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JFS T: Toxicology and Chemical Food Safety

Persistent Organic Pollutants in Fish Oil


Supplements on the Canadian Market:
Polychlorinated Biphenyls and
Organochlorine Insecticides
DOROTHEA F.K. RAWN, K. BREAKELL, V. VERIGIN, H. NICOLIDAKIS, D. SIT, AND M. FEELEY

ABSTRACT: Fish and seal oil dietary supplements, marketed to be rich in omega-3 fatty acids, are frequently con-
sumed by Canadians. Samples of these supplements (n = 30) were collected in Vancouver, Canada, between 2005
and 2007. All oil supplements were analyzed for polychlorinated biphenyls (PCBs) and organochlorine insecticides
(OCs) and each sample was found to contain detectable residues. The highest PCB and DDT (1,1,1-trichloro-di-
(4-chlorophenyl)ethane) concentrations (10400 ng/g and 3310 ng/g, respectively) were found in a shark oil sam-
ple while lowest levels were found in supplements prepared using mixed fish oils (anchovy, mackerel, and sardine)
(0.711 ng PCB/g and 0.189 ng DDT/g). Mean PCB concentrations in oil supplements were 34.5, 24.2, 25.1,
95.3, 12.0, 5260, 321, and 519 ng/g in unidentified fish, mixed fish containing no salmon, mixed fish with salmon,
salmon, vegetable with mixed fish, shark, menhaden (n = 1), and seal (n = 1), respectively. Maximum concentrations
of the other OCs were generally observed in the seal oil. The hexachlorinated PCB congeners were the dominant
contributors to PCB levels, while DDT was the greatest contributor to organochlorine levels. Intake estimates
were made using maximum dosages on manufacturers’ labels and results varied widely due to the large difference
in residue concentrations obtained. Average PCB and DDT intakes were calculated to be 736 ± 2840 ng/d and
304 ± 948 ng/d, respectively.
Keywords: contaminants, dietary supplements, organochlorine insecticides, persistent organic pollutants, poly-
chlorinated biphenyls

Introduction than those collected from the wild (Easton and others 2002; Hites

F ish consumption is associated with health benefits in part due


to the presence of the essential polyunsaturated fatty acids
(PUFAs), particularly the omega-3 fatty acids in fish, which cannot
and others 2004). In contrast to the PUFAs present in fish oils,
POPs have been associated with negative health implications in-
cluding immunotoxicity and carcinogenicity (Fernandez and oth-
be synthesized by mammals (Hamilton and others 2005). The other ers 2004). Impacts to normal endocrine function and reproduction
essential lipids, omega-6 fatty acids, are found in fish tissue; how- also have been observed in fish and other wildlife, leading to con-
ever, they are also available through other foods (Hamilton and oth- cerns regarding potential impacts to humans (Safe 2000; Safe 2004;
ers 2005). The intake of the omega-3 fatty acids in fish is associated Sapozhnikova and others 2004). Public concern over potential neg-
with improvement in vascular health and reduced risk of coronary ative health impacts due to contaminant exposure has resulted in
heart disease in humans (Storelli and others 2004; Covaci and oth- follow-up surveys and assessments to establish the level of risk as-
ers 2007). Additionally, consumption of fish has been linked to both sociated with consumption of retail fish/seafood in Canada. The re-
a reduction in incidence of diabetes and symptoms of rheumatoid sults of this study indicated that the levels of POPs in fish did not
arthritis (Storelli and others 2004). As a result of the health benefits, pose a human health risk (Tittlemier and others 2004; Rawn and
Canadians continue to be encouraged to eat fish on a frequent basis others 2006; Health Canada 2007b).
(for example, 2 fish servings weekly) (Health Canada 2007a). Because the public remains interested in enjoying the health
Over the last decade, elevated levels of persistent organic pol- benefits associated with the consumption of food rich in essential
lutants (POPs), including polychlorinated biphenyls (PCBs) and fatty acids, individuals consume fish oil supplements to enhance
organochlorine insecticide (OC) compounds, have been reported their health. PCBs and OC insecticides are lipophilic compounds
in fish products around the world, particularly in farmed fish rather and, therefore, are anticipated to be present in fish oils. The prepa-
ration of fish oil supplements, however, does include the processing
of raw fish oils to remove specific contaminants including trace el-
MS 20080599 Submitted 8/5/2008, Accepted 10/8/2008. Author Rawn is ements, pigments, odors, oxidation products, and so on, and can
with Food Research Div., Bureau of Chemical Safety and author Feeley is also result in a corresponding reduction in the POP levels (Hilbert
with Chemical Health Hazard Assessment Div., Health Products and Food and others 1998). Reductions can range from 0% to 100% depend-
Branch, Health Canada, Sir Frederick Banting Research Centre, 251 Sir
Frederick Banting Driveway, Tunney’s Pasture, Ottawa, ON, Canada, K1A ing on the refinement step (Hilbert and others 1998). Compara-
Chemical Food Safety

0K9. Authors Breakell, Verigin, Nicolidakis, and Sit are with Food Direc- tive testing of different grades of fish oil, however, has shown that
torate, Western Region, 3155 Willington Green, Burnaby, BC, Canada, V5G
T: Toxicology &

4P2. Direct inquiries to author Rawn (E-mail: Thea Rawn@hc-sc.gc.ca). POP concentrations in fish oils vary widely and do not always cor-
respond to the marketing grade (Jacobs and others 1998).

C 2008 Her Majesty the Queen in Right of Canada, as Represented by
the Minister of Agriculture and Agri-Food Canada
T14 JOURNAL OF FOOD SCIENCE—Vol. 74, Nr. 1, 2008 C 2008 Institute of Food Technologists
Journal compilation  R

doi: 10.1111/j.1750-3841.2008.01020.x
Further reproduction without permission is prohibited
PCB, OCs in fish oil dietary supplements . . .

POP concentrations in fish oils vary due to the type of fish used plied by Fisher Scientific. Glass wool, celite, silica, sodium sulfate,
in the oil preparations as well as the location from which the fish and Florisil were all Soxhlet extracted for several hours with DCM
were collected (Falandysz and others 1994; Jacobs and others 2004; and subsequently heated overnight to 300 ◦ C prior to use. They
Akutsu and others 2006). For example, cod liver oils have elevated were stored in a desiccator until use. Trace pure grade anhydrous
POP levels relative to those measured in other fish oils or fish oils sodium sulfate was purchased from Baker (Cheshire, U.K.), and
mixed with vegetable oils (Jacobs and others 2004). Although POP heated at 300 ◦ C for 18 h prior to use.
levels in biota are readily available in the literature, concentrations Analytical standards of both the native and 13 C analogues of the
in fish-based oils are not reported as frequently. PCBs and OC insecticides were purchased from Wellington Labora-
A wide variety of fish oils are available on the Canadian re- tories (Guelph, ON, Canada). All standards were prepared as mix-
tail market and can be consumed as part of an individual’s daily tures in toluene or nonane.
health regimen. Individual supplements may contain oil from a sin-
gle fish, marine mammal (for example, seal), or a mixture of oils Extraction and clean up
from more than 1 type of fish. Additionally, some supplements con- The oil from individual capsules of a given product were re-
tain vegetable or grain oils combined with fish oil. This study was moved from the capsules and combined. Subsamples of the oil
developed to evaluate the concentrations of POPs in dietary (0.5 g) were spiked with surrogate standards containing 35 13 C PCBs
supplements containing fish-based oils marketed as sources of (1, 3, 4, 8, 15, 19, 28, 52, 54, 70, 77, 81, 95, 101, 104, 105, 114, 118, 123,
omega-3 fatty acids, available in on the Canadian market. Sam- 126, 128, 138, 153, 155, 156, 157, 167, 169, 170, 180, 189, 202, 205,
ples were collected between 2005 and 2007, with the analyses com- 208, 209) and 13 C analogues of all the OC compounds measured
pleted in 2007. (1,2,3,4 tetrachlorobenzene, pentachlorobenzene, α-HCH, β-HCH,
γ -HCH, hexachlorobenzene, oxychlordane, trans-chlordane, trans-
Materials and Methods nonachlor, cis-nonachlor, p,p -DDE, p,p -DDT, and mirex) with the
exception of 1,2,3,5 tetrachlorobenzene, prior to extraction. The
Samples subsample was diluted to 3 mL in a 15-mL centrifuge tube with
Fish oil supplements were collected from pharmacies, health DCM.
food stores, Internet distributors, and large supermarkets in Van- The initial step in lipid removal was performed using an Agi-
couver, Canada. The supplements selected included those that lent high performance preparative gel permeation chromatogra-
were available locally, via small suppliers, in addition to those dis- phy (GPC) system (New Castle, Del., U.S.A.), consisting of an 1100
tributed across Canada to ensure collection of a wide range of Series quaternary pump, autosampler, and a fraction collector. Two
categories of these products. A total of 30 samples (Table 1) were Envirogel columns (150 × 19 mm and 300 × 19 mm) (Waters,
collected for analysis and included supplements containing oil Milford, Mass., U.S.A.) were used in series and DCM as the mobile
from individual species (for example, salmon, seal, or shark) or mix- phase with a flow rate of 5 mL/min. The GPC eluate was evaporated
tures of oil from a variety of fish sources (for example, salmon, to near dryness and was reconstituted in 1 mL hexane.
anchovy, sardine, mackerel). Although oil type was identified on Following the GPC step, 10 mL disposable serological pipettes
sample containers in most cases, the geographical location from plugged with glass wool were filled with 4 g silica gel that had been
which the fish, marine mammals, or vegetables were collected was treated with ACS grade sulphuric acid (75 g silica gel: 50 g H 2 SO 4 )
not available. Some supplements contained fish oil mixtures, but (EM Science) and topped with anhydrous sodium sulfate. Prior to
species types were not identified (n = 3) and 2 samples were mixed adding a sample to the column bed, 4 × 5 mL volumes of hexane
with unspecified vegetable oils. were used to condition the column. After the samples were quanti-
tatively transferred to the silica column, the sample flask was rinsed
Chemicals and materials with 3 × 5 mL volumes of hexane and added to the top of the
All solvents (acetone, cyclohexane, dichloromethane [DCM], column. Individual columns were then eluted with 50 mL hexane
hexane, nonane, and toluene) used in sample and standard prepa- and the eluate was taken down to approximately 1 mL using rotary
ration were distilled in glass grade (Omnisolve, EM Science, Gibb- evaporation.
stown, N.J., U.S.A.). Prior to use, glass wool and glassware were Sample extracts were cleaned up further on 5 mL serological
rinsed with acetone and hexane. Florisil (60 to 100 mesh) (Fisher pipettes filled with activated Florisil (1.5 g) and topped with sodium
Scientific, Hampton, N.H., U.S.A.) was activated at 300 ◦ C for 7 h sulfate. The columns were preconditioned with 2 × 5 mL DCM fol-
and silica gel (100 to 200 mesh) was supplied by Sigma-Aldrich lowed by 2 × 5 mL hexane. Samples were quantitatively transferred
(Oakville, ON, Canada). Activated carbon (Carbopack C) was pur- to the top of the column bed and washed onto the column with
chased from Supelco (Oakville, ON, Canada), while celite was sup- 4 × 1 mL hexane and the eluate discarded. The sample flasks were

Table 1 --- Range of PCB concentrations [median] (ng/g) in oil supplements by type.
Type n Maximum recommended dosage (g) PCBsa Marker PCBsb
No identification 3 3 to 6 5.84 to 40.9 [34.5] 2.57 to 18.9
Mixed (no salmon) 8 1.2 to 3 0.711 to 37.9 [24.2] 0.227 to 14.4
Mixed (including salmon) 6 3 to 6 19.3 to 26.5 [25.1] 8.88 to 12.3
Salmon 7 2 to 6 36.1 to 170 [95.3] 12.7 to 54.8
Vegetable and mixed 2 1.2 to 2.7 7.70 to 16.3 [12.0] 3.30 to 7.63
Shark 2 1.5 81.0 to 10400 [5260] 38.6 to 5080
Menhaden 1 3 321 104
Seal 1 3 519 295
Chemical Food Safety

a
 of PCB 1, 3, 4/10, 6, 8, 19, 18, 15, 16, 54, 31, 28, 33, 22, 52, 49, 104, 44, 37, 41, 40, 74, 70, 66, 95, 155, 60, 84/90/101, 99, 119, 97, 87, 81, 85, 110, 77, 151,
T: Toxicology &

135, 123, 149, 118, 114, 188, 153, 168, 105, 141, 137, 138, 158, 178, 129, 126, 187, 183, 167, 128, 174, 177, 202, 171, 156, 157, 201, 180, 193, 191, 200, 169,
170, 199, 203, 189, 208, 207, 194, 205, 206, 209.
b
Marker PCBs: 28, 52, 101, 118, 138, 153, 180.

Vol. 74, Nr. 1, 2008—JOURNAL OF FOOD SCIENCE T15


PCB, OCs in fish oil dietary supplements . . .

then rinsed 3 times with 4 mL DCM, which was then added to the The oil supplements tested in this study were found to have
top of the column bed, and the eluate was collected in a 15-mL cen- 100% lipid and, therefore, whole or wet weight was considered
trifuge tube. This fraction, containing organochlorines and most equivalent to lipid weight for these samples.
PCBs, was concentrated using gentle blowing with ultra-high pu- Mean, median, and standard deviation values were calculated
rity nitrogen using 200 μL nonane as a keeper. These extracts were using Microsoft Excel (2002; Redmond, Wash., U.S.A.). Correlations
reconstituted in approximately 1 mL hexane and cleaned up on a were determined using the Mann–Whitney Rank Sum Test with
2nd Florisil column as previously mentioned. SigmaStat for Windows version 3.11 (2004; San Jose, Calif., U.S.A.).
This fraction was then evaporated, as before, to 200 μL using
nonane as a keeper and then transferred to 700 μL autosampler Results and Discussion
vials with 2 × 200 μL DCM and evaporated to near dryness, but the
extracts were never allowed to go to complete dryness. Finally, the Concentrations
extracts were reconstituted in 25 μL of recovery standard contain- PCBs and OC insecticides were detected in all supplement sam-
ing 13 C PCB 9, 37, 79, 111, 162, 194, and 206. ples collected. Lowest PCB concentrations (0.711 ng/g) were ob-
served in a supplement that was comprised more than 1 fish oil
Analysis but had no salmon or vegetable content. In contrast, the highest
Both PCBs and OC compounds were analyzed using a Waters PCB levels (10400 ng/g) were observed in a supplement identi-
Autospec Premier high-resolution mass spectrometer (Manchester, fied as containing shark oil (Figure 1). Although this 1 shark sample
U.K.) linked to an Agilent 6890 gas chromatograph (GC) (Palo Alto, had PCB concentrations exceeding 10000 ng/g, total PCBs in the
Calif., U.S.A.) equipped with a splitless injection system. The col- 2nd shark oil supplement tested was 81 ng/g. The PCB concen-
umn used for the GC separation was a fused silica DB-5 60 m × tration observed in the 2nd sample more closely reflects the results
0.25 mm × 0.25 μm (J & W Scientific, Folsom, Calif., U.S.A.) with a reported by other researchers where PCBs in shark liver oils ranged
1 m × 0.53 mm (J & W Scientific) retention gap. The injector tem- in concentration from 16 to 340 ng/g (Akutsu and others 2006).
perature was set to 300 ◦ C for all analyses, with a purge time of The production differences in the 2 shark samples are expected to
1.5 min. be minimal because they were marketed by the same company. The
The initial oven temperature for the PCB analyses was 80 ◦ C and 2 samples, however, were from different lots and, therefore, are ex-
held for 1.5 min, raised to 200 ◦ C at 30 ◦ C/min, followed by an in- pected to have been prepared using different sharks. Differences in
crease to 280 ◦ C at 5 ◦ C/min, and held for 3 min. The oven tem- shark species, gender, geographical region, and season of collection
perature for the OC compounds was initially set to 80 ◦ C and held contribute to a wide variability in POP levels.
for 1.5 min, raised at a rate of 30 ◦ C/min to 200 ◦ C, followed im- In a limited sample (n = 6) of fish oil supplements available
mediately by a 2nd increase in temperature to 280 ◦ C at a rate of on the Swiss market, total PCBs (reported as PCB congeners 28,
5 ◦ C/min, which was maintained for 3 min before the final temper- 52, 101, 138, 153, and 180) ranged from 0.23 to 17 ng/g (Zennegg
ature increase of 15 ◦ C/min to 300 ◦ C where it remained for 9 min, and Schmid 2006). In comparison, the sum of marker PCB con-
which completed the analytical run. geners (PCB 28, 52, 101, 118, 138, 153, 180) from the present sur-
The electron energy was set to 37 eV, with a photomultiplier volt- vey of fish oil containing supplements, exclusive of the menhaden,
age of 350 V. The trap current was 650 μA and both the source seal, and shark oils, ranged from 0.227 to 54.8 ng/g, while results
and capillary line temperatures were maintained at 260 ◦ C. The from a survey of fish oil supplements collected in the United King-
re-entrant temperature was 270 ◦ C and perfluorokerosene-H (PFK) dom (n = 33) reported marker PCB concentrations of only 0.008 to
was used as the reference substance for tuning at 393 m/z. The mass 0.267 ng/g (mean value 0.098 ng/g) (Fernandes and others 2006).
resolution was set to 10000 for all analyses. Shim and others (2003) reported mean total PCB concentrations in
26 oil supplement samples, 24 containing fish oils and 2 comprising
Quality assurance algae oils, with concentrations ranging from below detection lim-
The recovery of the 13 C surrogate analogues was determined its to 276 ng/g. Although the present study resulted in detectable
for each sample and the average recovery of surrogate standards levels of PCBs in all samples, no algae or pure vegetable-based
ranged from 22% for PCB 209 to 92% for PCB 189. In addition to 13 C supplement samples were tested, limiting the comparison. PCB
PCB 209, 13 C PCB 155 had average recoveries of <50% (42%). Aver- concentrations in the fish oil supplements in the present study,
age recoveries for the OC surrogates ranged from 30% to 102% for however, were found to be similar to those reported by Shim and
mirex and p,p -DDT, respectively. The average recoveries of the 13 C others (2003) (Table 1).
analogues of both 1,2,3,4 tetrachlorobenzene and pentachloroben- Maximum OC concentrations frequently were observed in the
zene were low (40% and 45%, respectively). Analytes were corrected single seal oil supplement analyzed relative to most other oil types
for surrogate recoveries. tested. The shark oil sample that had very high PCB concentrations,
A reagent blank and cod liver oil certified reference mate- however, also had the highest concentration of DDT (sum of p,p
rial (Natl. Inst. for Standards and Technology, Gaithersburg, Md., DDT and p,p -DDE) (3310 ng/g) and mirex (10 ng/g) of all supple-
U.S.A.) was processed and analyzed with each set of samples pre- ments. Although residue data in seal tissue are available in the sci-
pared for PCB and OC analysis. Because PCB and OC concentra- entific literature (Schantz and others 1993; Tanabe and others 1994;
tions in blank samples were very low relative to oil supplement Vorkamp and others 2008), data in seal oil supplements are scarce.
samples, concentrations were not corrected for the level in blank Median PCB concentrations, determined by oil type ranged
samples. Analytes were present in the acceptable range based on from 12 ng/g in vegetable and mixed fish oils to 5260 ng/g in
certified concentrations. shark oils. With the exception of the menhaden, seal, and shark
The method detection limits (MDL) were established based on oil supplements, all median PCB concentrations were below
a 3:1 signal to baseline noise ratio and are reported as averages of 100 ng/g (Table 1). Owing to the limited number of samples from
Chemical Food Safety

individual chromatograms, ranging from 1.39 to 8.61 pg/g and 2.52 these supplement categories, the data observed in this study may
T: Toxicology &

to 9.28 pg/g for PCBs (104 and 40) and OC insecticides (HCB and not accurately reflect the concentrations in oils of this type in
p,p -DDT) analyzed in this study, respectively. general.

T16 JOURNAL OF FOOD SCIENCE—Vol. 74, Nr. 1, 2008


PCB, OCs in fish oil dietary supplements . . .

Levels of PCBs in salmon oil supplements ranged from 36.1 to oil sample found to have very high PCB residues was also found
170 ng/g (Table 1) where 3 or approximately half of the samples to have extremely high levels of DDE although the maximum con-
tested had concentrations exceeding 100 ng/g. PCB concentrations centration of most OC insecticides were observed in the seal oil
observed in supplements prepared using salmon oil were consis- analyzed (Table 2). The supplements containing seal, shark, and
tent with the levels reported in salmon tissue samples from the salmon oils had elevated levels of OC compounds relative to those
Canadian market in 2002 (Rawn and others 2006). PCB concen- containing other fish and vegetable oils (Table 2).
trations in the salmon oils from the present study are lower than
reported in a pharmaceutical grade salmon oil collected from the Trends
United Kingdom (Jacobs and others 1998). Marker PCBs were de- In general, the hexachlorinated congeners contributed the great-
tected in salmon oils in the present study and ranged from 12.7 est extent to total PCB levels, followed by the pentachlorinated and
to 54.8 ng/g, which contrasts with the salmon oil originating from heptachlorinated congeners (Figure 2). Although the concentra-
Norway/the United States reported by Jacobs and others (2004), tions were high in shark oil, the congener profile in these samples
where PCBs were below detection limits. was consistent with other oil types. Jacobs and others (2004) also
Reported marker PCBs (92 ng/g) in a menhaden fish oil sup- found the hexachlorinated congeners to be the dominant contrib-
plement tested (Santillo 2007) were similar to the concentration utors to total PCB levels in fish oil supplements.
observed in the present study (104 ng/g). The menhaden oil In contrast to the observations of Jacobs and others (2002),
supplement tested in the present study had residues greater than β-HCH was the predominant HCH isomer (mean ratio β-
those obtained in supplements containing anchovy, mackerel, sar- HCH:HCH = 0.643 ± 0.267) in the oil supplements in the present
dine, and salmon oils, however, the maximum concentrations were study. DDE was the predominant contributor to total DDT in both
observed in seal and shark supplements. Only the PCB concen- the present study and the study reported by Jacobs and others
trations in the menhaden, seal, and 1 shark oil sample would ex- (2002). The DDE:DDT ratio was determined to be 0.866 ± 0.145
ceed the U.S. Council for Responsible Nutrition’s recommended in the present study.
PCB standard for supplements containing fish oil (90 ng/g) based A strong correlation between PCB and DDT concentrations
on marker PCB concentrations (Council for Responsible Nutrition in these supplement samples was found to occur (r 2 = 0.988), how-
2006). ever, this was not the case for the other OC compounds. Jacobs
Similar to PCBs, OC levels in oil supplement samples varied and others (2004) similarly found a correlation between PCB and
widely between supplement types. Although individual contribu- DDT concentrations in oil supplements. Although a weak cor-
tors to HCH (for example, α-HCH, γ -HCH) and chlordane (for relation between total chlordane levels and PCBs was observed
example, oxychlordane) were below detection limits in a few sam- (r 2 = 0.223), the correlations between PCB concentrations and
ples, only 1 mixed fish oil sample, with no salmon content, was the other OC compounds analyzed were not found to be significant,
found to have nondetectable residues of HCH (Table 2). Mirex with r 2 values < 0.07.
also was below method detection limits in this sample, but was de- Owing to the limited number of supplements containing simi-
tected in all other samples tested in the present study. The shark lar types of oil in the present study, direct comparisons between

Figure 1 --- Total PCB concentrations


in oil supplement samples grouped
by oil type (veg = vegetable).

Chemical Food Safety


T: Toxicology &

Vol. 74, Nr. 1, 2008—JOURNAL OF FOOD SCIENCE T17


PCB, OCs in fish oil dietary supplements . . .

the levels of PCBs and OC insecticides in 1 supplement type gle 150 g meal of farmed salmon with an average PCB concentra-
relative to another were not possible. PCB and OC concentrations tion of 17.5 ng/g would result in exposure to 2630 ng PCBs. Of the
in salmon oil (n = 6) supplements, however, were compared to OC insecticide related compounds, the highest mean intake was
the levels observed in all mixed fish oil supplements, where sam- estimated for DDT (304 ng/d) and mirex intake was calculated
ples containing any mixtures of anchovy, mackerel, sardine, veg- to be the lowest (1.58 ng/d) (Table 3). The intake estimates deter-
etable, and salmon oil were included in the category (n = 16) for mined in the present study generally are quite similar to those re-
these comparisons. PCB and OC insecticide levels were statistically ported in cod liver oil supplements (Storelli and others 2004). Total
significantly lower in mixed fish oils relative to salmon oils (PCB PCB intakes reported by Storelli and others (2004) ranged from 4 to
P < 0.001, HCB, mirex, chlorobenzenes, HCH, chlordanes, DDT; 2000 ng/d in individual cod liver oils, while DDT intakes ranged
P < 0.001, P < 0.001, P < 0.001, P < 0.001, P < 0.001, P = 0.035) from 4 to 1240 ng/d. Mean intakes determined in the present
in the present study. study are within the values reported by Storelli and others (2004)
(Table 3).
Intakes
Daily intake estimates were calculated by multiplying the con- Conclusions
centration of contaminant in each supplement with the maximum
recommended daily dosage following label directions. Total PCB in-
takes ranged between 0.896 ng/d (0.285 ng/d marker PCBs) and
C onsumption of shark, seal, and menhaden oil supplements
would contribute more to PCB intake than other oil types,
based on the results of this study. Seal oil consumption, however,
15700 ng/d (7620 ng/d marker PCBs), in a supplement contain- would result in increased exposure to most OC insecticides an-
ing anchovy, mackerel, and sardines and a shark oil supplement, alyzed, with the exception of DDT and mirex. The mixed fish
respectively. The seal oil supplement resulted in the next highest oils tested in the present study had lower PCB and OC insecticide
intake estimate (1560 ng/d). In comparison, consumption of a sin- levels than other oil types. Although a limited number of

Table 2 --- Range of organochlorine concentrations [median] (ng/g) in oil supplements by type.
Category CBza HCHb HCB Chlordanec DDTd Mirex
No identification 0.062 to 0.081 0.011 to 0.571 0.023 to 1.07 0.042 to 2.43 0.301 to 13.5 0.052 to 0.092
[0.067] [0.065] [0.088] [0.252] [4.23] [0.066]
Mixed (no salmon) 0.021 to 0.103 ND to 0.839 0.021 to 0.628 0.011 to 0.654 0.189 to 15.2 ND to 0.044
[0.030] [0.396] [0.217] [0.342] [10.6] [0.024]
Mixed (including salmon) 0.037 to 0.796 0.752 to 1.77 0.361 to 2.71 0.500 to 2.29 9.31 to 24.9 0.020 to 0.511
[0.047] [0.836] [0.597] [0.636] [11.1] [0.042]
Salmon 0.177 to 2.83 1.37 to 36.9 1.55 to 21.9 3.51 to 84.7 4.76 to 250 0.099 to 3.53
[2.19] [29.7] [15.3] [22.9] [59.2] [0.618]
Vegetable and mixed 0.106 to 0.307 0.448 to 1.57 0.174 to 1.22 0.224 to 0.958 3.71 to 5.63 0.029 to 0.069
[0.206] [1.01] [0.697] [0.591] [4.67] [0.049]
Shark 0.058 to 0.180 0.052 to 0.101 2.52 to 3.40 5.92 to 121 309 to 3310 3.40 to 10.0
[0.119] [0.077] [2.96] [63.4] [1810] [6.72]
Menhaden 0.028 0.153 0.054 9.14 28.9 0.309
Seal 9.84 79.0 52.1 211 267 1.27
a
of 1,2,3,4 tetrachlorobenzene, 1,2,3,5 tetrachlorobenzene, and pentachlorobenzene.
b
of α-HCH, β-HCH, and γ -HCH.
c
of oxychlordane, trans-chlordane, trans-nonachlor, and cis-nonachlor.
d
 of p,p -DDT and p,p -DDE.

Figure 2 --- Relative contribution of


each homologue group to total PCBs
by oil type (veg = vegetable).
Chemical Food Safety
T: Toxicology &

T18 JOURNAL OF FOOD SCIENCE—Vol. 74, Nr. 1, 2008


PCB, OCs in fish oil dietary supplements . . .

Table 3 --- Intake estimates following maximum suggested Health Canada. 2007b. Fish and Seafood Survey 2002. Updated 26 March
dosage and contaminant concentration (ng/d). 2007 [Internet]. Available from: http://www.hc-sc.gc.ca/fn-an/securit/chem-
chim/mercur/servey sondage e.html. Accessed Jan 28, 2008.
Compound Range Average ± SD Hilbert G, Lillemark L, Balchen S, Højskov S. 1998. Reduction of organochlorine con-
taminants from fish oil during refining. Chemosphere 37(7):1241–52.
PCB 0.896 to 15,600 736 ± 2840 Hites RA, Foran JA, Carpenter DO, Hamilton MC, Knuth BA, Schwger SJ. 2004. Global
Marker PCB 0.285 to 7620 345 ± 1380 assessment of organic contaminants in farmed salmon. Science 303(5655):226–9.
DDT 0.265 to 4970 304 ± 948 Jacobs MN, Santillo D, Johnston PA, Wyatt CL, French MC. 1998. Organochlorine
residues in fish oil dietary supplements: comparison with industrial grade oils.
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Chemical Food Safety


T: Toxicology &

Vol. 74, Nr. 1, 2008—JOURNAL OF FOOD SCIENCE T19

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