Food Control 101 (2019) 121–125

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Food Control
journal homepage: www.elsevier.com/locate/foodcont

Geographical origin authentication of onions using stable isotope ratio and T

compositions of C, H, O, N, and S
Jin Hee Parka, Seung-Hyun Choib,c, Yeon-Sik Bongc,∗
a
School of Environmental and Biological Chemistry, Chungbuk National University, Cheongju, 28644, Republic of Korea
b
Graduate of Analytical Science and Technology, Chungnam National University, Daejeon, 31434, Republic of Korea
c
Division of Earth and Environmental Sciences, Korea Basic Science Institute, Cheongju, 28119, Republic of Korea

A R T I C LE I N FO A B S T R A C T

Keywords: Both stable isotope ratio and content of carbon (C), hydrogen (H), oxygen (O), nitrogen (N), and sulfur (S) were
Onion employed to evaluate the possibility of geographical origin discrimination for onions grown in different regions
Stable isotope in Korea. Significantly different elemental compositions were found in H, N, and S compositions, which might be
Discriminant analysis related to different agricultural practices. The stable isotope ratio of C, H, O, N, and S was significantly different
Geographical origin
among classified regional groups. A linear discriminant analysis relatively well discriminated onions produced
Elemental composition
from different regional groups based on stable isotope and elemental composition data. Better discrimination of
geographical origin of onions was achieved by combining groups located at similar latitude. Inclusion of the ratio
of elemental compositions such as H/C and C/N improved the discriminative power for determining geo-
graphical origin of onions. Further distinct geographical differentiation of onion origin can be achieved by
additional multi-elemental analysis.

1. Introduction
Identifying the geographical origin of agricultural products is im-
portant because of the globalization of food markets along with the
increasing demand for food safety and high quality (Chung et al.,
2016). Determination of geographical origin of agricultural products
not only protects consumers and producers from fraud; it also helps
preserve economic gain. Various analytical techniques have been used
for the authentication of geographical origin, which include instru-
mental techniques such as high performance liquid chromatography
(HPLC) and nuclear magnetic resonance (NMR), trace element analysis,
stable isotope, and recently genomics, proteomics, and metabolomics
(Consonni & Cagliani, 2010; Fernández-Cáceres, Martin, Pablos, &
González, 2001; Ortea, O'Connor, & Maquet, 2016; Ouni et al., 2011).
Among the various techniques for provenance determination, stable
isotope data have been successfully used to identify food sources or
origins by applying statistical analyses for data interpretation (Oulhote,
Le Bot, Deguen, & Glorennec, 2011). Stable isotopes refer to the same
elements with different mass and isotope ratio mass spectrometry
provides the isotope ratios. Stable isotopes are grouped by atomic mass.
Light stable isotopes are bio-elements such as 2H/1H, 13C/12C, 18O/16O,
15
N/14N, and 34S/32S while heavy isotopes are 87Sr/86Sr, 206Pb/204Pb,
207
Pb/204Pb, 208Pb/204Pb, and 143Nd/144Nd (Danezis, Tsagkaris, Camin,
Brusic, & Georgiou, 2016). Because the isotope ratio of C, H, O, N, S and
Sr is affected by evaporation, condensation, precipitation, plant species,
agricultural practice, age of rock, and bacterial action, stable isotope
ratio was shown to be a useful tool for determining the geographical
origin of agricultural products (Kelly, Heaton, & Hoogewerff, 2005).
Stable isotope ratio analysis has been employed in geographical origin
authentication of food, especially honey and cereal grains. Adulteration
of commercial honey was identified by elemental analyzer and liquid
chromatography coupled to isotope ratio mass spectroscopy (Dong
et al., 2016, 2018). Geographical origin of wheat and rice was dis-
criminated by stable isotope ratio analysis of carbon and nitrogen (Luo
et al., 2015; Wu et al., 2015).
Stable isotope data combined with elemental composition and a
multi-elemental approach provide better discrimination for geo-
graphical origin (Bong, Gautam, La, & Lee, 2012; Rummel, Hoelzl,
Horn, Rossmann, & Schlicht, 2010). Photosynthetic metabolism of
plants is reflected in carbon ratio and environmental conditions affect O
and H stable isotope ratios (Martinez et al., 2003). Nitrogen and C
isotope ratios are related to the climate and agricultural practices and S
isotope ratio is an indicator of geology, distance from the sea and an-
thropogenic effects (Denizis et al., 2016). Suzuki, Chikaraishi, Ogawa,
Ohkouchi, and Korenaga (2008) reported that C and N content together
with δ13C, δ15N, and δ18O distinguished the geographical origin of rice

∗
Corresponding author.
E-mail address: bong_geo@kbsi.re.kr (Y.-S. Bong).

https://doi.org/10.1016/j.foodcont.2019.02.023
Received 11 September 2018; Received in revised form 30 January 2019; Accepted 19 February 2019
Available online 23 February 2019
0956-7135/ © 2019 Published by Elsevier Ltd.
J.H. Park, et al.
using a pentagonal radar plot. Zhang, Pan, and Zhu (2012) were also
able to cluster Chinese teas from different provinces using C and N
stable isotope ratios. In this study, stable isotope data were combined
with C, H, O, N, and S compositions and their ratios to improve dis-
criminative power.
One of the characteristics of the Korean diet is the high consumption
of herbs such as garlic, onion, red pepper, and ginger (Kim et al., 2016).
Onions are one of the most popular vegetables in the world, and agri-
cultural products that are often subject to dubious sales mechanisms.
Therefore, onions were selected as the target agricultural product for
discriminating geological origin in this study. The objective of the study
is to evaluate the possibility of geographical origin discrimination for
onions grown in different regions in Korea based on stable isotope data
combined with elemental composition.
2. Materials and methods
2.1. Onion collection and preparation
Onion samples were harvested from six different provinces in Korea.
The samples from six different provinces were organized into four dif-
ferent groups according to latitude and longitude (Fig. 1). The average
latitude and longitude values for Group 1, Group 2, Group 3, and Group
4 samples were 37°13′ and 128°55′, 37°33′ and 127°81′, 35°72′ and
128°24′, and 34°86′ and 126°47’, respectively. The collected onion
samples were washed several times with distilled water. The outermost
tunic layer was removed, and the outer layer of the edible onion portion
was used for analysis. The onion sample was chopped with a ceramic
knife and dried in a freeze-dryer (FDU-2100, EYELA, Japan). The dried
sample was pulverized using a mixer mill (MM 400, Retsch, Haan,
Germany) and stored in a vacuum oven (OV-12, JEIO TECH, South
Korea) until analysis.
2.2. Stable isotope analysis
Ten mg of onion sample was enclosed in a tin capsule for the C, N,
and S stable isotope ratios. Carbon, N, and S isotopes were measured
using an isotope-ratio mass spectrometer (IRMS, Isoprime VisION,
Fig. 1. Geographical locations and groups of onion sampling sites.
122
Food Control 101 (2019) 121–125
Isoprime Ltd., Stockport, U.K.) at the Korea Basic Science Institute. The
carbon, N, and S composition was simultaneously analyzed using an
elemental analyzer (vario PYRO cube, Elementar Analysen system
GmbH, Hanau, Germany) coupled to the IRMS. The sample was com-
busted at 1150 °C in a combustion reactor, and the reduction of gases
occurred at 850 °C reduction reactor. Helium carrier gas was set to
220 mL/min. Carbon and N isotope data were calibrated against USGS-
40, IAEA-600, and urea (in-house standard, δ13C = −8.02‰,
δ15N = +20.17‰) and sulfur isotope data were calibrated to NBS-127,
IAEA-SO-5, BaSO4 (in-house standard, δ34S = +5.82‰). For O and H
isotope analysis, a 0.3 mg sample was enclosed in a silver capsule and
analyzed using an IRMS (Delta V advantage, Thermo Scientific,
Bremen, Germany) coupled to an elemental analyzer (TC/EA, Flash
2000HT, Thermo Scientific, Bremen, Germany). For H isotope analysis,
encapsulated samples in a silver capsule were placed in a desiccator
together with reference material for longer than 72 h to adjust atmo-
spheric effect. For O and H isotope analysis, the data were calibrated to
IAEA-601, IAEA-602, USGS-56, and IAEA-CH-7, USGS-56, and USGS-
42, respectively. The sample for the O and H isotope was analyzed in a
1400 °C combustion tube and 90 °C column oven. Helium purging
equipment (NoBlank, MAS200R, Thermo Scientific, Bremen, Germany)
was used to minimize atmospheric effect during sample injection.
2.3. Statistical analysis
The XLSTAT-Pro statistical package (Addinsoft, New York, USA)
was used to analyze the elemental composition and isotope data sets of
C, H, O, N, and S from the onion samples of four different groups at 5%
significance level. The number of onion samples for the analysis was
130 (nGroup 1 = 27, nGroup 2 = 23, nGroup 3 = 47, nGroup 4 = 33). Before
analysis, the variables were standardized to rescale the dataset. One-
way analysis of variance (ANOVA) was used to compare the elemental
composition and isotope data among the groups. The differences be-
tween the individual mean values were further analyzed by Tukey's
post hoc test. Principal component analysis (PCA) was employed to
evaluate the relationship between variables used using SPSS software
(IBM Analytics, Chicago, USA). PCA is a statistical procedure to convert
correlated multivariate datasets into uncorrelated principal compo-
nents (Granato et al., 2018). Linear discriminant analysis (LDA) was
conducted to evaluate whether the onion samples from one group can
be discriminated from the other groups based on the elemental com-
position and ratio as well as isotopic data. LDA is a classification
techniques using maximum likelihood discriminant principal and pro-
vides visualized classification results (Granato et al., 2018). For PCA
and LDA, 13 variables (C, N, S, O, H, C/N, H/C, O/C, δ15N, δ13C, δ34S,
δ18O, and δ2H) were used.
3. Results and discussion
3.1. Variation of elemental composition and stable isotope of onions
depending on geographical region
The comparison of elemental composition in onions showed that C
and O composition was not much different between the regional
groups. Hydrogen (p < 0.05), N (p < 0.0001), and S (p < 0.0001)
composition was significantly different (Table 1). Hydrogen, N, and S
composition was the highest in the onion samples from Groups 1 and 2,
which were located at a relatively high latitude in Korea
(Supplementary Fig. 1). The higher N and S composition might be re-
lated to fertilizer application. The average amount of ammonium sul-
fate applied per arable land in Korea in 2017 was 6.82, 5.94, 5.26, and
5.54 kg/ha for Groups 1, 2, 3, and 4, respectively (MAFRA & Ministry of
Agriculture, 2017). Nasreen, Haque, Hossain, and Farid (2007) re-
ported that N and S uptake by onion bulb increased with N and S fer-
tilizer application.
The hydrogen composition of Groups 1 and 2 varied greatly
J.H. Park, et al. Food Control 101 (2019) 121–125

Table 1
Comparison of C, H, O, N, and S composition, atomic ratio, and stable isotope ratio.
Elements Group 1 (n = 27) Group 2 (n = 23) Group 3 (n = 47) Group 4 (n = 33)

C% 38.53 ± 0.48a 38.56 ± 0.74a 38.93 ± 1.20a 38.65 ± 1.03a

H% 6.22 ± 1.95a 5.94 ± 1.69 ab 5.70 ± 1.27 ab 5.17 ± 0.74b
O% 52.90 ± 2.83a 53.67 ± 2.79a 52.27 ± 7.11a 54.07 ± 3.73a
N% 1.35 ± 0.22a 1.41 ± 0.28a 1.06 ± 0.31b 0.91 ± 0.34b
S% 0.38 ± 0.08a 0.39 ± 0.10a 0.32 ± 0.08b 0.27 ± 0.07b
C/N 34.27 ± 5.61b 33.32 ± 7.13b 47.22 ± 16.21a 54.95 ± 15.97a
H/C 1.92 ± 0.60a 1.83 ± 0.49 ab 1.74 ± 0.39 ab 1.59 ± 0.21b
O/C 1.03 ± 0.06a 1.05 ± 0.07a 1.01 ± 0.14a 1.05 ± 0.08a
δ13CVPDB (‰) −25.79 ± 1.10 ab −26.52 ± 1.06c −25.42 ± 0.75a −26.13 ± 1.07bc
δ2HVSMOW (‰) −49.42 ± 6.33 ab −51.92 ± 8.22 ab −48.93 ± 6.24a −53.01 ± 5.67b
δ18OVSMOW (‰) 26.39 ± 1.45bc 26.02 ± 1.60c 27.90 ± 1.28a 27.14 ± 1.40 ab
δ15NAIR (‰) 2.38 ± 1.88c 5.18 ± 4.60b 7.94 ± 4.43a 1.69 ± 2.52c
δ34SCDT (‰) −1.06 ± 2.63b −0.60 ± 3.85 ab −0.80 ± 2.21b 0.86 ± 2.28a

Data represent the mean ± standard deviation. Different letter values indicate significant difference among groups (p < 0.05).

(Supplementary Fig. 1). The higher hydrogen composition of Group 1 can be useful for the geographical origin discrimination of onions. The
led to the higher H/C ratio, which indicated less aliphatic properties of highest δ34S value was found in the Group 4 samples, which were lo-
the onions belonging to Group 1 (Pujol et al., 2013). The H/C ratio also cated close to the sea and might be affected by ocean sulfate (Table 1).
could be related to the high amount of phenolic compounds, which
constitute variation in the antioxidant pool among the different types of 3.2. Determination of geographical origin by statistical analysis
onions (Lu et al., 2011). Highly unsaturated and phenolic compounds
have an H/C ratio of less than 1.5, aliphatic compounds have an H/C The five principal components with an Eigen value higher than 1
ratio between 1.5 and 2.0, and carbohydrate O/C ratio is between 0.67 accounted for 77.5% of the total variance of the data. PC1 explained
and 1.2 with H/C between 1.5 and 2 (Li et al., 2018). A high O/C ratio 24.4% of total variance, and PC2 explained 19.9% of total variance
indicates high polarity and higher COOH content in organic carbon (Table 2). Therefore, clear discrimination of the onions according to
(Hunt, Parry, & Hamilton‐Taylor, 2000). groups was not found in the score plots of PC1 and PC2 (Data not
The C/N ratio is used as a useful tool for evaluation of N limitation shown). PC1 was governed by N, S, C/N ratio, and δ18O compositions of
of plants and land sources. A low C/N ratio is beneficial to vegetative onions, while PC2 was influenced by O, H, and H/C ratio and O/C ratio.
development, while high C/N ratio favors regenerative development of PC3 has high loadings for δ2H, and PC4 was affected mainly by δ13C.
horticultural plants. The C/N ratio can be varied according to horti- PC5 showed the highest loading for δ34S.
cultural practices and growth stage development of onions can be de- Because the sample origin could not be clearly discriminated by
termined by the C/N ratio. Onion flowering is inhibited by pruning, PCA, LDA was employed to maximize the covariance among the groups.
which results in a low C/N ratio (Sanders & Cure, 1996). Nitrogen Initially, LDA was conducted with elemental composition and isotope
fertilizer application also decreases the C/N ratio of onions because it ratio of C, H, O, N, and S. LDA with elemental composition and isotope
increases the N content in onions (Díaz-Pérez, Purvis, & Paulk, 2003). ratio correctly classified only 66.7% of onion samples (60.3% after
The δ13C values vary depending on plant species. The δ13C value of cross-validation). Therefore, elemental ratios such as C/N, H/C, and O/
a C3 plant is −27.1 ± 2.0‰, while the δ13C value of a C4 plant is C were included in the LDA as variables. LDA with all variables cor-
−13.1 ± 1.2‰ (O'Leary, 1988). Because onions belong to a C3 plant, rectly classified 74.6% of the onion samples (63.6% after cross-vali-
the δ13C average values of onions ranged from −26.5 to −25.4‰. dation). Rao's approximation showed Wilk's lambda value of 0.199 at
Plant growth conditions also affect the δ13C value, and increasing p < 0.0001. According to the LDA results, the two discriminant axes
temperature and decreasing light intensity resulted in a more negative explained 84% of total variance. The scatter plot of the first two
δ13C value in a C3 plant (Hughes, Kelly, Pilcher, & LaMarche, 1982).
The δ15N was significantly different among samples from different Table 2
groups (Table 1 and Supplementary Fig. 1). Normally, δ15N values of Principal component loadings and total cumulative variance explained by the
photoautotrophs range from −9 to 10‰, being significantly affected by first five principal components. The bold number indicates loading > 0.5.
chemically synthesized fertilizers with δ15N ranging from −6 to 7‰
Principal components
(Ohkouchi, Ogawa, Chikaraishi, Tanaka, & Wada, 2015). The lowest
δ2H value was found in the Group 4 samples. Heaton, Kelly, 1 2 3 4 5
Hoogewerff, and Woolfe (2008) showed that the δ2H and δ18O value
related to the latitude of beef production regions, which was also re- C% −0.090 0.328 0.130 −0.243 0.343
N% 0.924 0.024 0.228 −0.081 0.097
lated to the H and O isotope content of precipitation. Samples from the S% 0.846 0.079 0.067 −0.091 0.059
Group 3 and 4 regions, which were located at a relatively lower lati- O% 0.124 −0.775 −0.260 0.448 0.090
tude, showed higher δ18O values. The 18O/16O ratio is also known to be H% 0.207 0.701 −0.593 0.306 0.062
highly dependent on the distance to the sea and on the altitude above C/N −0.922 0.049 −0.208 −0.010 −0.047
H/C 0.215 0.670 −0.612 0.339 0.027
sea level of the production site (Luykx & Van Ruth, 2008).
O/C 0.132 −0.810 −0.284 0.487 −0.009
The δ34S value can be used to improve the discriminative power of δ15N −0.156 0.332 0.281 0.408 0.323
the geographical origin identification (Luykx & Van Ruth, 2008). δ13C 0.027 0.359 0.392 0.525 −0.403
Sources of S for plants supplied from soil sulfate and atmospheric SO2 δ34S −0.339 −0.065 0.116 0.165 0.787
and ocean S affect soil sulfate as sea spray spreading up to 100 km. δ18O −0.649 0.163 0.348 0.214 −0.203
δ2H 0.260 0.100 0.674 0.421 0.060
Sulfate reduction by plants results in the synthesis of organic S, such as
S containing amino acids and vitamins as well as coenzymes (Krivachy, Eigen value 3.178 2.592 1.812 1.412 1.077
Rossmann, & Schmidt, 2015). Although the S content of most plants is Variability (%) 24.4 19.9 13.9 10.8 8.3
less than 1%, the S content of Brassicaceae and Allium sp. is higher and Cumulative (%) 24.4 44.4 58.3 69.2 77.5

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J.H. Park, et al. Food Control 101 (2019) 121–125

Fig. 2. Linear discriminant scatter plot of the first two discriminant functions
for onion samples from four groups.
discriminant functions acquired from LDA with all variables tended to
discriminate onions according to the four different groups (Fig. 2). LDA
with variables except for O/C ratio showed better cross-validation with
65.8% accuracy, although the correct classification for original grouped
cases (73.5%) was lower than LDA with all variables. The result showed
that 55.6%, 65.2%, 69.6%, and 72.7% of the Group 1, 2, 3, and 4
samples were classified correctly for cross-validated group cases
(Table 3).
Group 1 and Group 2 samples showed some boundary overlapping
(Fig. 2). Among the samples belonging to Group 1, 18.5% was classified
as Group 2, and 17.4% of Group 2 samples was classified as Group 1
samples, indicating that Group 1 and 2 samples have similar elemental
and isotopic compositions. Because the Group 1 and 2 sampling loca-
tions are in relatively close proximity to each other, these groups were
not clearly classified according to LDA. Close proximity results in small
climatic differences between Group 1 and 2 and similar latitude
(average latitude of sampling locations of 37°13′ and 1 37°33′ for
Groups 1 and 2, respectively), which do not have marked differences
among onions in these groups. A better classification of geographical
origin of onion samples was achieved with an overall correct rate of
77.7% and 74.9% for original and cross-validation, respectively, when
Group 1 and 2 samples were combined. The LDA with three groups
correctly classified 71.4% of Group 1 and 2 samples, 74.5% of Group 3
samples, and 74.9% of Group 4 samples. Stepwise LDA selected five
variables with Wilk's lambda of 0.285 at p < 0.0001, which are H%,
δ15N, δ13C, δ34S, and C/N ratio. The result indicates that H%, δ15N,
δ13C, δ34S, and C/N ratio were the important variables for the dis-
crimination of onion samples.
Natural abundance isotope ratios were used for provenance de-
terminations. Carbon and N isotope ratios provide information on plant
or diet type, while H, O, and S isotope ratios provide information on
geographical proxy (Kelly et al., 2005). Nitrogen isotope ratio is mainly
affected by the trophic level and agricultural practice, and S isotope
ratio provides supplementary information on regional agricultural
practices (Kelly et al., 2005). Additional information on elemental
compositions and their ratios provide better discrimination of onion
samples. Suzuki et al. (2008) also showed that the companion of C and
N compositions and the δ13C, δ15N, and δ18O ratio of polished rice were
useful in the discrimination of the geographical origin of polished rice.
Although the overall 77.7% of correct rate for geographical dis-
crimination of onions was achieved, correct discrimination rate is re-
latively low and geographical traceability needs to be improved. Multi-
elemental (25 trace elements) fingerprinting of Tropea red onion
showed that 94% of Tropea red onion was correctly categorized by LDA
(Furia, Naccarato, Sindona, Stabile, & Tagarelli, 2011). They compared
onions with the protected geographical certification (Tropea red onion)
and other onions (non-Tropea onion) from other Italian regions and The
Netherlands. Relatively better classification of the onion origin was
achieved compared to this study because the Tropea red onion was
cultivated following the production regulations. Multi-elemental (25
elements) fingerprinting also was able to authenticate organically
grown winter wheat, spring barley, faba bean, and potato (Laursen
et al., 2011). Geographical origin of Chinese green tea was well dis-
criminated by Fourier transform near-infrared spectroscopy with 100%
discrimination rates (Chen, Zhao, & Lin, 2009). Therefore, combination
of isotope ratio and other analytical methods can improve prediction
ability of geographical authentication. Multi-element analysis coupled
with strontium isotope ratio correctly classified the geographical origin
of Chinese cabbage (Bong et al., 2013). The combined technique of Sr
and Pb isotope ratios and multi-element concentrations by inductively
coupled plasma mass spectrometry identified country of rice origin in
Japanese market with 97% accuracy (Ariyama, Shinozaki, & Kawasaki,
2012).
Inclusion of elemental ratios for geographical origin determination
was first adapted in this study. The study showed that combination of
isotopic composition with elemental ratios led to the better classifica-
tion of geographical origin of onions rather than only adding elemental
compositions. Most of other geographical discrimination studies were
conducted on agricultural products from different countries to identify
country of origin. Although onions sampled in this study were not
significantly different in cultivation practices, climate and environ-
mental conditions because of close proximity of sampling sites within
Korea, the proposed method provided good discriminating power.
Therefore, stable isotope ratio analysis of C, H, O, N, and S coupled with
their compositions and ratios is suggested as a simple and rapid method
for discriminating geographical origin to prevent fraud in food market.
Further studies on multi-element isotope composition and trace element
concentrations of onions from other countries are also required to

Table 3
Confusion matrix for original and cross-validated classification by discriminant analysis with different variables.
Variables Elemental composition and Elemental composition and isotope Elemental composition and isotope Elemental composition and isotope data, C/
included isotope data data, C/N, and H/C ratio data, C/N, H/C and O/C ratio N, and H/C ratio, 3 groups

% correct Original Cross validated Original Cross validated Original Cross validated Original Cross validated

Group 1 55.56% 51.85% 70.37% 55.56% 70.37% 62.96% 75.51% 71.43%

Group 2 60.87% 43.48% 73.91% 65.22% 78.26% 52.17%
Group 3 74.47% 70.21% 73.91% 69.57% 73.91% 69.57% 78.72% 74.47%
Group 4 75.76% 75.76% 75.76% 72.73% 75.76% 69.70% 78.79% 78.79%

Total 66.66% 60.33% 73.49% 65.77% 74.58% 63.60% 77.67% 74.89%

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J.H. Park, et al.
improve discriminating ability.
4. Conclusions
Stable isotope ratios of C, H, O, N, and S, coupled with their com-
positions and ratio were useful for the geographical discrimination of
onion samples. Inclusion of elemental ratios enhanced the dis-
criminating ability. However, the prediction ability of the method in
this study was not perfect because of small differences in growth en-
vironments within Korea. Mismatching between administrative divi-
sions and growth conditions determining geographical origins might
lead to limited discrimination of onions grown within the country. More
distinct geographical differentiation of onion origin can be achieved by
additional multi-elemental analysis. This technique, however, still has
high potential for discriminating onions produced in Korea from those
produced in other countries.
Acknowledgments
This work was supported by the Korea Institute of Planning and
Evaluation for Technology in Food, Agriculture, Forestry (IPET)
through the Advanced Production Technology Development Program
(Project Number: 316075-04), funded by the Ministry of Agriculture,
Food and Rural Affairs.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://
doi.org/10.1016/j.foodcont.2019.02.023.
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