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Food Additives & Contaminants: Part A
ISSN: 1944-0049 (Print) 1944-0057 (Online) Journal homepage: https://www.tandfonline.com/loi/tfac20
Analysis of mineral oil in food: results of a Belgian
market survey
Annelies Van Heyst, Mathias Vanlancker, Joeri Vercammen, Kathy Van den
Houwe, Birgit Mertens, Marc Elskens & Els Van Hoeck
To cite this article: Annelies Van Heyst, Mathias Vanlancker, Joeri Vercammen, Kathy Van den
Houwe, Birgit Mertens, Marc Elskens & Els Van Hoeck (2018) Analysis of mineral oil in food:
results of a Belgian market survey, Food Additives & Contaminants: Part A, 35:10, 2062-2075, DOI:
10.1080/19440049.2018.1512758
To link to this article: https://doi.org/10.1080/19440049.2018.1512758
Published online: 10 Sep 2018.
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Analysis of mineral oil in food: results of a Belgian market survey
Annelies Van Heyst a, Mathias Vanlanckerb, Joeri Vercammenb, Kathy Van den Houwea, Birgit Mertensc,
Marc Elskensd and Els Van Hoecka
aService Organic Contaminants and additives, Sciensano, Brussels, Belgium; bInterscience, Louvain-la-neuve, Belgium; cService Risk and
health impact assessment, Sciensano, Brussels, Belgium; dDepartment of analytical and geochemistry Vrije Universiteit Brussel, Brussels,
Belgium
ABSTRACT
Recently, migration of mineral oil components from food contact materials into various foods has
been reported. The analysis of mineral oil in food is complicated since it consists of mineral oil
saturated hydrocarbons (MOSH) comprising a complex mixture of linear, branched and cyclic
compounds and variable amounts of mineral oil aromatic hydrocarbons (MOAH), mainly alkylated. Both MOSH and MOAH form ‘humps’ of unresolved peaks in the chromatograms with the
same range of volatility. Since these two fractions have a different toxicological relevance, it is
important to quantify them separately. Occurrence data on mineral oil are available only for a
limited number of food groups and only from few countries. In Belgium, data on the contamination of food by mineral oil are lacking. In this contribution, an in-house validated online
combination of liquid chromatography with gas chromatography (LC–GC) with flame ionisation
detection (FID) was used for the quantification of MOSH and MOAH. Totally, 217 packed food
samples were selected using a well-defined sampling strategy that targeted food categories
which are highly consumed and categories suspected to contain mineral oil. For 19 samples, the
method was not applicable. For the 198 remaining samples, MOSH was detected in 142 samples
with concentrations up to 84.82 mg kg-1. For the MOAH fraction, there are 175 samples with a
concentration below the limits of quantification (LOQ), while 23 samples had a higher concentration ranging from 0.6 to 2.24 mg kg-1. Finally, these results were compared with the action
thresholds as proposed by the Scientific Committee (SciCom) of the Belgian Food Safety Agency
(FAVV-AFSCA). Only one sample exceeded the threshold for MOSH, while the threshold for MOAH
was exceeded in 23 samples. For the samples exceeding the action threshold, further investigation is needed to identify the contamination source.
ARTICLE HISTORY
Received 8 June 2018
Accepted 2 August 2018
KEYWORDS
Mineral oil; food contact
materials; market survey;
online LC-GC; action
thresholds
Introduction
In the last few years, migration of mineral oil
components from packaging materials into various foods has been reported (Vollmer et al.
2011; EFSA CONTAM Panel 2012; Foodwatch
2015). Mineral oils are extremely complex mixtures of hydrocarbons with varying carbon numbers and structures. Thus, individual analysis of all
the different components is not possible. Among
the many different substances present in mineral
oil, two main types can be distinguished: the saturated hydrocarbons (MOSH) and the aromatic
hydrocarbons (MOAH).
Mineral oil can enter the food via different
routes: (i) certain mineral oils are allowed as additives (e.g. E905a) (European Commission 2008),
(ii) as a pollutant from atmospheric precipitation
or aquatic pollution, (iii) due to processing of food
(e.g. use of machine oils and anti-dusting products) and (iv) as a residue coming from ingredients from pesticides, or components from printing
inks on paper and board packaging. Since recycled
paper and board was identified as a major source
of mineral oil contamination (Vollmer et al. 2011),
the market of cardboard packaging has evolved,
using different amounts of recycled fibres, or
using a functional barrier (e.g. an inner bag that
is impervious for these substances) to prevent
migration of mineral oil. However, the barrier
capacities of the inner bags currently used are
insufficient or even unknown (Vollmer et al.
2011). Other possible measures are to discontinue
the use of recycled fibres for food packaging. Yet,
CONTACT Annelies Van Heyst annelies.vanheyst@sciensano.be Service Organic Contaminants and additives, Sciensano, Rue Juliette
Wytsmanstraat 14 | 1050, Brussels, Belgium
FOOD ADDITIVES & CONTAMINANTS: PART A
2018, VOL. 35, NO. 10, 2062–2075
https://doi.org/10.1080/19440049.2018.1512758
© 2018 Taylor & Francis Group, LLC
this is in contradiction to the measures laid down
in EU Directive 94/26/EC to promote recycling of
food contact materials in the context of sustainability (European Commission 1994).
A question that immediately arises is if this
contamination of the food with mineral oil forms
a threat for public health. Unfortunately, it is not
possible to formulate an unambiguous answer to
that question because assessment of the risks associated with the consumption of food contaminated
with mineral oil is complicated by the lack of
exposure data, and also by the limited number of
adequate toxicological studies. However, all
mineral oils have been shown to be mutagenic
unless they are treated specifically to remove
MOAH (Mackerer et al. 2003). MOSH are not
carcinogenic, though long chain MOSH can act
as tumour promoters at high doses. Furthermore,
MOSH are able to accumulate in tissues (EFSA
CONTAM Panel (EFSA Panel on Contaminants
in the Food Chain) 2012; Barp et al. 2017). Since
these two fractions have a different toxicological
relevance, it is important to quantify them separately. Several methods have already been reported
in the literature for the analysis of mineral oil in
food and food contact materials. Most of them
involve the online coupling of liquid chromatography (LC) and gas chromatography (GC) with
flame ionisation detector (HPLC–GC–FID) as
described by Biedermann et al. (Biedermann
et al. 2009). Coupled techniques are highly reproducible, allow processing of a large number of
samples per day and are less susceptible to contamination during sample preparation. However,
dedicated instrumentation is needed which is not
commonly available in analytical laboratories.
Alternatively, an offline technique can be used.
Here, the LC-column (of the online coupled LCGC technique) is replaced by a solid phase extraction (SPE) where a glass cartridge is filled with a
sorbent able to retain interfering substances and
allowing an efficient separation of MOSH and
MOAH. Afterwards, the samples always require
re-concentration, followed by analysis with
GC-FID. Large volume injection represents the
best approach to reach high sensitivity, limiting
at the same time losses by volatilisation (possibly
occurring when concentrating the sample to
low volume). Moret et al. have developed this
SPE-GC-FID method (Moret et al. 2011), and
the Bundesinstitut für Risikobewertung (BfR) has
created a method development kit for the analysis
of mineral oil in packaging materials and dry food
(Bundesinstitut für Risikobewertung (BfR) &
(KLZH)).
Up till now, no harmonised European
Regulation exists for mineral oil, nor any national
legislation. Hence, last year, the European commission requested a monitoring of mineral oil
hydrocarbons in food and in materials and articles
intended to come into contact with food
((European Commission 2017). Results should be
provided by 28 February 2019 and until then, no
regulation will be implemented.
In Germany, a fourth draft of the so-called
‘Mineral Oil Regulation’ was released, thereby
establishing a compositional limit for MOAH of
0.5 mg per kg food (German Federal Ministry of
Food and Agriculture 2017). For MOSH, no
migration limits are mentioned. Recently, the
Scientific Committee (SciCom) of the Belgian
Food Safety Agency (FAVV-AFSCA) published
an advice with action thresholds for MOSH and
MOAH. The proposed thresholds are based on the
available information and possible risks (SciCom
of FAVV-AFSCA (Scientific Committee of the
Federal Agency for the Safety of the Food Chain)
2017). Different thresholds varying from 5 to
150 mg kg-1 were established for MOSH depending on the food type, while the available toxicological information for MOAH was too limited to
propose a threshold. Therefore, the analytical
detection limit of 0.5 mg kg-1 was set as action
threshold (SciCom of FAVV-AFSCA (Scientific
Committee of the Federal Agency for the Safety
of the Food Chain) 2017).
Occurrence data of mineral oil in food is rather
scarce. In 2010, Switzerland and Germany performed large market surveys revealing that the
concentration of MOSH migrating from the cardboard packaging into dry foods frequently
exceeded the migration limits proposed by
Germany in the former third draft of ‘Mineral
Oil Regulation’ by a factor 10–50 (Vollmer et al.
2011). More recently, FoodWatch, an independent, non-profit consumer organisation, demonstrated in a market survey that several dry food
products are still contaminated with MOH. A total
FOOD ADDITIVES & CONTAMINANTS: PART A 2063
of 120 food items packed in cardboard from three
different countries (the Netherlands, France and
Germany) were tested. Totally, 100 food items
were contaminated with MOSH, while 51 food
items contained MOAH (Foodwatch 2015).
However, in Belgium, data on the contamination
of the food by mineral oil is lacking.
Consequently, the aim of this paper is to evaluate
the presence of mineral oil in food sold on the
Belgian market. In contrary to previous market
surveys from other countries, samples were
selected based on consumption (i.e. highly consumed food) and not only based on the suspicion
of being contaminated with MOSH and MOAH,
resulting in a selection of a wide variety of different food matrices. The obtained results will be
compared with the action thresholds as proposed
by the SciCom of FAVV-AFSCA (SciCom of
FAVV-AFSCA (Scientific Committee of the
Federal Agency for the Safety of the Food Chain)
2017). Finally, these results will also be used in the
European monitoring programme of mineral oil
hydrocarbons (European Commission 2017).
Materials and methods
Chemicals, solvents and instrumentation
Certified glass 60-ml EPA tubes and Suprasolve
n-hexane and toluene were purchased from VWR.
Dichloromethane (DCM), alkane mixture
(C7-C40), silica gel 60 (particle size 0.063 –
0.2 mm, 70–230 mesh), silver nitrate, aluminium
oxide (alox) 90 active basic (0.063 – 0.2 mm),
3-chloroperbenzoic acid (CPBA) and sodium carbonate (Na2CO3) were obtained from Sigma
Aldrich®. Glass microfiber filters were bought
from Whatman®. The Restek reference standard
containing nine reference standards (n-undecane
(CAS 1120–21-4) [300 µg/ml], n-tridecane (CAS
629–50-5) [150 µg/ml], 1-methylnaphthalene
(CAS 90–12-0) [300 µg/ml], 2-methylnaphthalene
(CAS 91–57-6) [300 µg/ml], 5α-cholestane (CAS
481–21-0) [600 µg/ml], bicyclohexyl (CAS 92–51–
3) [300 µg/ml], pentylbenzene (CAS 538–68-1)
[300 µg/ml], perylene (CAS 198–55-0)[600 µg/
ml] and 1,3,5-tri-tert-butylbenzene (CAS
1460–02-2) [300 µg/ml]) was supplied by
Interscience.
The automated online LC and GC instrumentation with FID (HPLC–GC–FID) consisted of a
Phoenix 9000 syringe pump with five valves, a
UV-4070 detector, a Thermo Trace 1310 gas chromatograph (equipped with two on-column injectors, solvent vapour exit and a transfer switching
valve) and two FID detectors. Injection was by a
CTC Pal with Robotic Tool Change (RTC) of
Thermo Scientific.
Samples
A total of 217 food samples were purchased at
supermarkets in Belgium. A sampling strategy
was developed containing three main steps. First,
food items suspected to be contaminated with
mineral oil were identified. Therefore, results of
previous market surveys conducted in Switzerland
(EFSA CONTAM Panel (EFSA Panel on
Contaminants in the Food Chain) 2012) and
Germany (Vollmer et al. 2011) were investigated
and all foods that contained mineral oil were
listed according to version 2 of the EFSA food
classification and description system for exposure
assessment also known as FoodEx 2 (EFSA 2011).
In the second step, the most important contributors within each food category were identified
based on the consumption frequency. Finally, the
applicability of the method was evaluated for the
selected foods.
Sample preparation
Immediately after purchasing, the samples were
homogenised. Packaging materials were wrapped
in aluminium foil and stored at room temperature. Different extraction methods were applied
depending on the food matrices. During the sample preparation special attention must be paid to
avoid contamination with mineral oil. Therefore, a
few precautions were made. First, it was prohibited for the sampler to use cosmetics containing
mineral oil (e.g. hand creams and lip balsams).
Second, inert glass containers and mineral-oilfree aluminium foil were used to store the food
samples and corresponding packaging. Also tapes
or adhesives were not used to seal the aluminium
foil. Finally, a mineral-oil-free mixer was used for
homogenising the samples.
2064 A. VAN HEYST ET AL.
Dry foods
For dry food, 10 g of the homogenised sample was
weighed into a 60-ml EPA glass tube and 10 µl
Restek standard was added. Mineral oil was
extracted with 10 ml n-hexane overnight after
intense shaking. Then, the sample was again shaken, centrifuged and decanted. A maximum of
100 µl was analysed.
Vegetable and animal fats and oils
The CEN 16995 method was applied for vegetable
and animal fat and oil (European Committee for
Standardization 2017). A 300 mg sample was weighed
into an autosampler vial, filled up with 1 ml n-hexane
and 30 µL Restek standard added. The vial was intensively shaken and placed into the autosampler.
Afterwards, 100 µl was used for analysis.
Wet food
Biedermann and Grob (2012a) developed a specific method for samples containing water. In total,
20 µl Restek standard and 25 ml ethanol were
added to 5 g sample. After 1 h, the sample was
centrifuged, the ethanol was decanted and stored
in a glass vessel. Then, 20 ml n-hexane were added
to the residue and allowed to stand overnight
following which the sample was shaken on a vortex and centrifuged. The decanted n-hexane was
added to the previously decanted ethanol. To
eliminate the ethanol, 50 ml water were added.
After vortexing, an aliquot of the hexane phase
was taken and analysed.
Sweets
For sweets, the procedure as described by
Biedermann and Grob was applied, meaning that
10 µl Restek standard was added to 10 g of sample.
Next 100 ml warm water was added. After adding
10 ml n-hexane, the sample was intensively shaken. A maximum of 100 µl n-hexane phase was
used for analysis (Biedermann and Grob 2012a)
Auxiliary methods
Some samples contained naturally occurring olefins or primarily odd numbered n-alkanes which
complicate the mineral oil analysis as extensively
described by Biedermann and Grob (Biedermann
and Grob 2012a). Therefore, auxiliary methods
were developed.
To eliminate olefins that interfere with the
MOAH analysis, an epoxidation was developed
by Biedermann, Fiselier and Grob (Biedermann
et al. 2009). Totally, 300 mg of sample were
weighed in a 15-ml glass centrifuge tube, and
30 µl Restek standard and 3 ml of DCM
were added. After cooling in ice for 5 min, 1 ml
of cooled 10% CPBA solution was added. The
sample was intensively shaken and allowed to
warm to ambient temperature for 15 min.
Afterwards, 3 ml of 10% Na2CO3 solution was
added. The sample was shaken for 15 s and centrifuged. The aqueous supernatant was discarded,
and the sample was washed with 3 ml water. Of
the DCM phase, 1.5 ml was transferred to an
autosampler vial and brought to dryness by a
stream of nitrogen. The residue was dissolved in
1 ml of n-hexane. Finally, 100 µl was analysed.
For elimination of natural n-alkanes that interfere with the MOSH analysis, an additional cleanup with aluminium oxide (alox) was required
(Fiselier et al. 2009; Fiselier and Grob 2009).
Approximately, 300 mg sample were weighed in
a 60-ml EPA tube and 30 µl of Restek standard
were added. The sample was dissolved in 2 ml
n-hexane. Then, the Other Article: was transferred to an alox/silica SPE cartridge previously
prepared with 10 g alox and 3-g activated silica
gel. The cartridge was rinsed with 20 ml n-hexane
and the sample was loaded. The aliphatic hydrocarbon fraction was eluted with 25 ml n-hexane. A
few drops of toluene were added as keeper and the
solvent was evaporated with a rotary evaporator
under vacuum (>300 mbar, 40°C). Attention was
paid that the residue was not evaporated to dryness to avoid loss of volatile hydrocarbons. The
extract was dissolved in 2 ml n-hexane and 1 ml
was transferred to an autosampler vial. A total
amount of 100 µl was analysed.
Analysis of mineral oil
Mineral oil was determined with an online
coupled HPLC-GC-FID (Biedermann et al.
2009). Briefly, 5–100 µl of the extracts (depending
on the fat content) were injected onto a
25 cm × 2 mm i.d. HPLC column packed with
Luna Silica 100 (5 µm) and analysed at
300 µl min-1 using a gradient starting with nFOOD ADDITIVES & CONTAMINANTS: PART A 2065
hexane and reaching 35% DCM after 0.2 min. The
column was back flushed after the injection with
DCM at 500 µl min-1 for 9 min, and then reconditioned at 500 µl min-1 with n-hexane for 10 min
and at 300 µl min-1 up to the subsequent injection. Both fractions were transferred to the GC
while passing the UV detector for controlling the
gradient in the column effluent at 230 nm: breakthrough of DCM was observed after 4.5 min as a
steep increase of absorption to a plateau level. The
elution of perylene was verified indicating the end
of the transfer. The MOSH fraction was transferred by a switching valve to the first GC column
and the MOAH fraction to the second GC column. Both fractions were analysed simultaneously
with the same GC programme. The carrier gas
inlet pressure of the GC was set to 60 kPa. The
oven temperature was programmed at 30°C min-1
from 55°C to 360°C after elution of the solvent
(8 min after starting transfer). The FID was set at
370°C. The method was validated in-house and
afterwards, the validated methods were successfully applied in proficiency tests organised by the
German reference office for proficiency testing
and reference materials (DRRR). The limits of
quantification (LOQ) for MOSH and MOAH
were always below 0.5 mg kg-1, but varied
depending on the type of mineral oil and the
food matrix. However, an LOQ of 0.5 mg kg-1
was applied for all food matrices in the discussion
of the results.
Interpretation of chromatograms
Bicyclohexyl and 1-methylnaphthalene were used to
calculate the concentrations for MOSH and MOAH,
respectively. Additional verification standards were
added to check performance of the method (see
Figure 1) (Vollmer et al. 2011; Biedermann and
Grob 2012b). Integration of mineral oil humps was
done semi-automated with Chromeleon, a software
tool for chromatography data interpretation
Figure 1. Chromatograms of MOSH and MOAH fractions of chocolate flakes.
2066 A. VAN HEYST ET AL.
(Thermo scientificTM DionexTM chromeleonTM 7
Chromatography data system 7.2 SR5). The key
aspects of the integration can be listed as follows:
first, the baseline must be horizontal till the end of
the mineral oil hump. Therefore, in the chromatogram, a point was selected where no elution of solute
material was observed. Second, the beginning and
end of the mineral oil hump were determined using
a reference alkane mixture (C7-C40). Then, the
MOSH fraction was integrated from hydrocarbons
with 10 carbon atoms (C10) till hydrocarbons with
40 carbon atoms (C40). If in the same retention time
range a hump was found for the MOAH fraction,
this hump was also integrated from C10 till C40.
Next, the internal standards were automatically
identified and integrated resulting in an automatic
evaluation of the performance of the method.
Finally, components naturally occurring in food or
other non-mineral oil peaks on top of the hump
were subtracted from the MOSH and MOAH
humps (Biedermann and Grob 2012b).
Results and discussion
Selection of the samples
The aim of the sampling strategy was to target
food items which were suspected to contain
mineral oil, and items which are highly consumed
both in quantity and in frequency, because results
will be used for the calculation of the exposure to
mineral oil of the Belgian population. To compare
results more easily with previous exposure studies,
food items were classified according to FoodEx 2.
This is a food classification system developed by
EFSA in 2009 with the objective of simplifying the
linkage between occurrence and food consumption data when assessing the exposure to hazardous substances (EFSA 2011, 2012)
A first selection was made by identifying food
categories suspected to be contaminated with
mineral oil. All food categories related to drinks
were excluded since packaging is the predominant
source of mineral oils and packaging of drinks
always include a functional barrier. For the
remaining food categories, only those with food
items contaminated with mineral oil according to
previous market surveys were withheld. These
food categories are ‘animal and vegetable fats
and oils’, ‘grain and grain-based products’, ‘vegetables and vegetable products’, ‘composite dishes’,
‘legumes, nuts, oilseeds and spices’, ‘coffee, cocoa,
tea and infusions’, ‘sugar and similar, confectionery and water-based sweet desserts’, ‘fish, seafood,
amphibians, reptiles and invertebrates’, ‘meat and
meat products (incl. edible offal)’ and ‘major isolated ingredients, additives, flavours, baking and
processing aids’. In the second step, the most
important contributors to the daily intake of
food items of the adult population within each
food category were identified using the consumption frequency of the food consumption survey of
2014 performed by the Scientific Institute of
Public Health (De Ridder et al. 2016). Only food
items with a cumulative frequency of 90% or
higher were selected. In food categories where
none of the food items had a cumulative frequency of 90%, the 10 highest contributors were
taken into account. Next, the Euromonitor database ‘Packaged Food market research’, containing
valuable information on the brand shares of packaged food items in Belgium was consulted, resulting in a final selection of 217 samples. An
overview of the samples is given in Table 1.
Since the selection of the samples was based on
the dietary habits of the Belgian population, the
results could afterwards be used for the evaluation
of the exposure to mineral oil. Furthermore, this
also results in a selection of food matrices that
were rarely included in previous market surveys
on mineral oil such as sweets, vegetables, meat and
fish.
Sample analysis
After the selection of the samples, the applicability
of the method was evaluated. Four different
extraction methods were implemented based on
the different characteristics of the food: (i) dry
food, (ii) wet food, (iii) sweets and (iv) vegetable
and animal fats and oils. Next, the most appropriate method was allocated for each food item
included in the sampling. An overview is given in
Table 1. However, the methodology was not suitable for 19 (out of 217) samples. For example,
some tea samples and potato crisps showed severe
interferences in the MOSH and/or MOAH hump.
Application of the auxiliary methods was not
FOOD ADDITIVES & CONTAMINANTS: PART A 2067
sufficient to remove these interferences. Therefore,
it was not possible to correctly determine the
concentration of mineral oil in these samples.
Consequently, the results will be discussed for
the remaining 198 samples.
Mineral oil saturated hydrocarbons (MOSH)
The results obtained for the MOSH are presented
in Table 2. MOSH was detected in 142 samples
with concentrations up to 84.82 mg kg-1, while a
concentration below LOQ was determined for 56
samples. It should be noted that these MOSH
concentrations were generally lower compared
with previous studies. (Vollmer et al. 2011). This
might indicate that the market has evolved and
has taken some important measures. For instance,
the share of recycled fibres that is in direct contact
with food has significantly decreased, and there
has been a shift to migration-poor and/or migration-free ink when printing packaging or the use
of functional barriers between food and packaging
cardboard (Matissek and Industry 2014).
As previously mentioned, some food matrices
were analysed that were rarely included in the
previous market surveys such as fish meat (cod
and sole samples), where only canned fish was
tested earlier, and meat products (chicken leg
and beef). Only one meat sample contained
MOSH (i.e. 16.86 mg kg-1), while all other fish
and meat samples had no quantifiable amount of
MOSH. Similarly, vegetables (e.g. carrot, mushroom, onion and tomato) were never included in
previous studies. Similarly to fish and meat, concentrations of MOSH were always below the LOQ
for these vegetables. A possible explanation could
be that these food items are less in contact with
potential sources of mineral oil. Additionally, the
characteristics of these foodstuffs are less prone to
absorption of the very apolar mineral oil.
Other interesting samples were coffee and tea.
For these samples, only the dry product was analysed and not the infusion or prepared beverage. A
few coffee samples and one tea sample showed a
relatively high MOSH concentration (i.e. ranging
from 1.91 mg kg-1 to 7.42 mg kg-1). The reason
for this contamination can be found in the jute
bags that are used for transportation of the raw
product since they are impregnated with a substance to preserve the food. However, this substance often contains mineral oil.
A category that was rarely analysed up till now,
but that gave interesting results, is ‘Sugar and
similar, confectionery and water-based sweet
desserts’, namely chocolate flakes, sweets and
Table 1. Number of samples and extraction method grouped by FoodEx 2 food categories.
FoodEx 2 level 1 FoodEx 2 level 2
Number of
samples
Extraction
method
Animal and vegetable fats and oils and primary derivatives
thereof
Animal and vegetable fats/oils 13 Vegetable oils
Grain and grain-based products Bread and similar products 10 Dry food
Fine bakery wares 30 Dry food
Pasta, dough and similar products 14 Dry food
Cereals and cereal primary derivatives 28 Dry food
Breakfast cereals 16 Dry food
Vegetables and vegetable products Bulb vegetables 1 Wet food
Fruiting vegetables 2 Wet food
Fungi, mosses and lichens 1 Wet food
Root and tuber vegetables (excluding starchy- and sugar-) 1 Wet food
Composite dishes Soups and salads 1 Wet food
Fried or extruded cereal or root-based products 6 Dry food
Legumes, nuts, oilseeds and spices Processed legumes, nuts, oilseeds and spices 14 Dry food
Nuts, oilseeds and oil fruits 18 Dry food
Coffee, cocoa, tea and infusions Coffee, cocoa, tea and herbal ingredients 13 Dry food
Sugar and similar, confectionery and water-based sweet
desserts
Confectionery including chocolate 17 Dry food/
Sweets
Sugar and other sweetening ingredients (excluding
intensive sweeteners)
10 Dry food
Fish, seafood, amphibians, reptiles and invertebrates Fish meat 7 Wet food
Meat and meat products (incl. edible offal) Mammals and birds meat 6 Wet food
Major isolated ingredients, additives, flavours, baking and
processing aids
Starches 9 Dry food
Total 217
FoodEx 2, food classification system developed by EFSA
2068 A. VAN HEYST ET AL.
sugars. No sugar sample contained mineral oil
(i.e. below LOQ). The chocolate flakes, on the
one hand, had an average MOSH value
(6.64 mg kg-1). There are a few possible explanations for this contamination. Similarly, to the
coffee beans, the cacao beans were transported
Table 2. MOSH concentrations grouped by food types.
LOQ Auxiliary method MOSH Total (mg kg-1)
Sample FoodEx 2 level 2 category N mg kg-1 Alox Mean Maximum
Advent calendar
Almond
Beef, rump steak
Biscuit with chocolate, coating
Biscuit, Nic nac
Biscuit, Petit beurre
Biscuit, Spiced ordinary
Bread brown, ordinary (water)
Bread white, farmers
Breakfast cereals, flakes, white
Breakfast cereals, muesli
Breakfast cereals, puffed balls, rings
Bulgur
Cake, ordinary (sponge cake)
Carrot
Cashew nut
Chicken, leg, whole
Chocolate flakes dark
Confectionery including chocolate
Nuts, oilseeds and oilfruits
Mammals and birds meat
Fine bakery wares
Fine bakery wares
Fine bakery wares
Fine bakery wares
Bread and similar products
Bread and similar products
Breakfast cereals
Breakfast cereals
Breakfast cereals
Cereals and cereal primary derivatives
Fine bakery wares
Root and tuber vegetables
Nuts, oilseeds and oilfruits
Mammals and birds meat
Confectionery including chocolate
1
3
3
4
4
3
4
5
5
5
6
5
2
3
1
3
3
3
Chocolate flakes milk
Confectionery including chocolate
3
Chocolate powder and analogous products Coffee, cocoa, tea and herbal ingredients
1
Cod
Coffee with caffeine
Common sole, Dover sole
Couscous
Cucumber
Fish meat
Coffee, cocoa, tea and herbal ingredients
Fish meat
Pasta, dough and similar products
Fruiting vegetables
4
5
3
3
1
Deep frying fat
Animal and vegetable fats and oils
5
Frangipane
Lentil, dry
Lentil, oil
Mixed nuts
Mushroom, champignon
Oatmeal
Oil, Olive
Oil, Sunflower
Onion, normal
Pasta, white, lasagna ‘sheets’
Pasta, white, long
Pea, dry
Pea, oil
Peanut
Pine kernel
Potato crisps
Pudding, corn starch/pudding powder
Quinoa
Rice, white
Rice, whole meal
Semolina
Starch, Maïzena
Sugar, brown
Sugar, white, granulated
Sugar, white, powdered
Sweetener, base stevia, crystals
Sweetener, base stevia, powder
Sweets
Tea, Black
Tomato
Vegetables, mix for soup
Waffle, ‘Liege’
Fine bakery wares
Processed legumes, nuts, oilseeds and spices
Processed legumes, nuts, oilseeds and spices
Nuts, oilseeds and oilfruits
Fungi, mosses and lichens
Cereals and cereal primary derivatives
Animal and vegetable fats and oils
Animal and vegetable fats and oils
Bulb vegetables
Pasta, dough and similar products
Pasta, dough and similar products
Processed legumes, nuts, oilseeds and spices
Processed legumes, nuts, oilseeds and spices
Nuts, oilseeds and oilfruits
Nuts, oilseeds and oilfruits
Fried or extruded cereal or root-based products
Starches
Cereals and cereal primary derivatives
Cereals and cereal primary derivatives
Cereals and cereal primary derivatives
Cereals and cereal primary derivatives
Starches
Sugar and other sweetening ingredients
Sugar and other sweetening ingredients
Sugar and other sweetening ingredients
Sugar and other sweetening ingredients
Sugar and other sweetening ingredients
Confectionery including chocolate
Coffee, cocoa, tea and herbal ingredients
Fruiting vegetables
Soups and salads
Fine bakery wares
3
2
3
3
1
5
4
4
1
4
7
3
5
3
3
1
4
6
5
5
1
5
3
4
1
1
1
4
1
1
1
4
Waffle, vanilla
Walnut
Wheat bran
Fine bakery wares
Nuts, oilseeds and oilfruits
Cereals and cereal primary derivatives
4
3
4
Total
198
MOSH, mineral oil saturated hydrocarbons; FoodEx 2, food classification system developed by EFSA; N, number of samples; LOQ, limit of quantification; Yes°,
auxiliary method was not applied to all samples in this category; * only one sample thus calculation of the mean was not possible. To calculate the mean,
values below LOQ were considered as zero.
FOOD ADDITIVES & CONTAMINANTS: PART A 2069
in jute bags. Additionally, the chocolate flakes are
always in direct contact with the (recycled) cardboard packaging, i.e. without the presence of a
functional barrier used. Sweets, on the other
hand, contained relatively high amounts of
MOSH (i.e. up to 84.82 mg kg-1). The MOSH
profile clearly shows the presence of n-alkanes
in a typical wax profile. Since mineral-oil-containing food additives are allowed to be used for
surface treatment of sweets, this could explain the
presence MOSH in sweets. However, these additives were not listed on the label. To identify the
source, the ingredients should carefully be
investigated.
Finally, it was evaluated whether the type of
packaging could explain the concentrations that
were found in the food. Whereas, all pudding
powder samples contained MOSH (ranging from
1.71 mg kg-1 to 11.40 mg kg-1) and they are all in
direct contact with paper and board packaging,
the packaging should be analysed to identify the
potential source of the contamination. However,
the results in the categories ‘grain and grain based
products’ and ‘Legumes, nuts, oilseeds and spices’
could not be linked to the type of packaging. In
the former, 86 of the 99 samples have MOSH
values above LOQ, including samples packed in
cardboard and plastic. The latter category contains
peas and lentils that are sold and packed in two
different ways: dry packed in cardboard or in oil
packed in cans. An interesting observation is that
MOSH was found only in the dry samples. This
could indicate that mineral oil is not naturally
present in the food items but more likely migrates
from packaging material into the food.
Mineral oil aromatic hydrocarbons (MOAH)
For this fraction, there were 175 samples with a
concentration below the LOQ. They all belonged to
the following categories: ‘composite dishes’, ‘fish,
seafood, amphibians, reptiles and invertebrates’,
‘legumes, nuts, oilseeds and spices’, ‘meat and meat
products’ and ‘vegetables and vegetable products’.
However, 23 samples contained MOAH with a concentration ranging from 0.6 to 2.24 mg kg-1
(Table 3). For instance, almost all vegetable oils
and chocolate flakes showed concentrations above
LOQ (see Figures 1-3). Also, for one of the six
analysed coffee samples, a MOAH concentration
was found. The cocoa and coffee beans were likely
transported in jute bags. To make them flexible,
these bags are often treated with a batching oil containing a high boiling mineral oil fraction (Grob
et al. 1991). The remaining samples with a concentration greater than LOQ, including pudding powder, lasagne sheets, oatmeal, couscous, wholemeal
and white rice, were all packed in direct contact
with cardboard (see Figures 4 and 5). Therefore, it
would be interesting to analyse the packaging to
identify the source of contamination.
Evaluation of the results
To date, there are no official regulatory limits at
European or national level. Therefore, results are
compared with the action thresholds for MOSH
and MOAH proposed by SciCom in Advice
19–2017 (SciCom of FAVV-AFSCA (Scientific
Committee of the Federal Agency for the Safety
of the Food Chain) 2017). The SciCom proposed
thresholds based on the available information
and possible risks. Different thresholds varying
from 5 to 150 mg kg-1 were established for the
MOSH fraction C16 – C35, depending on the
food type. Since the SciCom used another fraction for MOSH, C16 – C35 instead of C10 –
C40, only the fraction C16 – C35 will be taken
into account for the comparison. All samples
except one comply with the proposed action
thresholds for MOSH (see Table 4). This sample
has to be further investigated to identify the
source of contamination. Therefore, the packaging material must be analysed, such as the food
additives mentioned on the packaging (e.g.
E905) as other ingredients, for example coconut
fat or gum that were used to produce the
sample.
As for MOAH the available toxicological information was too limited to propose a threshold, the
analytical detection limit of 0.5 mg kg-1 was used.
Totally, 23 samples contained a concentration above
the analytical detection limit of 0.5 mg kg-1 food for
the MOAH fraction C16 till C35 (see Table 5).
However, it should be noted that the CEN method
used for the analysis of vegetable fat and oils has a
specific application limit of 10 mg kg-1 (European
Committee for Standardization 2017). This application limit has been established by interlaboratory
tests organised by ITERG in commissioned by the
2070 A. VAN HEYST ET AL.
European Committee for Standardisation. From
these interlaboratory tests, it was concluded that
the variability between the results was too large for
values below 10 mg kg-1. Therefore, an application
limit was set at 10 mg kg-1 vegetable fat and oil
(European Committee for Standardization 2017).
Table 3. MOAH concentrations grouped by food types.
LOQ Auxiliary method MOAH Total (mg kg-1)
Sample FoodEx 2 level 2 category N mg kg-1 Epoxidation Mean Maximum
Advent calendar
Confectionery including chocolate
1
Almond
Beef, rump steak
Nuts, oilseeds and oilfruits
Mammals and birds meat
3
3
Biscuit with chocolate, coating
Fine bakery wares
4
Biscuit, Nic nac
Fine bakery wares
4
Biscuit, Petit beurre
Fine bakery wares
3
Biscuit, Spiced ordinary
Fine bakery wares
4
Bread brown, ordinary (water)
Bread and similar products
5
Bread white, farmers
Bread and similar products
5
Breakfast cereals, flakes, white
Breakfast cereals
5
Breakfast cereals, muesli
Breakfast cereals
6
Breakfast cereals, puffed balls, rings
Breakfast cereals
5
Bulgur
Cereals and cereal primary derivatives
2
Cake, ordinary (sponge cake)
Fine bakery wares
3
Carrot
Root and tuber vegetables
1
Cashew nut
Chicken, leg, whole
Nuts, oilseeds and oilfruits
Mammals and birds meat
3
3
Chocolate flakes dark
Confectionery including chocolate
3
Chocolate flakes milk
Confectionery including chocolate
3
Chocolate powder and analogous products Coffee, cocoa, tea and herbal ingredients
1
Cod
Fish meat
4
Coffee with caffeine
Common sole, Dover sole
Couscous
Coffee, cocoa, tea and herbal ingredients
Fish meat
Pasta, dough and similar products
5
3
3
Cucumber
Fruiting vegetables
1
Deep frying fat
Animal and vegetable fats and oils
5
Frangipane
Lentil, dry
Lentil, oil
Mixed nuts
Mushroom, champignon
Oatmeal
Fine bakery wares
Processed legumes, nuts, oilseeds and spices
Processed legumes, nuts, oilseeds and spices
Nuts, oilseeds and oilfruits
Fungi, mosses and lichens
Cereals and cereal primary derivatives
3
2
3
3
1
5
Oil, Olive
Animal and vegetable fats and oils
4
Oil, Sunflower
Animal and vegetable fats and oils
4
Onion, normal
Pasta, white, lasagna ‘sheets’
Pasta, white, long
Pea, dry
Pea, oil
Peanut
Bulb vegetables
Pasta, dough and similar products
Pasta, dough and similar products
Processed legumes, nuts, oilseeds and spices
Processed legumes, nuts, oilseeds and spices
Nuts, oilseeds and oilfruits
1
4
7
3
5
3
Pine kernel
Nuts, oilseeds and oilfruits
3
Potato crisps
Pudding, corn starch/pudding powder
Fried or extruded cereal or root-based products
Starches
1
4
Quinoa
Cereals and cereal primary derivatives
6
Rice, white
Cereals and cereal primary derivatives
5
Rice, whole meal
Cereals and cereal primary derivatives
5
Semolina
Cereals and cereal primary derivatives
1
Starch, Maïzena
Starches
5
Sugar, brown
Sugar and other sweetening ingredients
3
Sugar, white, granulated
Sugar and other sweetening ingredients
4
Sugar, white, powdered
Sugar and other sweetening ingredients
1
Sweetener, base stevia, crystals
Sugar and other sweetening ingredients
1
Sweetener, base stevia, powder
Sugar and other sweetening ingredients
1
Sweets
Tea, Black
Tomato
Confectionery including chocolate
Coffee, cocoa, tea and herbal ingredients
Fruiting vegetables
4
1
1
Vegetables, mix for soup
Soups and salads
1
Waffle, ‘Liege’
Fine bakery wares
4
Waffle, vanilla
Walnut
Fine bakery wares
Nuts, oilseeds and oilfruits
4
3
Wheat bran
Cereals and cereal primary derivatives
4
Total
198
* <LOQ
* <LOQ
* <LOQ
* <LOQ
* <LOQ
* <LOQ
* <LOQ
* <LOQ
* <LOQ
* <LOQ
* <LOQ
MOAH, mineral oil aromatic hydrocarbons; FoodEx 2, food classification system developed by EFSA; N, number of samples; LOQ, limit of quantification; Yes°,
auxiliary method was not applied to all categories; * only one sample thus calculation of the mean was not possible. To calculate the mean, values below
LOQ were considered as zero.
FOOD ADDITIVES & CONTAMINANTS: PART A 2071
Figure 2. Chromatograms of MOSH and MOAH fractions of olive oil.
Figure 3. Chromatograms of MOSH and MOAH fractions of sunflower oil.
2072 A. VAN HEYST ET AL.
Figure 4. Chromatograms of MOSH and MOAH fractions of rice.
Figure 5. Chromatograms of MOSH and MOAH fractions of lasagne sheets.
FOOD ADDITIVES & CONTAMINANTS: PART A 2073
With the application limit taken into account, only
14 samples went above the detection limit. These 14
samples comprise chocolate flakes, lasagne ‘sheets’,
oatmeals, pudding powder, couscous, rice and coffee. Further investigation is needed.
Conclusion
Consistent with previous studies, this study demonstrated that mineral oil is present in food. Mineral oil
was detected by implementing a LC-GC-FID method
developed by Biedermann and Grob (Biedermann
and Grob 2012a, 2012b). Concentrations were found
for MOSH up to 84.82 mg kg-1 and for MOAH just
up to 2.24 mg kg-1. However, the measured concentrations are lower compared with previous market
surveys, indicating that the adaptations made by
packaging industries and food industry in their processes to prevent migration of mineral oil are improving the situation effective (Vollmer et al. 2011; EFSA
CONTAM Panel (EFSA Panel on Contaminants in
the Food Chain) 2012; Biedermann et al. 2013).
Nevertheless, there is still a fraction of mineral oil
able to migrate into food items, a migration that is
not controlled at this moment. This is a matter of
concern especially for the MOAH fraction.
When comparing the results with the proposed
action thresholds of the SciCom, it can be concluded that most of the samples are in compliance.
However, a few samples show high concentrations
and thus further investigation is needed such as
analysing packaging or individual ingredients of
the food samples. Due to the mutagenic potential
of the MOAH fraction, attention must be paid to
avoid mineral oil contamination.
Acknowledgments
The research that yielded these results was funded by the
Belgian Federal Public Service of Health, Food Chain Safety
and Environment through the contract RF 15/6296 MinOil.
Séverine Goscinny of SCIENSANO shared her expertise on
developing sampling strategies and interpretation of consumption data of the Belgium population.
Disclosure statement
No potential conflict of interest was reported by the authors.
Funding
This work was supported by the Belgian Federal Public
Service of Health, Food Chain Safety and Environment [RF
15/6296 MinOil].
Table 4. MOSH concentrations compared with action thresholds SciCom.
Category
Action threshold SciCom <Action threshold >Action threshold
[MOSH] (mg kg-1) # Samples # Samples
Animal and vegetable fats and oils 100 9 0
Grain and grain-based products 15 99 0
Vegetables and vegetable products (incl. fungi) 20 13 0
Legumes, nuts and oilseeds 150 29 0
Snacks, desserts and other foods 20 10 0
Sugar and similar, confectionery and desserts 30 24 1
Fish and other seafood 60 7 0
Meat and meat products (incl. edible offal) 30 6 0
Total 197 1
SciCom, Scientific Committee of the Belgian Food Safety Agency (FAVV-AFSCA); MOSH, mineral oil saturated hydrocarbons.
Table 5. MOAH concentrations compared with analytical detection limit SciCom.
Category
Analytical detection limit <Detection limit >Detection limit
[MOAH] (mg kg-1) # Samples # Samples
Animal and vegetable fats and oils 0.5 5 8
Grain and grain-based products 0.5 95 7
Vegetables and vegetable products (incl. fungi) 0.5 11 1
Legumes, nuts and oilseeds 0.5 31 0
Snacks, desserts and other foods 0.5 3 2
Sugar and similar, confectionery and desserts 0.5 17 5
Fish and other seafood 0.5 7 0
Meat and meat products (incl. edible offal) 0.5 6 0
Total 175 23
SciCom, Scientific Committee of the Belgian Food Safety Agency (FAVV-AFSCA); MOAH, mineral oil aromatic hydrocarbons.
2074 A. VAN HEYST ET AL.
ORCID
Annelies Van Heyst http://orcid.org/0000-0002-5549-5675
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