5
Chapter 2
Sources and Pathways of Persistent Organic Pollutants
ญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญ
The previous AMAP assessment summarized the path-
(crustaceans, fish, marine mammals) and migratory birds,
ways of pollutants in general (Gregor et al., 1998), and
animals that migrate in large groups throughout differ-
POPs (de March et al., 1998) specifically, as they were
ent climate zones into the Arctic. These organisms can
understood in the mid-1990s. Recent reviews have up-
transfer the pollutants into higher-level organisms via
dated this information (Macdonald et al., 2000; 2003).
the Arctic food web.
The general principles are briefly described in the fol-
In general, present levels of most POPs cannot be re-
lowing sections and the reader is referred to the above
lated to known potential sources within the Arctic, and
reviews for more details. In addition we also consider a
can therefore only be explained by long-range transport
novel pathway, biotic transport.
from lower latitudes (Hansen et al., 1996; de March et
al., 1998; Macdonald et al., 2000). However, there are
sources of POPs within the Arctic that have local and
2.1. Pathways
possibly regional significance but are minor contributors
For pristine regions like the Arctic, generally four possi-
from a circumpolar perspective. These include PCB
ble pathways exist for the transport of POPs (Figure
emissions from military bases, harbors, and landfills, as
2ท1). The atmosphere, ocean currents, transpolar ice pack,
well as PCDD/Fs and PAHs from smelters located in
and large Arctic rivers (Ob, Pechora, Yenisey, Lena,
high latitudes (Section 2.3.2). Owing to increasing activ-
Mackenzie) are the main transport routes by which per-
ities related to exploration and production of oil and
sistent organics enter Arctic ecosystems. The relative im-
gas, especially in the Russian and Norwegian Arctic, pe-
portance of each pathway depends on the chemical and
troleum hydrocarbon releases are a potential local source
physical properties of the substance and its emissions in
of pollution for PAHs in ocean waters and sediments
the source region, which may vary over time. In addition
(Robertson, 1998; Hansen et al., 1996). A future AMAP
to the above mentioned transport routes, POPs may also
assessment of petroleum hydrocarbons will consider this
be transported into the Arctic via pelagic organisms
particular source in more detail.
Catchment area
ea
for Hudson B
on Bay, Baffin Bay,
on Bay
B
and adja
djacent seas
dja
ea
nt
rre
u
Ala s ka C
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Kolyma
Ko
o
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ac enz
T
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In
nd gi
g
a
rans
Lena
Len
na
po
Beaufort
Beaufo
u
l
a
r
Gyre
G
D
Khatanga
Khatang
Khata
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Khata
t
ata
Khata
K
an
an
a
a
nga
r
ift
Yenisey
Yen
e
ey
O
Ob
b
.Cd
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Pechora
Pe
ech
Pech
e
echora
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urrent
la
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pe
o
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a
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rab
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atch
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a
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ct
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for
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and
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nt seas
nt
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and
and
d
d
nd
t
ent
North Atlantic Current
Figure 2ท1. Illustration of the different physical path-
ways by which POPs enter the Arctic. Transport into,
and within, the Arctic occurs via air currents, ocean
currents, rivers, and transpolar ice movements.
Pacific currents
Atlantic currents
River outflow
Wind flow
Other currents

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6
AMAP Assessment 2002: Persistent Organic Pollutants in the Arctic
2.1.1. Atmospheric transport
2.1.1.2. Light conditions
and deposition of POPs
The polar night at 80ฐ northern latitude lasts from Oc-
2.1.1.1. Meteorological conditions
tober until March and then changes into the midnight
Under favorable meteorological conditions, rapid air
sun period. These special seasonal light conditions have
transport can take place in a few days or weeks, from
tremendous effects on the photochemical reactivity and
the source regions into the Arctic. Almost twenty years
degradation of some persistent pollutants. Lack of pho-
ago, it was postulated that the global dispersion of
tochemical degradation processes may be the main rea-
semivolatile POPs occurred mainly via the atmosphere
son why long-range transport of highly- and semivolatile
and was dependent on their vapour pressures (Ottar,
organic compounds such as 2- and 3-ring PAHs is
1981). Today, this is well documented and models de-
mainly observed during the winter. Photochemical pro-
veloped show that atmospheric transport is probably
cesses during the 24-hour summer light period may
the most important long-range transfer route for these
quickly degrade chemicals that react rapidly with OH
compounds (Wania and Mackay, 1993; Strand and
radicals or degrade by direct UV photolysis. In winter,
Hov, 1996; Wania and Mackay, 1996; Wania et al.,
on the other hand, air concentrations of these types of
1999a).
compounds are usually elevated by one or two orders of
In winter, the lower tropospheric circulation is
magnitude. Indications of a seasonally dependent photo-
dominated by high pressures over the continents and
chemical degradation were also found for the persistent
low pressures over the northern Pacific (Aleutian Low)
pesticide trans-chlordane. Seasonal shifts in the chlor-
and Atlantic Oceans (Icelandic Low). The Siberian
dane patterns have been found during year-round ambi-
High tends to force air on its western side into the
ent air sampling campaigns at Ny-ลlesund (Svalbard,
Arctic acting as an effective atmospheric conduit from
Norway) and at Alert (Ellesmere Island, Canada)
industrialized regions of Siberia and eastern Europe
(Oehme, 1991; Halsall et al., 1998).
into the high Arctic ( Figure 2ท1 ). The high-pressure
ridge over North America then forces air southward
2.1.1.3. Precipitation inputs of POPs
giving a net transport out of Eurasia into the Arctic,
across the Arctic and south over North America. The
Precipitation is a key factor in contaminant transport.
Icelandic Low produces westerly winds over the east-
Rain and snow scavenge aerosols and gasses from the at-
ern North Atlantic and southerly winds over the Nor-
mosphere and deposit them at the Earth's surface (Gre-
wegian Sea providing a conduit for airborne contami-
gor et al., 1998; Macdonald et al., 2000). Scavenging by
nants from eastern North America and Europe to reach
precipitation may be relatively weak in the desert-like
the Arctic rapidly. Finally, the Aleutian Low tends to
conditions of the High Arctic. For example, mean pre-
steer air that has crossed the Pacific from Asia up into
cipitation for the Arctic Ocean is estimated at about
Alaska, the Yukon, and the Bering Sea (Bailey et al.,
25.2 cm/yr and evaporation is about 13.6 cm/yr for a net
2000; Li et al., 2002; Wilkening et al., 2000). During
moisture flux to the ground of 11.9 cm/yr (Barry and
winter, these three routes into the Arctic ญ southerlies
Serreze, 2000). Precipitation over land in the Arctic
in the Norwegian Sea (40%), Eastern Europe/Siberia
drainage basins is greater, with the runoff yield (precipi-
(15%), and Bering Sea (25%) account for about 80%
tation minus evaporation) being estimated at 21.2 cm/yr
of the annual south to north air transport (Iversen,
from the network of gauged discharge by rivers (Lam-
1996). Thus during winter, the polar front expands
mers et al., 2001).
into an area encompassing southern regions of the
Due to the low annual average temperature, snow is
northern hemisphere into central Europe, central U.S.,
the dominant form of precipitation in the Arctic. The in-
Asia, the European part of Russia, Belarus, and the
fluence of snow and ice on the fate and airญsurface ex-
Ukraine. Eighty percent of the main source areas for
change of organic contaminants has been reviewed by
persistent pollutants are situated in these regions.
Franz et al. (1997) and Wania et al. (1998). Wania et al.
Therefore, during the winter season, the polar front is
(1999b) demonstrated that falling snow serves as an ex-
not limiting the atmospheric transport from these
tremely efficient scavenger of both vapour and particulate
sources into the Arctic region.
phase compounds, with vapour scavenging of lower chlo-
Summer pressure fields and air-flow patterns are
rinated PCBs and 2- and 3-ring PAHs being a predomi-
markedly different from those of winter. In summer,
nant process. Also the waterญair partition coefficient
the continental high-pressure cells disappear and the
and the iceญair sorption coefficient increase at low tem-
oceanic low-pressure cells weaken with the result that
peratures thus increasing the potential for vapour scav-
northward transport from low latitudes weakens. Dur-
enging (Wania et al., 1999b). In addition, a snow crystal
ing summer, the polar front is situated far north
possesses a large surface area and adsorbs particles and
and creates a meteorological barrier often difficult to
contaminants to its crystalline surface more efficiently
penetrate for air masses transported from southern
than a water droplet (Franz and Eisenreich, 1998).
regions. According to Iversen (1996), summer ac-
Therefore snow precipitation transports contaminants
counts for only 20% of the annual south to north air
more efficiently to the ground (soil, water surface) than
transport (southerlies in the Norwegian Sea (10%),
rain droplets. In contrast to rainwater, the surface prop-
eastern Europe/Siberia (5%), and Bering Sea (5%)).
erties of snow crystals change during aging after deposi-
Prevailing winds provide a means to transport contam-
tion. The surface of a snow crystal diminishes dramati-
inants from industrialized North America and Europe
cally after a short time on the ground because of the over-
to the North Atlantic but penetration into the Arctic
all pressure of the surrounding snow, and the weather and
weakens.
climate conditions during the ageing process. Thus, due

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Chapter 2 ท Sources and Pathways of Persistent Organic Pollutants
7
to surface reduction, the adsorbed contaminants are ei-
HCH isomers (Li et al., 2002). However, some degrada-
ther released into the ground, stay adsorbed to the snow
tion does occur in seawater. For example, - and -
crystal, or are re-evaporated into the atmosphere. These
HCH have recently been shown to undergo biotransfor-
three possibilities are dependent on the vapour pressure
mation in Arctic seawater with half-lives estimated to be
of the respective contaminant and the ambient climatic
19 years for -HCH and 5.9 years for the + enantiomer
conditions. Therefore, high POP levels can often be
of -HCH (Harner et al., 1999).
found in upper layers containing new snow surface
Prolonged half-lives in abiotic compartments, com-
whereas in aged snow, situated near the ground, the con-
bined with efficient biomagnification and bioaccumula-
taminants are already released into the soil.
tion in the Arctic food web due to lipophilicity and
resistance to biological degradation, give rise to high
concentrations of the long-range transported POPs in
2.1.1.4. Seaญair gas exchange
the higher trophic levels of the Arctic ecosystem, includ-
Gas absorption and volatilization of POPs are important
ing indigenous people.
pathways of deposition and removal in the Arctic
The low annual average temperature of the Arctic is
Ocean. Evaluation of relative fugacities of PCBs and
the main reason why microbiological degradation of or-
toxaphene in air and seawater, based on measurements
ganic material slows to a minimum, especially in terres-
in the mid-1990s, indicated that these compounds are
trial and freshwater environments. This potentially ex-
still loading into the Arctic Ocean via the atmosphere,
tends the half-lives of many compounds in the Arctic
while -HCH is volatilizing (Macdonald et al., 2000).
relative to temperate regions.
Verification of the seaญair exchange process for -HCH
was accomplished using the distribution of the enan-
2.1.3. Riverine inputs and sea-ice transport
tiomers of this chiral pollutant as indicators (Falconer et
al., 1995; Jantunen and Bidleman, 1996; Jantunen and
Riverine input is considered to be another important
Bidleman, 1997). Enantiomeric ratios (ER) found in sur-
source of contaminants to the Arctic Ocean (Barrie et
face water and in high-volume ambient air samples were
al., 1992; Pavlov and Pfirman, 1994; de March et al.,
similar, implying a seawater source. A significant devia-
1998; Gregor et al., 1998) and can be considered as an
tion from the racemic distribution (ER = 1) in environ-
important circumpolar source draining environmental
mental samples was also found. This deviation can only
pollutants into the Arctic Basin. Particles transported to
occur when biochemical transformation (microbiologi-
the coast by large Russian Arctic rivers (e.g., Yenisey,
cal or in higher organisms) takes place. Therefore, the
Ob, Lena, and Pechora) during the melting period are
authors concluded that -HCH found in the ambient air
contaminated with pollutants originating in the indus-
had been subject to earlier microbiological degradation
trial areas of the northern Urals and western Siberia. As
in the water column before being re-evaporated into the
a result of various physical processes, the particles are
atmosphere. This finding represents the first evidence for
incorporated in the coastal ice which may then carry
waterญair gas exchange of -HCH using an experimen-
large loads of contaminated sediments.
tal approach.
The general movement of sea ice from the coast of
the Kara Sea is northward to join the Siberian branch of
the Transpolar Drift between the Franz Josef Land and
2.1.2. Ocean transport
Severnaya Zemlya archipelagos. Ice-bound particles
POPs are also transported by ocean currents. Ocean cir-
with possible contaminants may thus be carried out of
culation is driven by a combination of various forces
the area and released in the main ice-melting areas east
and a particular force (e.g., tidal forces, wind stress,
of Svalbard and in the Fram Strait (Figure 2ท1). It is esti-
mixing of water masses) may dominate in a particular
mated that ice-rafted material forms up to 80% of the
area. Within the Arctic Ocean, the main surface circula-
sediment on the ridges and upper slopes in the central
tion features are the clockwise circulation of the Beau-
Arctic Ocean (Darby et al., 1989).
fort Gyre and the Transpolar Drift, which flows from
Siberia (Russia), across the pole, and then southward,
2.1.4. Biotic transport
exiting as the East Greenland Current (Gregor et al.,
1998; Macdonald et al., 2003). The major current sys-
Transport of pollutants, particularly POPs in migratory
tems whereby water is exchanged between the Arctic
animals may also be a significant pathway in the Arctic,
Ocean and other oceans, are found in Fram Strait. For
where many important species such as seabirds, ceta-
example, the West Spitsbergen Current flows northward
ceans (beluga, bowhead whales, minke whales), pinni-
off the west coast of Spitsbergen (Svalbard, Norway),
peds (harp seals), salmon, and Atlantic cod are migra-
transporting Atlantic water from the Norwegian Sea
tory. Some animals cover long distances, often crossing
into the Arctic Ocean (Gregor et al., 1998). The trans-
international boundaries and linking industrialized/agri-
port via sea currents, however, may take years. Studies
cultural and remote regions during their migration.
of the transport of radioactive isotopes released from the
Some species can be important prey of resident Arctic
nuclear power plant in Sellafield (U.K.) indicates a four
animals, for example, Barents Sea harp seals consumed
to five year transport over the 2200 km from southern
by polar bear in eastern Svalbard and Franz Josef Land.
Norway to northern Spitsbergen (Svalbard). Neverthe-
A unique example is salmon entering Alaskan rivers to
less, ocean transport is important for POPs with low
spawn and die. Ewald et al. (1998) described the entry
HLCs such as -HCH, which is selectively removed
of PCBs and DDT into the grayling population of the
from the air by precipitation-scavenging as it heads
Copper River in Alaska by migrating sockeye salmon.
northward and is enriched in seawater relative to other
The grayling in a salmon spawning lake had contami-

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8
AMAP Assessment 2002: Persistent Organic Pollutants in the Arctic
nant concentrations more than double those found in
fluxes in migrating birds are much lower for PCBs, DDT
grayling from a nearby, but salmon-free lake.
or HCH than the transport rates in the physical media.
Wania (1998) estimated that the amount of POPs
The importance of biological transport media obviously
transferred in and out of the Arctic via seabirds migrat-
increases with decreasing volatility and water solubility,
ing annually from the Canadian Arctic to northwest At-
and with increasing bioaccumulation potential of a
lantic waters was in the range of grams to kilograms per
chemical.
year based on the fact that the populations involved are
Ewald et al. (1998) pointed out that the pollutants in
in the hundred thousands to millions of birds. Seabirds
biological transport media are more readily available for
also leave behind guano which may contain significant
bioaccumulation than those in abiotic media. In the case
quantities of persistent OC contaminants. Evenset et al.,
of the investigated Alaska freshwater system, they point
(2002) have shown that elevated PCBs and other OCs
out that the `migrating salmon, the salmon roe, and the
in fish and sediments from Lake Ellasj๘en on Bj๘rn๘ya
carcasses are fed upon directly by predators such as bald
(74ฐ30'N, 19ฐE) are due to seabird guano (see Section
eagles, bears, and grayling, allowing the pollutants to be
4.3.5). The seabirds at Bj๘rn๘ya are functioning as a
transferred to biota in a direct and efficient way'. Simi-
transport link for POPs from the marine ecosystem to
larly, the studies on migrating salmonids in the Great
the freshwater ecosystem.
Lakes (Scrudato and McDowell, 1989) concluded that
While many Arctic whales migrate regionally within
resident fish in salmon-accessible tributaries derived their
the Arctic, the Eastern Pacific stock of gray whales (Es-
excess pollutant load by directly ingesting the contami-
chrichtius robustus) spends the summer in the Bering
nated salmon eggs. Ewald et al. (1998) even suggested
and Chukchi Seas, and the winter off the Pacific coast of
that biotransport may provide a transport mode for
Mexico and California (Baker, 1978). Relatively reliable
POPs, whose physical chemical properties prevent them
population estimates and recent contaminant concentra-
from long-range transport in atmospheric and water
tions in stranded individuals exist for this stock, allow-
currents (extremely low volatility or water solubility,
ing for an estimate of the amount of some POPs con-
high atmospheric degradability, but resistance to meta-
tained in these whales. Wania (1998) estimated that the
bolic degradation).
total amount of PCBs and DDT contained in the gray
whale population and therefore transported annually
2.2. Modeling transport and distribution
with gray whales is thus in the range of 20 to 150 kg
of POPs in the Arctic
PCBs, and 1 to 40 kg DDT. Of course only animals that
die in the Arctic would leave the contaminants there.
2.2.1. Global fractionation
However, carcasses of dead or hunted whales are scav-
The most widely accepted hypothesis about atmospheric
enged by Arctic fox and polar bears, thereby transfer-
long-range transport and distribution of POPs is `global
ring contaminants from the temperate to the Arctic envi-
fractionation' (Wania and Mackay, 1995; 1996) (Figure
ronment.
2ท2). The `global fractionation hypothesis' explains at-
Considering all migratory whale populations, Wania
mospheric transport as a complex phenomenon depend-
(1998) concluded that the amount of PCBs and DDTs
ing on the physical-chemical properties of the trans-
moved around in these whales is likely of the order of
ported contaminant (e.g., solubility, vapour pressure,
tens of tons per year. Especially for DDTs, these gross
molecule size). The physical-chemical properties of the
fluxes with whales may be comparable to those in air
substance are responsible for the atmospheric transport
and ocean currents. On the other hand, for the more
distance and the subsequent deposition via rain, fog or
water soluble, more volatile, and less bioaccumulative
snow in the water column, sediment or soil. Relatively
HCHs the amounts in organisms are relatively low by
volatile hydrocarbons, characterized by a high vapour
comparison to the mass in the water column. Gross
pressure, are taken directly into the gaseous phase and
High volatility (CFC/HCFC)
Relatively high volatility (HCB/HCH)
Polar region
Relatively low volatility
(DDT)
Temperate region
Low volatility
(B[a]P)
Warm emission area
Figure 2ท2. Schematic representation of
the global fractionation hypothesis and
the revolatilization (ท) or `grasshopper'
effect. From Wania and Mackay (1996).

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Chapter 2 ท Sources and Pathways of Persistent Organic Pollutants
9
immediately transported into the deposition region as
used in an evaluative fashion to understand global trans-
shown for lower chlorinated PCBs (CBs 8-99) and CBz.
port and accumulation processes without the availability
Semivolatile compounds such as lindane ( -HCH) and
of realistic emission scenarios. The first of these uses is
chlordanes as well as some highly chlorinated PCBs
primarily limited by the availability of suitable emission
(CBs 101-153), are distributed between airborne parti-
estimates, which need to be global in spatial scale and
cles and the gaseous phase depending on temperature.
span decades in time. Such estimates only exist for -
These can be washed out via precipitation and tem-
HCH and PCBs at the present time (Section 2.3), and the
porarily deposited in seawater or soil and can absorb to
Globo-POP model has been employed for simulation of
water, plant and soil surfaces from the gaseous phase.
the environmental fate of these two POPs (Section
During favorable warm weather conditions, these com-
4.2.1.4). The model has also been used to identify chem-
pounds evaporate again into the atmosphere and un-
ical property combinations that make a chemical suscep-
dergo further atmospheric transport. This remobiliza-
tible to accumulation in remote polar regions (Wania et
tion is also called the `grasshopper effect'. The role of
al., 2001).
stormy weather situations in remobilization of semi-
volatile compounds into the atmosphere is obvious but
2.2.2.2. Three-dimensional
still scarcely investigated.
global atmospheric transport models
As a consequence of these processes, the levels of the
more volatile POPs, such as HCHs and HCB, are found
Koziol and Pudykiewicz (2001) modeled the global
at comparable or even higher levels in Arctic biota com-
transport of - and -HCHs in 1993 and 1994 on a
pared to areas closer to source regions. However, the
2ฐ
2ฐ grid, using a three-dimensional global atmos-
`global fractionation hypothesis' and the `grasshopper
pheric transport model with high spatial resolution, and
effect' are focused mainly on neutral, persistent organics
compared the measured and modeled air concentrations
transported via the atmosphere. At the present time,
for several Arctic locations. The assumption of constant
therefore, they are less useful for predicting levels of
ocean water concentrations limits the model to fairly
polar and water soluble persistent compounds that may
short time periods. The model also does not include par-
be associated mainly with seawater.
ticle-associated atmospheric transport, which may be
important at the low temperatures of high altitudes and
high latitudes.
2.2.2. Global transport modeling
A different modeling approach to quantifying the
A summary of the various modeling approaches for at-
transport of POPs to the Arctic was used by Commoner
mospheric and oceanic transport of contaminants in the
et al. (2000). Using emission estimates for PCDDs for
Arctic was presented in the previous AMAP assessment
North America, in combination with air mass trajecto-
report (de March et al., 1998). Macdonald et al. (2000)
ries calculated with the HYSPLIT (Hybrid Single-Par-
also described box models of POP distribution and
ticle Lagrangian Integrated Trajectory) air transport
global transport of POPs using numerical models. The
model, they derived sourceญreceptor relationships for
current state of knowledge on modeling the global fate
several communities in the Canadian High Arctic. The
and transport of POPs has recently been reviewed by
model estimated the amount of PCDD emitted by each
Scheringer and Wania (2002).
of 44 000 sources that is deposited at each of eight re-
ceptor sites in Nunavut over a one-year period (1 July
1996-30 June 1997). A fairly limited number of North
2.2.2.1. Global scale box models
American sources outside of Nunavut were found to be
The basic approach for global box modeling is to use
responsible for almost all of the PCDDs deposited on
models that divide the global environment into a series
that territory.
of zonal bands, each of which is described by a series of
well-mixed environmental compartments. This type of
global model has seen further development and use dur-
2.3. Global and circumpolar sources of POPs
ing the past five years. In particular, the global distribu-
including emission inventories
tion model by Wania and Mackay (1993; 1995), has
2.3.1. Historical and current uses
seen further improvement, evaluation, and use, and a
version of that model, named Globo-POP, is now avail-
The previous AMAP assessment report (de March et al.,
able (Wania and Mackay, 2000). A new model of this
1998) gives an overview of sources of POPs in circum-
type was also introduced by Scheringer et al. (2000).
polar countries. Since the preparation and completion of
A detailed example of global modeling of POPs can be
the first assessment report, several regional and global
found in the recent study by Wania et al. (1999a), and
studies have been completed.
Wania and Mackay (1999), on the global chemical fate
One important example is the European emission in-
of -HCH. While -HCH is no longer a significant POP,
ventory of heavy metals and POPs for 1990 that has
the detailed knowledge of its physicalญchemical proper-
gained substantial interest (Berdowski et al., 1997). This
ties and use patterns enabled validation of the model
study was prepared based on submissions of emission
predictions of prevailing and temporal trends of air and
data from the parties to the Oslo-Paris Commission
water concentrations over time, including contamina-
(OSPARCOM), Helsinki Commission (HELCOM) and
tion of the Arctic.
Convention on Long-Range Transboundary Air Pollu-
These global scale box models can be used in two
tion (LRTAP). For the countries where sources and com-
different ways. They can be used to describe the fate of
pounds were lacking in officially submitted data, default
POPs using historical emission estimates, or they can be
emission estimates were prepared to make the inventory

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10
AMAP Assessment 2002: Persistent Organic Pollutants in the Arctic
Table 2ท1. Estimates of the global historical usage or production of selected deliberately produced POPs, by-products, and potential POPs
(thousands of tonnes) (modified after Macdonald et al., 2000). For most chemicals, the major-use areas were, and are at present, the north
temperate regions of Europe, North America, and Asia.
ญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญ
Estimated total
Current
Production
global usage /
annual global
Chemical
Use
period
production (kt)* emissions (kt)**
Reference
ญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญ
Legacy organochlorine pesticides
DDT
Insecticide
1950-present
2600
ญ
Voldner and Li, 1995
Toxaphene
Insecticide
1950-1993
1330
ญ
Voldner and Li, 1995
Technical HCH
Insecticide
1948-1997
10000
ญ
Li, 1999a
Chlordane
Insecticide
1945-1988
78
ญ
Barrie et al., 1992
Aldrin
Insecticide
1950-1992
500
ญ
Barrie et al., 1992
Dieldrin
Insecticide
1950-1992
34
ญ
Barrie et al., 1992
Legacy industrial organochlorines and by-products
PCBs
Various
1930-1992
1320
ญ
Breivik et al., 2002a
CB 28
57
ญ
Breivik et al., 2002a
CB 52
38
ญ
Breivik et al., 2002a
CB 101
31
ญ
Breivik et al., 2002a
CB 138
25
ญ
Breivik et al., 2002a
CB 153
27
ญ
Breivik et al., 2002a
CB 180
14
ญ
Breivik et al., 2002a
By-products
PCDD/Fs (as ITEQs)
By-products
1920-present
ญ
0.8-3.6 10ญ5
UNEP, 1999
Hexachlorobutadiene
Intermediate
1920-present
10
0.002-0.02
Van de Plassche, 2001a;
Environment Canada, 2000
HCB
Pesticide by-product
1920-present
ญ
0.012-0.092
Bailey, 2001
Pentachlorobenzene
By-product and
1920-present
15
0.001-0.005
Environment Canada, 1993
dielectric fluid
Octachlorostyrene
By-product
1920-present
ญ
0.0003-0.001
US EPA, 1999a
Polychlorinated
Flame retardants
1920-1980 (as products) 200-400
ญ
Van de Plassche, 2001b
naphthalenes
and by-products
1920-present
0.01
<1 10 ญ4
Van de Plassche, 2001b
(as by-products)
Currently produced organohalogens ญ potential POPs
Short chain (C10-C13)
Cutting oils and
Tomy et al., 1998;
chlorinated paraffins
flame retardants
1945-present
500-700
50
Muir et al., 2000a
Medium and long chain Flame retardant
1930-present
2000-4000
250
OSPAR, 2000
chlorinated paraffins
plasticizers
(C14-C30)
TeBDE- and PeBDEs
Flame retardants
1960-present
70-120
8.5
BSEF, 2000
Octa- and Deca-
Flame retardant
1980-present
500-800
55
BSEF, 2000
bromodiphenyl ether
Hexabromo-
Flame retardants
1980-present
100-200
16
BSEF, 2000
cyclododecane
Tetrabromobisphenol-A Flame retardants
1990-present
600-1000
121
BSEF, 2000
Perfluoroalkyl Surfactant
and
1950-present
50 ท
?
US EPA, 2000b
sulfonates
flame suppressant
Perfluoroalkanoic acids Surfactant and
1950-present
50 ท
?
US EPA, 2000b
flame suppressant
Current-use pesticides
Lindane
Insecticide
1950- present
720
> 2
Voldner and Li, 1995
Endosulfan
Insecticide
1956- present
57
1-2
Barrie et al., 1992;
USEPA, 2001
Butyltins
Tributyltin
Algicide/fungicide
1960- present
100-500 ท
< 10
Hoch, 2001
Mono- and dibutyltin
Stabilizers
1960- present
200-1000 ท
approx. 35
Hoch, 2001
ญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญ
** Estimated global use (to the late 1990s) as reported or inferred from published reports. Values with ท are rough estimates assuming linear
growth in production over the use period.
** Estimated annual emissions (kilotonnes) include use in consumer products and open applications as a pesticide. Volatilization losses (e.g.,
from treated soils) are not estimated; thus emissions of legacy OC pesticides are not given. Question mark indicates emissions are presently
unknown.

---

Chapter 2 ท Sources and Pathways of Persistent Organic Pollutants
11
complete. One of the major strengths of this study is
lished for the global production and usage of such com-
thus the wide coverage of different priority substances as
pounds. Table 2ท1 presents selected values compiled in a
identified by OSPARCOM and HELCOM. This inven-
recent review (Macdonald et al., 2000) along with up-
tory covered a wide range of deliberately produced and
dated figures for PCBs and `new' chemicals of concern.
accidentally formed POPs and related organic chemicals,
Among the insecticides discussed below, most informa-
including PAHs, PCBs, PCDD/Fs, HCB, several pesti-
tion is available for HCHs (technical HCH and lindane).
cides, and solvent chemicals. Another European emission
The global estimates are described in a series of publica-
inventory was recently presented by Pacyna (1999). This
tions (Voldner and Li, 1995; Li et al., 1996; Li et al.,
study focused on a subset of POPs, notably the PCBs,
1998a; Li, 1999a; 1999b) and were recently utilized to
PCDD/Fs, HCHs, HCB, DDTs, and benzo[a]pyrene
model the global distribution and fate of -HCH (Wania
(B[a]P). One objective of this study was to estimate the
et al., 1999a; Wania and Mackay, 1999).
historical trend in European emissions from 1970 to
1995 and to facilitate an analysis of the environmental
PCBs
response to changes in emissions. As individual constitu-
The estimates in Table 2ท1 account for a reported histor-
ents within groups of compounds (e.g., PCDD/Fs, PCBs,
ical global usage of approximately 1300 kt of PCBs of
HCHs) may behave quite differently in the environment,
which more than 70% have been estimated as TrCBs,
a particular emphasis was on the emissions of individual
TeCBs, and PeCBs. The results further suggest that al-
isomers and congeners (Pacyna, 1999; Breivik et al.,1999).
most 97% of the global historical use of PCBs may have
Similar research efforts have been undertaken at the na-
occurred in the northern hemisphere. Figure 2ท3 shows
tional level to estimate emissions of other POP con-
the estimated cumulative global consumption pattern
stituents. In the United Kingdom, there have been stud-
for total PCBs (Breivik et al., 2002a). Most (approxi-
ies on the national emissions for selected PCBs (Harrad
mately 86%) of the use (and thus emission to air) oc-
et al., 1994) and selected PCDD/Fs (Alcock et al., 2001).
curred in the industrialized, northern temperate lati-
The best possibilities for deriving consistent and reli-
tudes, between 30 - 60ฐN. France, Germany, Italy, Japan,
able source and emission estimates are for the deliber-
Spain, the U.K., and the U.S. were responsible for 68%
ately produced POPs. Several databases have been estab-
of global PCB usage. The latitudinal distribution of
PCB usage,
tonnes /grid cell
0
0.032-1
1-5
5-10
10-50
50-100
100-500
500-1000
> 1000
Figure 2ท3. Use of PCBs in the
northern hemisphere (adapted
from Brevik et al. 2002a). Esti-
mated cumulative global usage
of PCBs with 1ฐ 1ฐ longitude
and latitude resolution.

---

12
AMAP Assessment 2002: Persistent Organic Pollutants in the Arctic
Total PCB usage, kt
PCB concentration in soil, ng/g organic matter
100
250
Circumpolar
PCB usage
region
Soil samples
80
200
60
150
40
100
Figure 2 ท 4. The latitudinal distribu-
tion of global PCB usage and PCBs in
20
50
surface soils from Ockenden et al.
(2002) illustrating the large reservoir
in soils of the north temperate zone
0
0
(45- 60ฐN latitude).
90ฐS
70ฐS
50ฐS
30ฐS
10ฐS
10ฐN
30ฐN
50ฐN
70ฐN
90ฐN
PCBs in surface soils derived from a global survey (Ock-
1970s to early-1980s and in China in 1991. Worldwide,
enden et al., 2002) is shown in Figure 2ท4 along with the
lindane usage between 1948 and 1993 was estimated to
latitudinal distribution of PCB usage.
be 720 kt (Voldner and Li, 1995). Although lindane is
Using the data from the global background soil sur-
still important on a global scale, many countries have re-
vey and information on the latitudinal land surface area
stricted or eliminated its usage. Breivik et al. (1999) give
and soil organic matter content, Ockenden et al. (2002)
the total lindane application in Europe as 81 kt between
estimated that 45 kt of PCBs were present in background
1970 and 1996, and 2.2 kt in 1996. According to Centre
surface (0-5 cm) soils globally. A further burden is pres-
International d'ษtudes du Lindane (CIEL, 1998), the av-
ent in the sub-surface (> 5 cm depth) soils. Adding esti-
erage lindane consumption in Europe was 2.1 kt/yr from
mates of the burden in the sub-surface (5-20 cm; 22.5
1992 to 1997. France was the major user of lindane in
kt) and urban (0.2 kt) soils increases the estimated bur-
Europe and in the world during this period, with an an-
den in soils globally to approximately 67 kt. This is close
nual average consumption of 1.6 kt (CIEL, 1998), more
to recent estimates of the total emissions of PCBs into
than 76% of total lindane usage in Europe. In July 1998,
the environment, of 82-100 kt (Wania, 1999; Axelman
lindane usage was stopped in France (CIEL, 1998). Lin-
and Broman, 2001).
dane use in Sweden, Finland and other countries border-
Russia discontinued production of PCB in 1992 (AMAP,
ing the Baltic Sea, except Russia, was approximately
2000). In a recent Russian inventory, it was found that
0.001 kt in 1995 (HELCOM, 2001). Estimated lindane
approximately 27 kt of PCB is currently still in circula-
use in Russia was 0.019 kt in 1995, a decrease from
tion in PCB-containing equipment in Russia and there-
0.044 kt in 1990 and 0.657 kt in 1985 (HELCOM, 2001).
fore represents a source to the environment (AMAP,
Lindane use was severely restricted in Russia in 1987.
2000). Current quantities of PCB wastes and amounts
Lindane became one of the top ten insecticides used
that have been released from equipment or spilled dur-
in Canada during the 1990s (Environment Canada,
ing dismantling were an additional 4.4 kt. The Arctic
1992). However, pesticide information from Canadian
Council Action Plan against Pollution (ACAP) has initi-
companies is proprietary; therefore, surrogate cropland
ated a cooperative project to assist Russia in phasing out
information was used to estimate lindane usage for Can-
PCBs and in dealing with PCB-contaminated waste.
ada (Li and Bidleman, 2003). Intensive use of lindane on
croplands was concentrated in the prairie region of
Technical HCH and lindane
Canada including the provinces of Alberta, Saskatche-
The use of a mixture of -, -, -, and -HCH isomers,
wan, and Manitoba where it is used as a seed treatment
known as technical HCH, began in 1943, and global
on canola (Waite et al., 2001). The other major use is as
consumption since then has been estimated to be about
a seed treatment on corn in eastern Canada. Annual lin-
10 000 kt (Li et al., 1998a). Technical HCH use was ban-
dane applications in Canada to canola and corn seed are
ned in most western countries and Japan in the 1970s
estimated to have increased from approximately 0.163
but continued in India, Russia and China. China is re-
kt in 1970 to 0.477 kt in 2000, with a cumulative usage
ported to have been the major world producer account-
of about 9 kt over this time period.
ing for about 4500 kt between 1945 and 1983 (Li et al.,
Information on lindane use patterns in the U.S. is
1998b; Li, 1999a). In 1990, India banned the technical
limited, especially in the case of quantities used for seed
product for agricultural use but kept it for public health
treatment (Li and Bidleman, 2003). Direct spray appli-
uses. The circumpolar use pattern for technical HCH in
cation of lindane to crops was estimated to be 28 kt/yr in
1980 and 2000, adapted from Li (1999b), is shown in
the mid-1990s, with 81% on pecans grown in the south-
Figure 2ท5.
eastern U.S. (NCFAP, 2001). Based on the National Cen-
Lindane, containing almost pure -HCH (the only
ter for Food and Agricultural Policy (NCFAP) survey, it
insecticidally active isomer), replaced technical HCH in
seems likely that use of lindane in Alaska during the
Canada, the U.S., and western Europe during the late-
1990s was negligible.

---

Chapter 2 ท Sources and Pathways of Persistent Organic Pollutants
13
1980
2000
+ -HCH emissions,
tonnes / grid cell
0
0.0001-0.1
0.1-0.5
0.5-2
2-10
10-50
50-100
100-250
250-600
Figure 2ท5. Use of technical-HCH in the northern hemisphere in 1980 and 2000 (adapted from Li and Bidleman, 2003).
Only 3.2 kt of lindane was applied in China between
1950 to 1993 is approximately 2600 kt (Voldner and Li,
1991 and 2000. The rest was exported or stockpiled.
1995). Between 1945 and 1972, the total cumulative pro-
Consumption of lindane in China was 0.50 kt in 2000
duction in the U.S. was 1340 kt, with domestic sales ac-
(Li et al., 2001a; Li and Bidleman, 2003).
counting for 645 kt and the rest exported. DDT produc-
tion was discontinued in 1972 when some producers
DDT
ceased operations. According to information provided
Bans on the use of DDT were introduced in the U.S.,
to UNEP as part of the Stockholm Convention negotia-
Canada, and Japan and in most western European coun-
tions, DDT production continues in China and India, for
tries in the early-1970s. However, DDT production in
use in fighting malaria and other insect-borne diseases in
China, India, Russia, and possibly other countries con-
over 25 countries. The largest known current producer
tinued during the 1970s and 1980s. DDT production
is India (approximately 0.007 kt/yr).
peaked in China during the late-1970s and was phased
The gridded global annual usage of DDT on farm-
out in 1984 (Li et al., 1999). DDT use in Russia contin-
land for 1980 and 2000 is shown in Figure 2ท6. Total
ued until 1990 when 0.084 kt was reportedly used,
global DDT usage in agriculture for 1980 was around
down from 0.463 kt in 1980 (HELCOM, 2001). The
40 kt, and around 0.1 kt for 2000. Current uses for dis-
total estimated global usage of DDT in agriculture from
ease vector control in tropical countries are much larger
1980
2000
DDT emissions,
tonnes / grid cell
0
0.001- 0.01
0.01-1
1- 2
2 -10
10 - 20
20 -100
100 - 239
Figure 2ท6. Use of DDT in the northern hemisphere in 1980 and 2000 (Li and Bidleman, 2003).

---

14
AMAP Assessment 2002: Persistent Organic Pollutants in the Arctic
than agricultural uses; however, they are declining
mated to be 1.5 kt, however, global production has not
(UNEP, 2002). For example Mexico used about 1.80 kt
been estimated. The UNEP POPs survey indicated that
of DDT in 1991. This was reduced to 0.497 kt in 1997
there is no current mirex production. China, however,
and further reductions are planned (UNEP, 2002). The
requested a production exemption for mirex for use as
trade publication Europa Chemie, gave India's cumula-
a termiticide and it is therefore likely that minor uses
tive DDT usage to 1989 as 280 kt for malaria control
remain.
and 50 kt in agriculture (Li and Bidleman, 2003).
Chlordane
Polychlorobornanes and polychlorinated camphenes
Technical grade chlordane is a mixture of at least 120
(toxaphene)
compounds, with the major constituents being cis- and
The major use region for toxaphene was the U.S. cotton
trans-chlordane, heptachlor, cis- and trans-nonachlor,
belt, however, significant uses also occurred on other
chlordene, and others (Dearth and Hites, 1991). Chlor-
crop types. In 1983, toxaphene registration was can-
dane was released into the environment primarily from
celed by the U.S. Environmental Protection Agency (EPA)
its application as a soil insecticide and termiticide. The
and was banned in the U.S. in 1986. Use of toxaphene
U.S. was the major world producer and user of chlor-
continued in Central America and Mexico until the
dane. However, there was limited use in western Europe,
early-1990s. Production for use in this region took place
the former Soviet Union and tropical Asian countries. In
in Nicaragua until 1991. The total toxaphene residues
the U.S., chlordane was used extensively prior to 1983,
left in agricultural soils in the U.S. at the beginning of
and from 1983 to 1988 it was registered for termite con-
2000 are estimated to be about 29 kt. In 2000, almost
trol. In 1997, the sole U.S. manufacturer of chlordane
20 years after banning the use of this pesticide, approxi-
voluntarily ceased production at all of its national and
mately 0.360 kt of toxaphene was estimated to be emit-
international facilities. There are production facilities in
ted from agricultural soils in the U.S. (Li, 2001; Li et al.,
Singapore and China, however.
2001b). Total use in the U.S. and Mexico/Central Amer-
ica was estimated to be 540 kt.
Aldrin, dieldrin, endrin, and heptachlor
The former Soviet Union was also a significant pro-
World sales of aldrin and dieldrin ceased in 1991 when
ducer and user of polychloroterpenes. This insecticide
the major manufacturer voluntarily stopped production.
was introduced in the former Soviet Union in the 1950s
Endrin production ceased in the mid-1980s. Old stocks
and was still widely used in Russian agriculture at the end
of these chemicals, particularly dieldrin, were, however,
of the 1980s. The total toxaphene usage within the for-
donated to African countries in the 1980s-90s for insect
mer Soviet Union was less than 100 kt (Voldner and Li,
control, so emissions to the environment have continued
1993; 1995) and was applied mostly in the Ukraine (Kun-
(UNEP, 2002). Dieldrin was mainly used as a soil insec-
diev and Kagan, 1993). Toxaphene was still used to con-
ticide. In tropical countries it was used for the control of
trol sugar beet pests in 1993 (Kundiev and Kagan, 1993).
locusts and for disease vector control.
As of 1992, toxaphene was categorized as a `severely re-
stricted' pesticide in Russia (Voldner and Li, 1993).
Endosulfan
The former East Germany was a major producer
Use of endosulfan in the U.S. has recently been estimated
and exporter of polychloroterpenes under the name
to be 0.64 - 0.95 kt per year (USEPA, 2001). Endosulfan
`Melipax' until 1990 (Heinisch et al., 1994).
is also used in Canada and Europe. Global use is thus es-
China produced toxaphene between 1967 and 1972
timated to be in the range of 1-2 kt per year. It is regis-
with a maximum annual production of approximately
tered for use on a wide variety of speciality crops (pe-
1 kt in 1970 and a total production around 3.6 kt (Li
cans, pumpkins, squash). It is applied by boom sprayer
and Bidleman, 2003).
and by aircraft, and thus, has the potential for signifi-
With the signing of the Stockholm Convention, toxa-
cant dispersal in the environment.
phene is likely to be consigned to the history books. In-
formation supplied to UNEP as part of the Stockholm
Butyltins
Convention negotiations suggests it is no longer produced.
TBT and other organotin compounds were initially used
in agriculture. Subsequently, TBT has had wide applica-
Diene-organochlorine insecticides
tion as a marine antifoulant starting in the 1960s. It has
Members of the large diene-organochlorine group (in-
also been used as a wood preservative. TBT is found to
cluding chlordane/heptachlor, dieldrin/endrin/aldrin, mi-
provide effective protection for boat hulls at release
rex and chlordecone) were formerly used as insecticides
rates of less than 4 ตg/cm2/day, and has been a popular
and use-information was provided in the previous AMAP
antifoulant because it maintains its efficacy for up to five
POPs assessment (de March et al., 1998). Chlordecone,
years compared to about three years for other conven-
mirex, aldrin, endrin and chlordane are included in the
tional applications. TBT's most important entry route to
UN ECE POPs Protocol under the LRTAP Convention.
the sea is directly from boats, aquaculture pens, moor-
Chlordecone has not been measured in Arctic biota or
ings, and industrial cooling pipes to which products con-
abiotic samples. This chemical was marketed in the U.S.
taining it have been applied. It may also enter ocean wa-
as Kepone and pesticide registration was canceled in the
ters from municipal waste water and sewage sludge.
U.S. in 1978 following widespread contamination of the
Organotin-stabilized PVC is used in a wide variety of
James River in the eastern U.S. from factory releases.
applications including: pipes for drinking water, waste
Mirex, formed by further chlorination of chlordecone,
water, and drainage; packaging materials; and, window
was more widely used as an insecticide, termiticide, and
frames. The organotin constituents have been shown to
flame retardant. Total production in the U.S. was esti-
leach from PVC and other materials leading to contami-

---

Chapter 2 ท Sources and Pathways of Persistent Organic Pollutants
15
nation of food, drinking water, municipal water and,
HCB used in the manufacture of various substances such
sewage sludge (Forsyth et al., 1992; 1994; Fent, 1996b;
as pentachlorophenol, pentachlorothiophenol, and py-
Forsyth and Jay, 1997). In a Japanese study, plastic
rotechnical products (HELCOM, 2001).
products such as baking parchments of siliconized paper,
A recent assessment of global sources of HCB (Bai-
polyurethane gloves, dish-washing sponges, and cello-
ley, 2001) concluded that total current emissions could
phane film for wrapping food bought from a supermar-
be around 0.023 kt/yr with a possible range between
ket, were found to contain MBT, DBT, and TBT (Taka-
0.012 and 0.092 kt/yr (Bailey, 2001). A substantial por-
hashi et al., 1999). No information is available regard-
tion of the HCB measured in the atmosphere had un-
ing leaching from PVC materials at dump sites, but this
identified sources and/or was due to revolatilization (i.e.,
is a potential emission source to the environment in Arc-
currently known emissions could not account for pre-
tic communities.
vailing global air concentrations). Russia was estimated
TBT is degraded by sequential debutylation to DBT,
to emit 0.011 kt/yr of HCB in 1995, with other coun-
MBT and eventually to relatively non-toxic inorganic tin
tries bordering the Baltic Sea accounting for about 0.003
compounds, primarily by organisms. The breakdown of
kt/yr (HELCOM, 2001).
TBT is much slower in anaerobic sediments than in
water (Clark et al., 1988), and therefore, contaminated
OCS
sediments may act as an important environmental reser-
Maximum emissions of OCS in the Great Lakes region
voir for TBT as well as MBT and DBT, long after their
of North America occurred in the 1960s (USEPA,
use has been curtailed.
1999a), probably due to disposal of wastes related to
Most circumpolar and northern European countries
chlorine manufacturing using graphite electrodes, a pro-
now partially regulate the use of TBT (France, 1982;
cess abandoned in the 1970s. In Norway, emission of
U.S., 1986; U.K., 1987; Canada, 1989; Europe, 1991).
OCS and other chlorostyrenes was traced to production
Regulations vary, but generally, only controlled release
of magnesium using graphite electrodes (Lunde and Of-
formulations are permitted and TBT-based antifoulants
stad, 1976). Recent measurements have been made in
are prohibited for boats smaller than 25 m. The U.N. In-
Germany (Bester et al., 1998), however, in general, emis-
ternational Maritime Organization (IMO) has agreed to
sions and use of OCS are not well documented. Little is
a global ban on new use of TBT on ship hulls from
known about global emissions of OCS, however, magne-
1 January, 2003. After 2008, TBT-based antifouling
sium production and chlorine manufacturing were his-
paints must be removed from ship hulls or encapsulated
torically important sources (USEPA, 1999a). Hydroxy-
with an impermeable paint so no leakage to the environ-
heptachlorostyrene, a metabolite of OCS, was identified
ment can occur.
recently as a major hydroxylated metabolite in polar
Global production of organotin compounds was esti-
bear and human plasma in the Arctic (Sandau, 2000;
mated to be 50 kt in 1992 (Mercier et al., 1994). Bio-
Sandau et al., 2000).
cides (primarily trialkyltins) make up approximately
20% of the total annual production (Bennett, 1996)
PCDD/Fs
with PVC stabilizers (primarily mono- and dialkyltins)
PCDD/Fs enter the environment as by-products of in-
being approximately 70% (Hoch, 2001). Total bis(trib-
dustrial processes. The most significant sources are low-
utyltin) oxide (TBTO) production in the Federal Repub-
temperature, incomplete incineration of chlorine-con-
lic of Germany, was estimated to be 2.0 kt, of which
taining materials such as plastics. Other major sources
70% was used in antifouling paints, 20% as a wood pre-
include thermal processes, such as motor vehicle fuel
servative, and 10% as a preservative in textiles, leather,
combustion in countries where leaded fuel containing
and other materials (WHO, 1990). No estimates are
chlorine scavengers is still used, and metallurgical indus-
available for current annual global consumption or for
tries. Pulp and paper mills using chlorine in the bleach-
use patterns (Hoch 2001).
ing process have been important sources for inputs to
the aquatic environment. PCDD/Fs are also trace con-
HCB and pentachlorobenzene (PeCBz)
taminants in chlorophenoxy herbicides, PCB formula-
HCB is produced as a by-product in the production of a
tions, and chlorophenol wood preservatives.
large number of chlorinated compounds, particularly
Few studies are available estimating circumpolar
lower chlorinated benzenes, and in the production of
emissions of PCDD/Fs. Rough estimates of the global
several pesticides. In the 1960s, it had limited use as a
emissions of PCDD/Fs are available from Brzuzy and
fungicide. HCB is emitted to the atmosphere in flue
Hites (1996). In addition, an overview of the current sta-
gases generated by waste incineration facilities and met-
tus of national and regional emission inventories for
allurgical industries. Both HCB and PeCBz have previ-
PCDD/Fs globally can be found in UNEP (1999). This re-
ously been identified as by-products from production
port includes estimates of PCDD/F emissions for north-
of chlorinated solvents (Environment Canada, 1993;
ern Europe, Canada, the U.S., and Japan. Japan and the
USEPA, 1999c).
U.S. were considered the largest sources of PCDD/Fs
PeCBz was used in dielectric fluids in PCB-contain-
(5300 g TEQ/yr and 2700 g TEQ/yr, respectively). Swe-
ing transformers. A Canadian survey found that up to
den, the only Nordic country in the survey, had very low
0.2 kt of PeCBz was in use in transformers in the early-
annual estimated PCDD/F fluxes (22 g TEQ/yr) while
1990s. However, this figure is now out of date due to the
Canadian emissions were estimated to be 290 g TEQ/yr.
removal and destruction of most PCB- containing equip-
ment. Nevertheless, it illustrates that older PCB contain-
PAHs
ing devices in many circumpolar countries are potential
PAHs can be classified by their source type: petrogenic,
sources of PeCBz. PeCBz is also an impurity in technical
biogenic, and pyrogenic. PAHs of petrogenic origin are

---

16
AMAP Assessment 2002: Persistent Organic Pollutants in the Arctic
related to petroleum, including crude oil and its refined
MCCPs
products. The presence of naphthalene and its alkyl-sub-
MCCPs are mainly used as flame-retarding plasticizers
stituted homologues in sediments is characteristic of un-
in polyvinyl chloride plastics and releases to the envir-
weathered petroleum (Robertson, 1998). The naphtha-
onment are relatively small compared to production.
lene : phenanthrene ratio is much greater than 1.0 for most
MCCPs are large-volume production chemicals with
petroleum types. PAHs of petrogenic origin are also char-
global capacity estimated to be 0.25 kt/yr (Muir et al.,
acterized by homologous families of related PAHs (naph-
2000a; OSPAR, 2000), and a steady production during
thalenes, phenanthrenes and dibenzothiophenes), where
the 1990s. Thus it is likely that over 5000 kt have been
the parent PAH for each family is less abundant than the
produced since the mid-1970s when production volumes
alkylated homologues (Page et al., 1999). PAHs of biogenic
were significantly increased. Annual releases of MCCPs
origin are generated by biological processes or by the
to air and water in western Europe were estimated to be
early stages of diagenesis in marine sediments (e.g., pery-
1.87 kt in 1998, compared with production of 55 kt
lene) (Venkatesan, 1988). PAHs with 4- to 6-ring hydro-
(OSPAR, 2000). There are, as yet, no reports on these
carbons are generally of pyrogenic origin and are gener-
compounds in the Arctic environment.
ated by the combustion of fossil fuels and recent organic
material. The relative abundance of these PAHs to 2- to
TeBDE and PeBDE
3-ring hydrocarbons can be used to help distinguish
TeBDE and PeBDE compounds have been used since the
between petrogenic and pyrogenic sources (Robertson,
1970s as flame retardants in, among other things, poly-
1998). PAHs in the atmosphere are primarily from com-
urethane foams (de Boer et al., 2000). The commercial
bustion of fossil fuels to produce electricity and heat, ve-
PeBDE product is comprised mainly of pentabromodi-
hicular exhausts, forest fires, as well as industrial activi-
phenyl ether with tetra- and hexabromodiphenyl ether
ties such as non-ferrous and ferrous metal production,
impurities (Hardy, 2001; de Boer et al., 2000). Annual
and fertilizer production. PAHs detected in the Arctic at-
worldwide production of PeBDE in 1990 was estimated
mosphere reflect contributions of emissions from middle
to be 4.0 kt (Arias, 1992) and use increased during the
and high latitudes in the circumpolar countries (Hoyau
1990s. Global use in 1999 was 8.5 kt, of which >90%
et al., 1996; Halsall et al., 1997; Masclet et al., 2000).
was in North America due to a phase-out of use in Eu-
rope (BSEF, 2000). Assuming a steady increase in pro-
PCNs
duction since the early-1980s, this implies a total pro-
Until the 1970s, PCNs were high volume chemicals,
duction in the range of 70-120 kt. Environmental con-
with the worldwide production being approximately 9.0
centrations were increasing during the 1990s in the
kt/yr in the 1920s (Jakobsson and Asplund, 2000). Pro-
Canadian Arctic (See Section 5.4.6).
duction of PCN decreased significantly after 1977. The
production of PCNs in the U.S. stopped in 1980. Given
OcBDE and DeBDE
the relatively high production volumes in the 1920-
The main use of OcBDE and DeBDE technical products
1930s, it seems likely that total PCN production was in
is in high impact polystyrene used to manufacture elec-
the range of 200-400 kt. Crookes and Howe (1993) con-
trical enclosures (e.g., television sets). The major compo-
cluded that it was not possible to derive a global emis-
nent of the OcBDE technical product is a heptaBDE as
sion estimated for PCNs. Furthermore, Haglund et al.
well as hexa-, octa- and nonaBDE impurities. Small
(1993) found that PCNs were contaminants in technical
amounts of octa- and nonaBDEs are found as impurities
PCB formulations. Falandysz (1998) mentions technical
in DeBDE. A minor but important use of DeBDE is in
PCBs as a potential source of PCNs and estimated a po-
flame-retarding of fabrics where it is applied as a fabric
tential release of 0.1 kt based on the worldwide produc-
back coat encapsulated in latex (Hardy, 2001). World-
tion of PCBs and a median value of 0.0067% PCNs in
wide (i.e., mainly western Europe and North America)
Aroclor and Clophen mixtures. A significant current
use of OcBDE and DeBDE technical products was 6.0
source of PCNs is incineration (Crookes and Howe,
and 30 kt respectively in 1990 (Arias, 1992). Global de-
1993; Falandysz, 1998). Indeed, PCN congeners associ-
mand for OcBDE and DeBDE was 3.8 kt and 54.8 kt,
ated with combustion are elevated in Arctic air in winter
respectively, in 1999. Assuming a gradual increase in
(Harner et al., 1998; Helm and Bidleman, 2003).
production since the early-1980s, this implies a cumula-
tive production to date of 500-800 kt Oc- and DeBDEs.
SCCPs
Most of this production was used in areas that are po-
SCCPs are used mainly as extreme temperature additives
tential source regions for atmospheric transport to the
in metal working fluids for a variety of engineering and
Arctic, i.e., countries of the western Pacific/eastern Asia,
metal working operations such as drilling, machining/
North America and western Europe.
cutting, drawing, and stamping (Environment Canada,
1993; Tomy et al., 1998). They are also used in paints
Other brominated flame retardants
and sealants and have a minor but environmentally sig-
Hexabromocyclododecane (HBCD) and TBBPA are
nificant use as fat liquors in the leather working indus-
other major brominated flame retardants. HBCD has re-
try. Due to concerns about the toxicity, bioaccumula-
placed pentaBDEs in Europe, with 8.9 kt used in 1999
tion, and persistence of SCCPs, use of these chemicals is
(BSEF, 2000). HBCD is produced by bromination of cy-
declining as users switch to alternative products. Use
clododecane in a batch process and has been used for
since the 1940s, however, has been very high compared
about 20 years. TBBPA is the major brominated flame
to most aliphatic chlorinated hydrocarbons of similar
retardant in current use primarily in electronic circuit
molecular weight (Table 2ท1). Global manufacturing ca-
boards (121 kt use globally in 1999; BSEF, 2000).
pacity is estimated to be 50 kt/yr.
TBBPA is covalently bonded into most materials but

---

Chapter 2 ท Sources and Pathways of Persistent Organic Pollutants
17
some TBBPA is not bound (Sellstr๖m and Jansson,
Current and former military bases throughout the
1995), leading to some environmental releases, though
circumpolar Arctic, especially those with older radar
probably minor compared to PBDEs.
equipment, have been previously identified as sources
and were discussed in the previous AMAP POPs assess-
Perfluoroalkyl sulfonates
ment (de March et al., 1998). Many of these sites have
Perfluorinated surfactants are employed for industrial
undergone cleanup which include removal of contami-
and commercial applications and are used in lubricants,
nated equipment and soils. For example, the cleanup of
paints, polishes, food packaging, and fire-fighting foams
21 sites in the Canadian Arctic is scheduled for comple-
(Hekster et al., 2002; Key et al., 1997). PFOS is an im-
tion in 2008 (Canada DND, 2001) and there have been
portant perfluorinated surfactant as well as a precursor
similar campaigns in Alaska, Greenland and Norway.
to other perfluorinated surfactants (Hekster et al., 2002;
The situation in the Russian Arctic regarding PCB use at
Key et al., 1997). In 2000, the estimated annual U.S.
military sites is unclear. The Russian Ministry of De-
production of PFOS was 2.9 kt, but as a result of the 3M
fence did not take part in the inventory of PCBs or PCB-
Company's phase-out, no PFOS production is antici-
containing equipment in Russia because their position
pated in the U.S. in 2003. Total production of all fluori-
was that PCB-containing equipment was not in use any-
nated surfactants (anionics, cationics and neutrals) was
more (AMAP, 2000). Thus no information is available
0.2 kt in the mid-1970s (Fielding, 1979), which suggests
on the disposal of PCBs and PCB-containing equipment
that a large increase in PFOS production occurred dur-
from military sites in the Russian Arctic.
ing the past 25 years. Assuming similar production vol-
umes for the past ten years and smaller volumes since
Svalbard
the introduction of these chemicals in the late- 1940s, it
On Svalbard, local coal mining activities and settlements
seems reasonable to estimate that at least 50 kt have
are the major primary sources of POPs (Kovacs, 1997),
been produced. Most of this production would have
with coal-fired power plants located in five settlements
been released into the environment due to open uses as
being sources of PAHs to the atmosphere. Calculation of
surface treatments. Production of PFOS, or its precur-
sulfur- and particle distribution as primary indicators of
sors, by other manufacturers outside of the U.S. or Eu-
contaminant sources for the coal mines at Longyearbyen
ropean Union may occur but is not presently docu-
and Svea suggests that mining activities could be a major
mented. The properties of PFOS suggest that it is a poor
source of PAHs to the Svalbard environment (Holte et
candidate for long-range atmospheric transport. These
al., 1996; dos Santos et al., 1996). It is also suggested
facts have previously led to speculation that the global
that the Russian coal mines at Barentsburg represent
dissemination of PFOS must occur via an airborne neu-
comparable sources. In a study of profiles of pyrogenic
tral derivative that yields the free acid upon degradation
PAHs in lake sediments on Spitsbergen, Rose et al.
(Renner, 2001). Long-range transport by ocean currents
(2003) found highest fluxes of PAHs in Tenndammen, a
cannot be ruled out given the stability of PFOS.
lake within 20 km of the coal mining towns of Barents-
burg and Longyearbyen.
Perfluoroalkanoic acids
The major sources of PAHs in marine sediments are
Like PFOS, these compounds, particularly perfluoro-
thought to be of natural petrogenic origin resulting from
octanoic acid (PFOA), are employed for industrial and
petrogenic seepage from the sea bed and erosion of coal
commercial applications and are used in lubricants.
seams (Akvaplan-niva, 1998). Higher DDT concentra-
PFOA has a unique application as a plasticizer in the flu-
tions (0.38 ng/g dw) were found at a deep site in Kongs-
orinated polymer Teflonฎ. PFOA was detected at low
fjorden relative to nearshore sites in eastern Svalbard (Lom-
levels in a global survey of marine and freshwater biota,
fjorden, Erik Eriksen Strait) which had DDT <0.2 ng/g
which included ringed seals (Phoca hispida) and polar
dw. OC concentrations in sediments near the settlements
bears, but results were not reported (K. Kannan, Michi-
in Svalbard were not assessed, however (Akvaplan-niva,
gan State University, pers. comm., 2002). No production
1998). Hop et al. (2001) found higher PCB and PAH
information is publicly available on the perfluoroalka-
concentrations in macrobenthos sampled near the settle-
noic acids.
ments of Billefjorden, Gr๘nfjorden, Adventfjorden, and
Kongsfjorden in Svalbard. PCB profiles from fjords with
Russian settlements had a higher proportion of lower
2.3.2. Local/regional sources within the Arctic
chlorinated congeners compared to fjords with Norwe-
Local sources of POPs are considered to be only minor
gian settlements, probably because of local pollution
contributors to contamination of the Arctic environment
and the different PCB products used in each community.
when considered on a continental or ocean-wide scale.
On a local scale, however, household heating in settle-
Coastal Norway and western Russia
ments, burning of hydrocarbons for electricity and trans-
PCBs have been found in surface sediments from har-
port, and incineration and open burning of garbage,
bors in northern Norway (Harstad, Hammerfest, Troms๘,
contribute significantly to the input of organic pollutants
Honningsvๅg) and Russia (Kola Bay, Guba Pechenga)
such as PAHs. Emissions of PCDD/Fs from these com-
(Dahle et al., 2000) with relatively high (10 -100 ng/g
bustion sources may also be important in Nunavut (Can-
dw) levels found in comparison with background sites
ada) although considered very minor compared to heav-
reported previously in the previous AMAP assessment (de
ily populated regions of North America (Commoner et
March et al., 1998). PCB levels and congener compo-
al., 2000). In several Arctic regions, mineral exploration,
sition among harbors was similar (higher chlorinated
coal mining and heavy industry account for the highest
PCBs predominated) except for Guba Pechenga, where
input of persistent pollutants such as PAHs and PCBs.
lower chlorinated PCBs predominated for unknown rea-

---

18
AMAP Assessment 2002: Persistent Organic Pollutants in the Arctic
sons. No large differences in OC concentrations were
was 40 times higher. The results suggest that villages are
found between Norwegian and Russian harbors. Har-
sources of legacy OCs such as PCBs, as well as currently
bors probably constitute hotspots for PCBs in the Arctic
used PBDEs, to the nearby marine environment.
marine environment with higher concentrations (up to
Previous studies of scallops (Chlamys islandicus) and
10 times) relative to non-harbor areas.
sediments have shown that Thule Air Base is a local
In a follow-up study in Kola Bay (1997), much higher
source of PCBs to the marine environment (Kj๘lholt and
concentrations of most OCs in question were found
Hansen, 1986).
compared to a control location (Guba Zapadnaya Litsa)
(Savinova et al., 2000a). The stations with the highest
Canada
levels of PCBs, toxaphene and HCB were located close
From 1996 to 2001, additional studies and remediation
to the harbor of Polarnyy City, situated on Kola Bay, 20
of old military sites contaminated with PCBs were con-
km north of Murmansk. Concentrations of PCB near
ducted in the Canadian Arctic. Detailed assessments of
Polarnyy City ranged from 650 to 8700 ng/g dw while
PCB contamination were conducted at two sites in the
levels were 24 ng/g dw in sediments in the outer reaches
eastern Canadian Arctic, Saglek Bay (58ฐ29'N, 62ฐ40'W)
of Kola Bay. A surprising observation was the presence
in northern Labrador, and Resolution Island at the south-
of relatively high levels of toxaphene in surface sedi-
eastern tip of Baffin Island.
ments in Kola Bay (3.5- 680 ng/g dw) and in Guba Za-
At Saglek Bay, high levels of PCBs (more than 50
padnaya Litsa (19 - 85 ng/g dw). Although there are few
ตg/g dw in soils) were found at a former military radar
other toxaphene measurements in marine sediments for
site (ESG, 2002). The cleanup from 1997 to 1999 effec-
comparison, the geometric mean levels in both Kola Bay
tively removed the terrestrial sources of contamination
and Guba Zapadnaya Litsa are higher than observed in
to the surrounding land and to the marine environment
freshwater surface sediments in the Great Lakes (Pear-
of Saglek Bay. PCB concentrations in sediment cores
son et al., 1998) or in northwestern Europe (Rose et al.,
from lakes near the former radar facility declined with
2001). This suggests significant use of toxaphene in
increasing distance from the site (Betts-Piper, 2001).
northern Russia, at least in the Kola Peninsula, possibly
Four of eight lakes within 5 km of the site had elevated
for insect control in urban areas or on ships.
levels (>100 ng/g dw) compared to background sites 30
km away (0.3 -17 ng/g dw) or to other remote lakes in
Jan Mayen
the Canadian Arctic (Muir et al., 1996a). The PCB con-
On the island of Jan Mayen, elevated PCB levels were
gener profile in both the near-site and remote lakes had a
found in soil within and in the immediate proximity of a
clear Aroclor 1260 profile similar to the product used at
dump used between 1960 and 1995 (Gabrielsen et al.,
the radar facility. Bright et al. (1995a) and Duskenko et
1997). The source of the PCBs was seven transformers,
al. (1996) reported similar results from a study of 24
each containing approximately 200 L of oil, that were
military radar sites in the Canadian Arctic. They con-
emptied into the dump in the late-1970s. Despite exten-
cluded that the radar sites were acting as sources of con-
sive sampling, it was only possible to estimate the amount
tamination to nearby lakes via aerial redistribution. This
of PCB in the dump as being between 10 and 2000 kg.
was confirmed at Saglek Bay by the detailed study by
There was no evidence of local PCB contamination ex-
Betts-Piper (2001).
tending from the dump into the freshwater lake or to
Marine investigations were conducted to study PCB
other areas on the island. Up until 1989, 2000-3000 L of
contamination in Saglek Bay over three seasons from
lubrication oil and other waste products (white spirits,
1997 to 1999. These studies delineated PCB-contami-
paint) were also dumped. The dump is located 25 m
nated sediments and quantified PCB uptake in the ma-
from the edge of a coastal cliff of porous vulcanic rock,
rine food chain, including benthic invertebrates, bottom-
which is subject to erosion, primarily by seawater. Cur-
feeding fish, pelagic fish, marine mammals, and seabirds.
rently, the rate of erosion is unknown.
They indicated that the contaminated sediments repre-
sented a source of PCBs to local wildlife. Inputs of PCBs
Greenland
to the marine environment occurred from a contami-
The distribution of persistent halogenated organics was
nated beach area associated with the original station.
studied during 2000 near the western Greenland villages
Sediment PCB concentrations near this beach were 500
of Quaqortoq (3500 inhabitants), Igaliko (30 inhabi-
ng/g to 130 000 ng/g dw in the intertidal sediment, and
tants) and Usuk (background site 3-5 km from Igaliko)
600 ng/g to 6200 ng/g dw in the Saglek anchorage.
(Christensen et al., 2002; Vorkamp et al., 2002). The an-
Concentrations declined exponentially with distance,
imals analyzed were shorthorn sculpin (Myoxocephalus
approaching background concentrations (<2 ng/g) with-
scorpius), Greenland cod (Gadus ogac), spotted wolffish
in 6 -10 km (ESG, 1999; 2002). PCBs were also present
(Anarhichas minor), starry ray (Raja radiata) and blue
in deepwater sediments of the bay, particularly imme-
mussels (Mytilus edulis). All concentrations of persistent
diately offshore and west of the contaminated beach
halogenated organics were low in mussels. The highest
(Figure 2ท7).
concentrations of PCBs and PBDEs were observed in
The samples of invertebrates collected from the im-
fish from Quaqortoq followed by Igaliko and Usuk. This
mediate vicinity of the contaminated beach contained
trend was not as pronounced for chlorinated pesticides,
PCBs at high concentrations, consistent with the concen-
which implied that there were local sources of PCBs and
trations measured in the beach sediment (ESG, 1998).
PBDEs, but not chlorinated pesticides. The levels of
Snails and scuds from the intertidal area had PCB con-
PBDEs were 15-24 times lower than PCB levels meas-
centrations of 8000 and 49 000 ng/g ww, respectively.
ured in the same individuals, except for shorthorn scul-
The concentration in sea urchins from this area was
pin collected at Quaqortoq, where the level of PCBs
slightly lower (5200 ng/g ww). Invertebrate tissue con-

---

Chapter 2 ท Sources and Pathways of Persistent Organic Pollutants
19
group. Biomarker responses were dose-dependent and in
PCB concentration in sediments, ng/g dw
some cases, sex-dependent (see Section 6.3.3.3).
Similar contamination by PCBs was investigated at
2
Resolution Island (61ฐ35'N, 60ฐ40'W) at the southeast-
5
ern tip of Baffin Island in the eastern Canadian Arctic
10
(ASU, 1997; 2001). Initial assessment of the site in the
50
early-1990s showed it to be highly contaminated with
100
1000
PCBs (ESG, 1994). The site contained at least twenty
5000
buildings requiring demolition, along with a large
amount of visible debris, tanks, and many barrels. Build-
ings in the communications complex contained electrical
Saglek Bay
equipment suspected of containing PCBs, and other
buildings contained asbestos. The total volume of soil
which was contaminated with PCBs at concentrations
above 50 000 ng/g (exceeding soil guidelines for PCBs
under the Canadian Environmental Protection Act) was
estimated to be 5000 m3 with about 20 000 m3 contam-
Areas of soil
formerly contaminated with PCBs
inated at the 1000 -50 000 ng/g level. Site remediation
initially involved building barriers composed of a variety
of oil absorbent booms across PCB leachate pathways to
prevent further PCB migration. PCB-containing compo-
5 km
nents and liquids from transformers were removed from
the main station to the registered PCB storage facility on
Figure 2ท7. PCB contamination in marine sediments of Saglek Bay
the site. An environmental assessment of contaminant
in northern Labrador based on 243 surface sediment sample results
migration to the marine environment made the assump-
from 1997, 1998 and 1999 indicating the dispersion from a con-
taminated beach.
tion that PCB movement was controlled by the barriers
and aerial transport of PCBs was insignificant. The as-
taminant concentrations generally return to near-back-
sessment concluded that the site does not present unac-
ground concentrations within 7-10 km of the formerly
ceptable contaminant exposure conditions to humans,
contaminated beach.
or terrestrial and marine wildlife (Golder, 1997). Reme-
PCB concentrations were relatively high in short-
diation work conducted from 1997 to 2001 involved ex-
horn sculpin sampled in the nearshore area close to the
cavation and removal of highly contaminated soils and
contaminated beach, exceeding 1000 ng/g ww (whole
debris from dump sites on the island (ASU, 2001). This
body minus liver, Aroclor equivalent) in two-thirds of the
material was stored in sealed containers on-site for fu-
samples and exceeding 10 000 ng/g ww in a few sam-
ture disposal.
ples. Concentrations also exceeded 1000 ng/g ww in
In addition to PCBs, some former military sites re-
some shorthorn sculpin samples collected at sites up to
ceived significant DDT applications. The bioavailability
1.5 km east and 3 km west of the beach. PCB concentra-
of this localized DDT contamination to the terrestrial
tions in muscle and liver of Arctic char (Salvelinus alpi-
Arctic environment was examined in a study at an aban-
nus) did not vary with the proximity of the fish to the
doned Long Range Aid to Navigation (LORAN) station
contaminated beach (ESG, 1998). PCB concentrations
located at Kittigazuit, Northwest Territories (69ฐ16'56"N,
ranged from a low of 13 ng/g ww to a high of 66 ng/g
133ฐ54'32"W) in the western Canadian Arctic (Nirwal,
ww (Aroclor equivalent), with both of these extremes
2001). The study site received applications of DDT be-
measured in char collected at the Okak reference site
tween 1948 and 1950. Despite the passage of time, soil
(ESG, 1998). These were similar to results for PCBs in
concentrations have remained high (maximum DDT =
anadromous char from the Labrador coast (Muir et al.
210 000 ng/g dw), and the composition of DDT com-
1999c; 2000c) and are consistent with the largely
pounds in soil still resembled the original pesticide for-
pelagic feeding habits of char.
mulation (59% p,p'-DDT). In soils, loss and degrada-
PCB concentrations in seals from the Saglek Bay
tion of DDT was less pronounced when compared to
area varied over a wide range, from a low of 500 ng/g
temperate and tropical environments. Samples of soil,
ww in the adipose tissue of one 11-year-old seal, to a
sediment, willow (Salix sp.), grass (Elymus sp.), and
high of 9400 ng/g ww in a 10-year-old seal. The result
Arctic ground squirrel (Spermophilus panyi) were col-
for this seal is exceptionally high, exceeding the results
lected at the LORAN station and at a nearby reindeer
for the other seals by a factor of 4 - 6. It is also much
herding camp. Concentrations of DDT in soils at the
higher than results reported for ringed seals from the
station ranged from 62 to 210 000 ng/g dw. Highest con-
community of Nain, further south on the Labrador
centrations were found within an area of approximately
coast, and elsewhere in the Arctic (Section 4.4.6.1).
4024 m2, while a smaller area (386 m2) at the herding
Black guillemots (Cepphus grylle) in Saglek Bay, Lab-
camp had elevated concentrations as well. Samples of
rador also had elevated PCB concentrations due to ma-
Elymus sp. and Salix sp. collected from the station had a
rine sediment contamination around the former military
higher median DDT concentration compared to the
site. PCB concentrations in liver of nestlings ranged
area near the herding camp or to background sites.
from 15 to 46 ng/g ww in a reference group, 24 to 150
Higher DDT was found in Salix sp. (12-10 000 ng/g
ng/g ww in a group from moderately exposed islands,
dw) compared to Elymus sp. (3.2-1500 ng/g dw). The
and 170 to 6200 ng/g ww in the highly exposed beach
concentration and composition of DDT in Arctic

---

20
AMAP Assessment 2002: Persistent Organic Pollutants in the Arctic
Table 2ท2. Examples of sites in Alaska known to be sources of POPs. This does not represent a comprehensive assessment.
ญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญ
POPs are
Contaminated
Affected
Site
a concern
wildlife
subsistence
Reference
ญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญ
Adak Island (Aleutian Islands)
Yes
Likely
Likely
Technical Memorandum,
ADEC website 1, 3
King Salmon Air Station
Yes (solvents)
Likely
Unknown
ADEC website 1, 3
Pribilof Islands
Fuels, POPs possible
Likely
Likely
ADEC website 1, 3
St. Lawrence Island
Yes
Potential
Likely
ADEC website 1, 3
Cape Romanzof
Yes
Yes
ADEC website 1, 3
Long Range Radar Site
Umiat (former Air Force Base
Yes
Very Likely
Yes
Army COE website 2, 3
on Colville River)
Operable Unit D, Fort Richardson
Yes
Unknown
Unknown
ADEC website 1, 3
Dutch Harbor, Unalaska
Yes
Possibly
Possibly
Army COE website 2, 3
Yakutat Airport
Yes
Unknown
Unknown
Army COE website 2, 3
Barter Island (Kaktovik)
Transformers (PCBs)
Unknown
Unknown
Army COE website 2, 3
Wildwood AFS
Dioxins?
Unknown
Unknown
Army COE website 2, 3
ญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญญ
1 www.state.ak.us/dec/dspar/csites
2 www.poa.usace.army.mil/fuds
3 www.akaction.net/pages/mapping
ground squirrel livers were clearly the result of contami-
tion on POPs in Arctic and subarctic Alaska exist, but
nation at the study site. Liver concentrations at contam-
they have not been peer-reviewed and are not generally
inated areas (maximum DDT = 4300 ng/g lw) declined
available. They do serve, however, to describe reliably
to background levels (maximum DDT = 4.5 ng/g lw)
what contaminants have been detected at these sites of
with increasing distance from contaminated areas. Esti-
concern. Sources include citations in published manu-
mated contaminant exposures were below no-observed
scripts, reports from a variety of organizations, and
effect levels, but a significant relationship between liver
websites. Hurwich and Chary (2000) recently outlined
size and DDT concentration was found. The concen-
and mapped POPs-based research in Alaska and some of
trations in ground squirrels from background sites in
these local areas of concern.
this study were below concentrations reported for Arctic
Environmental contamination in Alaska is often con-
ground squirrels in Alaska (Allen-Gil et al., 1997).
sidered from a general or statewide perspective (i.e.,
The contribution of atmospheric DDT dispersal and
large-scale inputs). Much of the local public awareness
transport at Kittigazuit was negligible because an abrupt
of contaminants, however, stems from concern about
transition existed between soil contaminant levels at the
local sites. Point sources are not typically addressed by
sites, and samples collected immediately off-site. For ex-
researchers studying contaminants, which serves to in-
ample, the median DDT concentration was 1300 ng/g
crease the anxiety of community members. Examples of
dw at the LORAN station, and 540 ng/g dw at the rein-
site-specific concerns in Alaska are the numerous mili-
deer herding camp. In comparison, results for soil sam-
tary sites targeted by the Installation Restoration Pro-
ples considered representative of background conditions
gram (IRP) and the Formerly Used Defense Sites (FUDS)
(3-10 km off site) were below the analytical detection
cleanup programs, which fall under the auspices of the
limit of 20 ng/g dw.
U.S. Department of Defense (Table 2ท2).
A scenario comparable to that at Kittigazuit was also
Table 2ท2 is based on a survey of non peer-reviewed
studied in the vicinity of Fort Churchill, Manitoba, on
documents and websites. Very little effort is made to
the western coast of Hudson Bay. Three years after
publish (in scientific journals) the results of studies at
aerial spraying for mosquito control, sampling within
these sites and to inform local communities. Examples
treated areas showed that the livers of collared lemmings
of documents include Technical Memorandum: Pro-
(Dicrostonyx groenlandicus) contained 5400 - 41 000
posed Biomonitoring Plan for the Nearshore Marine
ng/g lw of DDT and livers of red squirrels (Tamiasciu-
Ecosystems at Adak Island, Alaska. Adak Naval Com-
rus hudsonicus) contained 7400 -17 000 ng/g lw (Brown
plex, Adak, Alaska (Task Order 0204, February 1999)
and Brown, 1970), indicating the persistence and bio-
and the Report of Findings: Cape Romanzof Long
availability of DDT in other terrestrial Arctic environ-
Range Radar Site Military Cleanup, USDOI, Memo to
ments.
Refuge Manager, Yukon Delta National Wildlife Refuge
(January 17, 1991).
Alaska
The U.S. EPA Superfund National Priority List sites
Abandoned sites formally operated by both military and
in Alaska include Adak Naval Air Station, Ketchikan
private entities constitute hundreds of known or poten-
Pulp Company, Fort Richardson (U.S. Army), Elmen-
tial sources of contaminants in Alaska. While most of
dorf Air Force Base, Eielson Air Force Base, Fort Wain-
these sites involve oil-based hydrocarbons (e.g., fuel
wright, Standard Steel and Metals Salvage Yard, Alaska
spills, abandoned wells, etc.), many involve PCBs and
Battery Enterprises, Arctic Surplus, and King Salmon
OC pesticides as well. Many reports and other informa-
(US EPA, 2002).

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