, tensile test of alginate films increases with thickness. This is also true for
and kit number of SA films with increasing SA concentration are dis­ the SA coating films in this study and possibly contributes to the
played in Fig. 1e and f. increased TS values (Fig. 1e). The improvement in EB is due to the
The TS, EB, WVTR, WVP, and kit number values increased with the increasing amount of SA, which causes more cracks and fractures in the
SA concentration increasing (P < 0.05). One possible reason for the microstructure of the films (Fig. 1b), thus, resulting in the ability to

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Y. Li et al. International Journal of Biological Macromolecules 236 (2023) 124042

Fig. 4. Correlation between the properties of SA coating films and the water content, oil content, quality of French fries.

extend of a film improved [28]. surface gets sucked into these pores during the cooling phase due to a
The increasing WVTR and WVP are ascribed to an increase in the free subsequent decrease in internal pressure. Therefore, it is assumed that
volume due to the random entanglement of the SA molecules [29,30], the reduction in PSO and STO was caused by the SA coating forming a
which contributed to water vapor penetrating the films, as already network structure on the fries' surface, which involved hydrogen
stated in the EB results and shown for the cross-section of the micro­ bonding between SA molecules and hydration between SA-H2O mole­
structure (Fig. 1e and b). The increased kit number was caused by the cules. This reduced the porosity of the fries due to the escape of water
longer channels of oil penetration, for which the increased thickness vapor, leading to less oil penetrating into the fries.
may be a reasonable explanation.
3.2.3. Oil fraction percentages
In both control and coated fries, the STO fraction constituted most of
3.2. Effects of SA coating on the oil absorption and quality of French fries
TO, followed by PSO and SO (Fig. 2c), indicating that the oil absorption
of French fries mainly occurred during the frying process through the
3.2.1. Moisture content
pathway left by the removal of water. However, Zhang, Xie, & Fan [31]
The moisture content of fried products is an important parameter
obtained different results, in which the PSO percentage relative to the
related to oil uptake, color, and texture during frying [3]. The moisture
TO content in fried chips was the highest, followed by PSO and SO. This
content of French fries coated with different SA concentrations is shown
may be explained by the condensation mechanism being mainly suitable
in Fig. 2a. The moisture content of SA-coated samples shows a signifi­
for frying processes with high initial moisture content and large frying
cant increase compared with the control samples (P < 0.05). Further­
samples [32].
more, all coated samples show no significant difference in moisture
content (P > 0.05).
3.2.4. Correlation analysis between the moisture and total oil contents
A strong negative correlation can be observed between the moisture
3.2.2. Oil content
and TO contents of the fries (Fig. 2d), which confirms that the water
The TO content comprises SO (the oil adhering to the sample sur­
replacement theory is valid for the frying process. Meanwhile, the SA
face), PSO (the oil penetrating the fried sample during cooling), and STO
coating prevented the oil from entering the fries by reducing moisture
(the oil penetrating the sample interior during frying). The variation in
loss. This led to higher moisture content, lower oil content, and more
TO content is associated with changes in the three oil fractions' contents
crispness, which are consumers' pursuits in fried food [3].
(Fig. 2b). The SA coating showed no noticeable effect on the SO (P >
0.05). The PSO and STO contents first decreased and then increased with
3.2.5. Color
growing SA concentration and, at 1 % SA, reached minima that were
The golden yellow appearance of fried products, corresponding to
significantly lower than in control samples (P < 0.05). The TO content
higher L*, b* and lower a*, is a key organoleptic attribute that attracts
presented a similar trend with PSO and STO, being dramatically reduced
consumers' attention [4,33]. Fig. 3a and b shows the L*, a*, b*, ΔE, and
by 52.5 % compared with the control samples, which indicates that the
BI values of all samples.
PSO and STO contents are the main contributors to TO.
The coated samples showed a higher L*; lower a*, b*, BI, and ΔE than
The formation of STO and PSO can be explained by water replace­
the control samples (P < 0.05), which indicates that the Maillard reac­
ment and condensation mechanisms [1]: the heat flux from the surface
tion of the fries reduced, resulting in the surface browning being
to the inner core of the samples made the moisture within boil and
inhibited. This was because that sugars and amino-group-containing
evaporated, which resulted in a loose and porous crust, allowing the oil
compounds were buried due to the steric hindrance of the SA network
to penetrate the steam passages. Afterward, the oil adhering to the food

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Y. Li et al. International Journal of Biological Macromolecules 236 (2023) 124042

Fig. 5. Effect of sodium alginate coating on the water and oil macroscope distribution (a), oil macroscope distribution (b), oil microscope distribution (c), and surface
microstructure (d) of French fries.

structure. However, highly retained moisture also contributed to this to represent the crust hardness, and overall hardness of fried samples,
result. Liu, Liu, Man, & Liu [34] reported a more noticeable reduction in respectively (Fig. 3c and d). The crust hardness and overall hardness of
the free asparagine content of bread with starch coating than without it, the SA-coated samples were significantly higher than those of the con­
which confirms our results. Notably, the increased L* and decreased b* trol ones (P < 0.05). The increase in crust hardness was attributed to the
values may be explained by the SA-coated fries retained the higher fact that SA coating reduces the pores and cracks on the surface and thus
moisture content, which increases the light reflection [35]. Further­ acts as a barrier. The increasing overall hardness is related to the higher
more, less oil accumulated over the surface (Fig. 2b), making the color moisture content in the 1 % SA-coated fries, inhibiting the volume
lighter than that of the control samples. shrinkage caused by starch gelatinization, resulting in higher flexibility
[36].
3.2.6. Texture
The crispy and tender texture is one of the attractive attributes of 3.2.7. Sensory evaluation
French fries for consumers. The maximum force and area under the The sensory evaluation of French fries is given in Fig. 3e. A signifi­
force-time curve were obtained from a puncture test of texture analysis cant difference was observed in color and crispness between the control

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Y. Li et al. International Journal of Biological Macromolecules 236 (2023) 124042

and SA-coated fries. In contrast, there was no significant difference in the yellow and red edge areas showed less oil than the control ones,
the other sensory attributes. Compared to the control fries, the crispness implying that the crust of fries coated with 1 % SA is rigid and smooth,
of the SA-coated fries increased, while the color scores decreased. which makes it difficult for oil to penetrate [36]. Moreover, the center
Although the decreasing b* values in the SA-coated fries affected the red area of the SA-coated fries diminished considerably compared with
color adversely (Fig. 3e and a), the overall impression showed no sig­ the control ones, demonstrating that the STO content of SA-coated fries
nificant difference among all samples. Thus, SA coating are able to decreased (Fig. 2b).
inhibit oil absorption of fried food while maintaining its quality.
3.4.3. Microscopical oil distribution
3.3. Correlation analysis between SA films' properties and their inhibitory The location and proportion of the red area in the unfried, control,
effect on oil absorption of French fries and SA-coated samples were observed using CLSM to illustrate the dif­
ferences in oil absorption behavior at the micro-level (Fig. 5c). It can be
The correlation between the SA films' properties and water content, noted that the honeycomb-like structure outlined in red lines is recog­
oil content, and the quality of French fries is displayed by the heatmap in nizable in the unfried sample, indicating that a small amount of free oil
Fig. 4. The redder the grid, the stronger the positive correlation, and the was located in the cell gaps. After frying, the red color occupied nearly
bluer the grid, the stronger the negative correlation. The WCA value of the whole region, indicating that the oil filled the cells, cracks, and pores
the films negatively correlated with the water content, Fmax, and Area, due to the destruction of cell structure by the rapidly dissipating steam.
and positively correlated with the PSO, STO, and TO content in the The images of the SA-coated fries had a smaller red area than the control
French fries. This result can be explained by that the simple observation fries, which was mainly concentrated in the enlarged intercellular
that the higher the WCA values, the more hydrophilic groups exist in SA spaces due to the contraction and deformation of the cells during frying
films. The hydrophilic groups in the films inhibit water evaporation [10,37]. This result indicates that the 1 % SA coating protects the cell
during frying, which reduces the oil penetration into fries, resulting in structure from being destroyed by steam and, consequently, prevents the
the PSO, STO, and TO content decreasing. The viscosity, EB, and WVTR oil from entering the starch granules. This outcome corresponds well
values were positively correlated with the PSO, STO, and TO content. with the oil content (Fig. 2b) and macroscopical oil distribution
The increased EB and WVTR of the films were attributed to the films (Fig. 5b).
being compact in proper concentration due to the hydrogen bonds be­
tween SA molecules closely arranging, which allows the oil to penetrate 3.4.4. Microstructure
the samples (Fig. 2a). The correlation between the L* and TS value was The microstructure plays a key role in explaining the pathway of oil
strongly negative, which is owed to the higher the TS, the rigidity the penetration and changes in samples' texture. The microstructure on the
film. This compact structure can effectively reduce non-enzymatic sample surface is displayed in Fig. 5d. There are more ruptures and pores
browning by shielding some reducing terminals on the surface of fries. on the surface of the fried samples compared with the compact surface of
the unfried sample, which makes the products crispy and oily. The cell
3.4. Mechanism of inhibiting French fries' oil absorption by SA coating walls collapsed because the starch granules were separated from the cell
walls during frying. The pores in the fries were caused by the escape of
3.4.1. Macroscopic water and oil distribution water vapor due to intensive heat transfer. The percentage of the pores'
The macroscopic water, oil content, and distribution can be reflected area to the total area in the SA-coated fries is significantly lower than in
by the proton density pseudo-color images of unfried, control, and SA- the control ones, resulting in a smoother and more compact crust due to
coated samples (Fig. 5a). The color range from blue, green, yellow, less water vapor escape. Thus, the coated fries had a hard texture (Fig. 3c
and red indicate the total content of increased water and oil. Large areas and d) and less PSO, STO, and TO contents (Fig. 2b). Yu et al. [10] re­
of green and yellow occur on the longitudinal section of the unfried ported that the surface microstructure of potato chips coated with guar
samples. After frying, the edge of the fries was uniformly distributed gum/glycerol appeared smoother than that of those without coating.
with green color, and the center area was almost red. The blue area
between the edge and the center indicates that the water in the outer 3.4.5. Water states
region entirely evaporated and that the oil entered the center of the fries The water in food is divided into bound water (T2b, 1–10 ms),
to form a moist core. In the coated samples, the blue area between the immobile water (T21, 10–100 ms), and free water (T22, 100-1000 ms).
edge and center of the fries was significantly reduced. Compared to the Furthermore, the shorter the T2 relaxation time, the more closely the
uncoated samples, the red and yellow areas of the coated fries' center fries' components are bound to water [38]. The water status and content
were more evenly distributed. This result shows that the rate of water are closely related to the oil uptake, color, and texture of the French
migration reduced, which causes more water to remain at the center of fries, which are reflected by the T2 relaxation time and peaks' ratio
the fries, confirming the water replacement theory. (Fig. 6a1, a2, and a3). Compared to unfried fries, the T2b, T21, and T22
relaxation times, and P2b and P21 of the control samples significantly
3.4.2. Macroscopical oil distribution increased, while the P22 value decreased (P < 0.05). After treatment
Fig. 5b shows the proton density pseudo-color images of the unfried, with SA, the T21, and T22 relaxation times and the P21 value of the
controlled, and coated samples, indicating changes in oil content and samples significantly decreased (P < 0.05), while the P2b value increased
macroscopical oil distribution in the longitudinal sections. The color (P < 0.05). In the uncoated samples, the mobility of the water molecules
changes in the order of blue, green, and yellow to red denote a gradual in the fries increased because of the intensive water evaporation, which
increase in oil content. destroyed the ordered starch structure. Further, lots of starch hydroxyl
In the unfried samples, the area of the edge layer exhibits an evenly groups were exposed, which increased the interaction between starch
distributed green color, stronger than the inner regions (blue color), and water [18]. However, in the coated fries, the coating acted as a
creating a distinct boundary between the crust and interior of the strips. diffusion barrier that blocked heat transfer, resulting in reduced water
After frying, the color of the outer layer in the control samples changed evaporation. More free water was bound by the starch gel structure
from green to yellow and red, and the color of the center changed from during frying, reducing the interaction between starch and oil.
blue to red, indicating that the structure of the fries was broken and
numerous pores and cracks were created, providing passages for oil 3.4.6. Solubility and swelling power
infiltration. Huang et al. [7] also found that oil was mainly concentrated The tightness of the starch structure can be characterized by the
in the crust at the early frying stage. However, the core showed more oil starch solubility and swelling power (Fig. 6b1). Compared to the unfried
than the crust with the prolonged frying time. In the SA-coated samples, samples, the starch solubility in the control samples increased, while the

8
Y. Li et al.
9

International Journal of Biological Macromolecules 236 (2023) 124042


Fig. 6. The LF-NMR relaxation times' distribution (a1), the T2 relaxation times (a2), and T2 relaxation population (T2 peak ratio) (a3) of French fries; the solubility, swelling power (b1), XRD pattern (b2), thermal
properties (b3), molecular structure (c) of starch in French fries.
Note: Unfried: the unfried potato strips; Control: the uncoated potato strips after frying; SA1.0: the 1 % SA coated fries after frying.
The results are expressed as the mean ± standard error. Different lower-case letters (a-d) denote significant differences within different samples (P < 0.05).
Y. Li et al. International Journal of Biological Macromolecules 236 (2023) 124042

Fig. 7. The inhibiting mechanism of sodium alginate coating on oil absorption of French fries.

10
Y. Li et al. International Journal of Biological Macromolecules 236 (2023) 124042

swelling power decreased, significantly (P < 0.05). The solubility and molecules and SA-H20 molecules is reached (1 % SA), which allows for
swelling power decreased significantly when the fries were coated with the SA molecules to be arranged orderly and densely. However, if the SA
SA (P < 0.05). The changes in solubility and swelling power indicate concentration increases to >1 %, the hydrogen bonds between SA
that the starch structure in the control samples became loose [39], molecules are supersaturated, which leads to free SA molecules being
which increases the binding sites of the starch and water molecules, entangled and agglomerated. The more dense and hydrophilic the
resulting in an increased starch dissolution. Meanwhile, this loose coating is, the more effectively it inhibits water migration and oil up­
structure provides space for oil penetration and inhibits the expansion of take. The water content negatively correlates with the oil content, which
the starch. When the fries were coated with SA, the compactness of the confirms the water replacement mechanism in the frying process: the
fries' structure was due to the reduction of water evaporation, which temperature of the frying medium was transferred from the crust to the
decreases the binding of starch and water, and the pathway for oil center of the fries during frying, which causes the water evaporation to
penetration. move inward. In the control samples, the amorphous region of the starch
swelled; and even deprived starch chains of the crystalline region, which
3.4.7. Starch structure destroyed the double helices of amylopectin, leading to the formation of
Starch structures are composed of concentric alternating amorphous a left-handed single helical structure. This structure formed a helical
and semi-crystalline growth rings. The crystalline region is formed by cavity that lipids could enter by hydrophobic. Thus, the crystalline
aggregated double helices of amylopectin side chains. The amorphous structure became loose, resulting in an increased oil penetration.
region comprises branch points of amylopectin and a disordered In the SA-coated fries, the double helices of the starch increased;
arrangement of amylose [40]. meanwhile, the crystalline structure and growth ring became more
complete compared to the uncoated samples. This was attributed to the
3.4.7.1. Crystalline region. The starch crystalline region and relative SA coating hindering the heat and water transfer, hence reducing the
crystallinity of French fries were characterized by the peak position and spaces for oil penetration.
area in X-ray diffraction patterns (Fig. 6b2). There are four diffraction
peaks (2θ = 5.8, 17.3, 21.8, and 24.2◦ ) in the unfried samples [41]. In 4. Conclusions
the control fries, the diffraction peak at 2θ = 5.8◦ disappeared, and the
diffraction peak's intensity at 2θ = 17.3, 21.8, and 24.2◦ decreased. SA coating showed the ability to reduce French fries' water evapo­
Meanwhile, the relative crystallinity significantly decreased by 22.9 % ration and oil uptake. The inhibitive efficiency of the 1 % SA coating was
(P < 0.05). Compared to the control samples, the intensity of the peaks the most significant. Compared to the control fries, the L*, crispness of
at 2θ = 5.8 and 17.3◦ increased, and the relative crystallinity of the SA- the SA-coated samples improved, while b* and a* decreased, signifi­
coated samples increased by 30.2 %. The results indicate that the crys­ cantly (P < 0.05). A correlation analysis revealed that the film hydro­
talline region of the starch in the control samples was severely destroyed philicity positively correlates with the PSO, STO, and TO content and
because the amorphous regions swelled with water and even stripped negatively correlates with the Fmax and Area of the fries. Compared to
starch chains from the crystalline region [37]. However, in the SA- the control samples, water evaporation in SA-coated fries reduced and
coated samples, the ordered structure of the crystalline regions more water was locked in the starch gel network, which was confirmed
increased. This phenomenon could be explained by the fact that the SA by LF-NMR. In terms of starch, the crystalline structure and double he­
coating hinders the transfer of energy from the frying medium to the lices increased, reducing the water migration and oil penetration. MRI,
interior of the fries, thus reducing the pressure of water vapor on the CLSM, and SEM results indicate that the edible coatings formed a barrier
fries' tissue and improving their preservation. This compact structure on the fries' surface by changing surface structure, which reduces the
impeded the oil penetration into crystalline regions. formation of water vapor channels, leading to an altered oil absorptive
pathway and distribution. This study found that the main mechanism of
3.4.7.2. Double helix structure. The gelatinization temperature (T0, Tp, oil absorption in French fries is water replacement and confirmed that
Tc) and enthalpies (ΔH) of unfried, control, and SA-coated fries obtained SA coating effectively inhibits water migration and oil uptake in fries. In
from DSC curves are presented in Fig. 6b3, which can reflect the stability summary, this study developed an economical and effective coating
of double helices (Fig. 6c). The T0, Tp, Tc, and ΔH values of the unfried (estimated unit cost = 0.11CNY/Kg of French fries) that provides a
samples were 53.3, 60.0, 77.3 ◦ C and 2.7 J/g, respectively. After frying, theoretical basis for the industrial application of low-fat fried foods.
there was no endothermic peak in the control fries, while the peak
reappeared in the SA-coated fries, and the T0, Tp, Tc and ΔH values were CRediT authorship contribution statement
52.8, 60.3, 76.9 ◦ C, and 2.0 J/g, respectively.
The changes in gelatinization temperature and ΔH indicated that the Ying Li: Methodology, Software, Validation, Formal analysis,
double helices of amylopectin in control samples were destroyed and Investigation, Writing – original draft. Xue Bai: Investigation. Mengna
transformed into single left-hand helices, which formed a helical cavity. Zhao: Conceptualization, Resources. Hui Wang: Investigation. Jia
Consequently, the hydrophobic lipids could easily enter the starch helix Feng: Investigation. Xiufang Xia: Conceptualization, Supervision,
cavity to form a starch single helix-lipid complex [42] (Fig. 6c). How­ Formal analysis, Funding acquisition. Qian Liu: Formal analysis,
ever, the endothermic peak that appeared in the coated French fries Investigation.
indicates that the SA coating inhibited moisture migration. Hence, the
starch swelled, which increased the hydrogen bonds between starch Declaration of competing interest
molecules [43], resulting in the lipid being unable to enter the helical
cavity. The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
3.4.8. Schematic mechanism of oil reduction the work reported in this paper.
The inhibitory mechanism of SA coating on the oil uptake of fries
based on the exchange theory of water and oil is exhibited in Fig. 7. The Acknowledgments
inhibitory effect of SA coating on oil uptake is closely related to its
surface microstructure and hydrophilicity. If the SA concentration is This study was supported by the National Natural Science Founda­
lower than 1 %, the SA molecules are loosely arranged and disordered. tion of China (Grant No. 32172273).
As SA concentration increases, a dynamic equilibrium between SA

11
Y. Li et al. International Journal of Biological Macromolecules 236 (2023) 124042

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