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Chemometric Analysis for Pollution Source Assessment
of Harbour Sediments in Arctic Locations
Kristine B. Pedersen &Tore Lejon &Pernille E. Jensen &
Lisbeth M. Ottosen
Received: 25 November 2014 /Accepted: 6 April 2015
#Springer International Publishing Switzerland 2015
Abstract Pollution levels, pollutant distribution and
potential source assessments based on multivariate anal-
ysis (chemometrics) were made for harbour sediments
from two Arctic locations; Hammerfest in Norway and
Sisimiut in Greenland. High levels of heavy metals were
detected in addition to organic pollutants. Preliminary
assessments based on principal component analysis
(PCA) revealed different sources and pollutant distribu-
tion in the sediments of the two harbours. Tributyltin
(TBT) was, however, found to originate from point
source(s), and the highest concentrations of TBT in both
harbours were found adjacent to the former shipyards.
Polyaromatic hydrocarbons (PAH) ratios and PCA plots
revealed that the predominant source in both harbours
was pyrogenic related to coal/biomass combustion.
Comparison of commercial polychlorinated biphenyls
(PCB) mixtures with PCB compositions in the sedi-
ments indicated relation primarily to German, Russian
and American mixtures in Hammerfest; and American,
Russian and Japanese mixtures in Sisimiut. PCA was
shown to be an important tool for identifying pollutant
sources and differences in pollutant composition in re-
lation to sediment characteristics.
Keywords Harbour sediments .Heavy metals .PAH .
PCB .TBT.Principal component analysis
1 Introduction
International focus on the Arctic environment has in-
creased during the past decade due to the environmental
and geopolitical changes in the region. The effects of
climate change in the Arctic have become apparent,
accumulation of persistent pollutants in the environmen-
tal as well as bioaccumulation in the food chain of Arctic
mammals has been reported (Hung et al. 2010;OSPAR
2008; Rigét et al. 2010) and the northern areas are
continuously becoming more accessible for transport
and economic exploitation of mineral resources. There
is an international acknowledgement that countries out-
side the Arctic regions have an impact on the environ-
ment via air- and waterborne transport (LRTAP 2010).
The European Union (EU) is for instance developing an
Arctic policy based on the environmental and geopolit-
ical changes in the Arctic with the aim of supporting the
industrial development opportunities in an environmen-
tally sound way for the benefit of the European Arctic
population and citizens of the EU (Commission 2012).
In addition, the EU has qualified the impacts/effects of
human activities of the EU countries on the Arctic
environment in the Arctic Footprint and Assessment
Water Air Soil Pollut (2015) 226:150
DOI 10.1007/s11270-015-2416-4
Electronic supplementary material The online version of this
article (doi:10.1007/s11270-015-2416-4) contains supplementary
material, which is available to authorized users.
K. B. Pedersen :T. Lejon (*)
Department of Chemistry, University of Tromsø—The Arctic
University of Norway, Postbox 6050, Langnes, 9037 Tromsø,
Norway
e-mail: tore.lejon@uit.no
P. E . Jens e n :L. M. Ottosen
Arctic Technology Centre, Department of Civil Engineering,
Technical University of Denmark, Building 118,
2800 Lyngby, Denmark
project (Institute 2010). With respect to global sources
of pollution via long-range transport of pollutants and
effect on human health and the environment in the
Arctic, the Arctic Monitoring and Assessment Pro-
gramme (AMAP) of the Arctic Council focuses on
persistent organic pollutants (POPs), among these
polychlorinated biphenyls (PCB) and the heavy metals
Cd, Hg and Pb. Bioaccumulation of these priority pol-
lutants has been registered in mammals and humans in
the Arctic due to both local/regional and global sources
(AMAP 2002;Hungetal.2010). In addition to these
pollutants countries represented in the Arctic Council
include polyaromatic hydrocarbons (PAH), tributyltin
(TBT) and the heavy metals As, Cr, Cu, Ni and Zn as
priority pollutants (CCME; Danish EPA 2005; SFT
2007; USEPA). Research on the long-range transport
of these pollutants has not been extensive.
The increasing human activities in Arctic regions
such due to the economic exploitation increase the po-
tential local and regional environmental loads. The on-
going and expected increasing industrial development
especially within the mining, and oil and gas industries
in for instance Greenland, Northern Norway and NW
Russia, accentuates the need for continuously improv-
ing environmental management systems and technolo-
gies for minimising the environmental impact of the
increasing local/regional human activities. One area of
concern is the removal of pollutants that pose risk to
human health and the environment.
Harbours act as sinks for a wide variety of pollutants
caused by anthropogenic activities in the harbour as well
as on land. Examples of harbours located in Arctic
regions that have been exposed to several local sources
of pollution over the past 50–60 years are Hammerfest
in Northern Norway and Sisimiut in Greenland. In
Hammerfest, environmental investigations have re-
vealed complex composition of pollutants such as heavy
metals, PAH, PCB and TBT in the harbour sediments at
levels posing risk for human health and the environment
(Norwegian Environment Agency 2014). In Sisimiut,
high levels of Cd and Cu have been registered (Ottosen
and Villumsen 2006), investigations of organic pollut-
ants have however not been conducted. Hammerfest
harbour has been identified as one of the 17 harbours
of highest priority for remedial actions by the Norwe-
gian national action plan for polluted seabed (Ministry
of Environment 2007). In 2008, remedial actions to
remove and stabilise 1200 m
3
of polluted sediments
from part of the harbour were implemented (Norwegian
Environment Agency 2014). There however still remain
large areas of the harbour in need of remedial actions in
order to meet the environmental goals of Hammerfest
municipality. There are currently no remedial action
plans for the harbour in Sisimiut, however, due to the
increased national/international focus on the Arctic en-
vironment; similar remediation plans from the authori-
ties may be expected in the future.
Prior to implementing remedial action plans, it ap-
pears to be instrumental to identify the potential pollu-
tion sources to better understand and control/prevent
further pollution of the sediments. Statistical analyses
of the distribution of pollutants in relation to sediment
properties, e.g. grain size, content of organic matter and
buffer capacity, can extract trends linked to the pollution
sources. Principal component analysis (PCA) is a che-
mometric statistical tool for visualising the differences
and similarities in large data sets by calculating principal
components. These are mutually orthogonal vectors that
represent independent and uncorrelated variation of the
initial descriptors (pollutants/sediment properties), so
correlated descriptors are then described by the same
principal component. The systematic variation in the
data set can hence be simplified by using fewer new
descriptors than the original number of variables, and
this simplification is done without loss of systematic
information (Carlson and Carlson 2005).
Score plots are obtained by projecting the original data
onto the calculated orthogonal principal component vec-
tors. The influence of each original descriptor to the
principal component is reflected in a loading plot. De-
scriptors which have a strong contribution to the variation
depicted in the score plot are found far from the origin in
the loading plot. Positively correlated descriptors are
projected close to each other, while negatively correlated
descriptors are projected opposite to each other with
respect to the origin (Carlson and Carlson 2005).
ThePCAhaspreviouslybeenusedtoobtaininfor-
mation on pollutant distribution in sediment/soil/water
and to assess sources of pollution (Cheng et al. 2009;De
Luca et al. 2004;Fengetal.2014; Gao et al. 2013;Jan
et al. 2010). In some studies, PCA plots were used to
assess the distribution of PCB congeners and PAH com-
ponents in sediments and coupled with ratio calculations
of selected components, possible sources of pollution
were identified (Countway et al. 2003;Fengetal.2014;
Gao et al. 2013;Hartmannetal.2004).
The main focus of this study was to compare the
distribution of pollutants related to sediment properties
150 Page 2 of 15 Water Air Soil Pollut (2015) 226:150
for two harbours, Hammerfest and Sisimiut, located in
the Arctic for the assessment of possible differences in
pollution sources. This involved a preliminary chemo-
metric (PCA) assessment of the pollutant distribution
patterns in relation to sediment properties and in depth
evaluation of PCA plots of PAH components and PCB
congeners to evaluate possible pollution sources.
2MethodsandMaterials
2.1 Statement of Human and Animal Rights
The procedures and experiments undertaken in this
study were in accordance with the Helsinki Declaration
of 1975, as revised in 2000 and 2008.
2.2 Sample Collection
Sediments from Sisimiut, Greenland and Hammer-
fest, Norway were sampled from the top 10 cm of
the seabed using a Van Veen grab and were kept
frozen during transport and stored in a freezer until
analysed. The sediments were sampled at different
locations in the harbours based on potential land-
based pollution sources resulting in five sediments
from Hammerfest and four sediments from Sisimiut
sample points, and adjacent potential sources of pol-
lution are listed in Table 1.
Potential sources of pollution in Sisimiut include:
&Petrol station adjacent to the harbour (local oil spills,
leakage from pipes/tanks etc.)
&Fish factory adjacent to the harbour (discharge of
processed shrimp/crab with possible biomagnifications
of pollutants in shells)
&Former shipyard
&Discharge of untreated wastewater
&Discharge from boats
&Diffuse sources include boat traffic, urban run-off,
incineration of waste, district heating (limited use of
fossil fuels for energy production) and household
heating (stoves/oil boilers)
Potential sources of pollution in Hammerfest include:
&Petrol station adjacent to the harbour
&Former shipyard
&Discharge of untreated wastewater and sewage
&Outlet from freshwater lake, Storvatn, in
which elevated concentrations of PAH and
PCB in the lake sediments has been measured
(Akvaplan-Niva 2008)
&Fire of Hammerfest 1944 (in connection with the
withdrawal of the German occupation)
&Diffuse sources include boat traffic, district heating
(mostly sustainable energy sources and limited
incineration of waste), household heating (stoves/
oil boilers) and Melkøya (liquefied natural gas
processing station).
Based on the pollution sources in the two towns,
harbour sediments may be polluted by the following
pollutants; heavy metals, PAH, PCB and TBT. Disper-
sion pathways from land based sources include subsur-
face water, rainwater, cable routes, freshwater outlets
and snow melting (annually approximately 6 months
of snow cover in both towns). Dispersion pathways in
the harbour sediments include resuspension of sedi-
ments and marine species.
2.3 Analytical
Major elements and heavy metal concentrations (P, Al,
Ca, Fe, K, Mg, Mn, Na, V, Cr, Cu, Ni, Pb, Zn) were
measured based on digestion (Danish standard DS259).
Sediment dried at 105 °C (1.0 g) and HNO
3
(9 M,
20mL)wereautoclaved(200kPa,120°C,30min).
Solid particles were subsequently removed by vacuum
filtration through a 0.45 μm filter, and the liquid was
diluted to 100 mL. Metal concentrations in the liquid
were measured by Inductively Coupled Plasma–Optical
Tabl e 1 Sample points and potential sources of pollution
Harbour Sampling
point
Point sources of pollution
Hammerfest H_1 Former shipyard
H_2 Petrol station
H_3 Outlet from Storvatn (freshwater lake)
H_4 Sewage discharge
H_5
Sisimiut S_1 Former shipyard
S_2 Petrol station
S_3 Shrimp factory
S_4 Marina
Water Air Soil Pollut (2015) 226:150 Page 3 of 15 150
Emission Spectroscopy (ICP-OES) and are given as
milligram metal per kilogram dry matter.
Mercury, TBTand organic components (PAH16, PCB
and total hydrocarbons (THC)) were measured at a li-
censed laboratory, Eurofins in Moss, Norway. Mercury
was measured by Norwegian Standard NS 4768. PAH,
PCBandTHCweremeasuredbyISO/DIS16703.The
measurements included 16 PAH components and seven
PCB congeners, selected based on sediment quality
criteria for Denmark, Norway and OSPAR (Protection
of the Marine Environment of the North-East Atlantic).
The PAH components were acenaphtene, acenaphtylene,
anthracene, benzo(a)anthracene, benzo(a)pyrene,
benzo(b)flouranthene, benzo(k)fluoranthene,
benzo(ghi)perylene, chrysene, dibenzo(a,h)anthracene,
fluoranthene, fluorine, indeno(1,2,3-cd)pyrene, naphtha-
lene, phenanthrene and pyrene. The seven measured
PCB congeners were PCB28, PCB52, PCB101,
PCB118, PCB138, PCB153 and PCB180.
Chloride content was measured by agitating sedi-
ment (10 g) dried at 40
o
C with micropore water
(40 mL) for 20 h. Solid particles were removed by
0.45 μm vacuum filtration, and the chloride concentra-
tion was measured by ion chromatography. Measure-
ment deviation was ±10 %.
Carbonate content was measured by treating dried
sediment (5.0 g) with HCl (3 M; 20 mL), and the
developed CO
2
was measured volumetrically in a
Scheibler apparatus, calibrated with CaCO
3
.Measure-
ment deviation was ±15 %.
Organic matter was based on loss of ignition of dried
sediment (2.5 g) being heated at 550
o
C for an hour.
Measurement deviation was ±10 %.
Total Carbon (TC) and sulfur (S) were measured by
high temperature combustion. Dried sediment (0.5 g)
was combusted (1350
o
C) converting all carbon and
sulfide into carbon dioxide and sulfur dioxide, respec-
tively. The gasses were passed through scrubber tubes to
remove interferences, and the carbon dioxide and sulfur
dioxide were measured by infrared detector. Measure-
ment deviation was ±5-10 %.
Nitrogen (N) was measured by the Kjeldahl method.
Dried sediment (1.0 g) was heated to 370
o
CwithH
2
SO
4
(conc., 15 mL) and K
2
SO
4
(7 g) until white fumes were
observed (approx. 90 min) and subsequent to cooling
250 mL distilled water was added to the mixture. The
pH of the mixture was raised by adding NaOH (45 %),
and subsequently, the mixture was distilled and the
vapours were trapped in HCl (15 %, 85 mL). The
trapped vapour solution was subsequently titrated with
NaOH (5 M). Measurement deviation was ±10 %.
Cation exchange capacity (CEC) was measured by
extraction with NH
4
OOCCH
3
and subsequent cation
exchange with NaCl. Dried sediment (10 g) was agi-
tated with NH
4
OOCCH
3
(1 M, pH 7, 30 mL) for
5 min and subsequently centrifuged (2500 rpm,
10 min). The liquid was discarded and the step was
repeated two additional times. Subsequently, the step
was repeated two times using NH
4
OOCCH
3
(0.1 M,
30 mL). The sediment was then agitated with NaCl
(10 %, 20 mL) for 5 min and subsequently centrifuged
(2500 rpm, 10 min), and the step repeated three addi-
tional times. The liquids from all four NaCl treatments
were combined and diluted to 200 mL, and ammoni-
um content was measured by flow injection analysis.
Measurement deviation was ±10 %.
pH (KCl). Dried sediment (5.0 g) was agitated with KCl
(1 M, 12.5 mL) for an hour, and the pH was measured
using a radiometric analytical electrode. Measurement
deviation was ±1 %.
Conductivity. Dried sediment (5.0 g) was agitated with
distilled water (25 mL) for an hour, and the conductivity
was measured using a radiometric analytical electrode.
Measurement deviation was ±10 %.
Grain size was measured by wet sieving and dry
sieving. Wet sediment (75 g), distilled water (350 mL)
and Na
4
P
2
O
7
·10H
2
O (0.1 M, 10 mL) were agitated for
24 h. The slurry was then sieved through a 63 μmsieve
and the fraction above 63 μm was subsequently dried and
sieved for 15 min in a mechanical shaker using sieves with
screen openings of 0.063, 0.080, 0.125, 0.25, 1.0 and
2.0 mm. The slurry fraction below 63 μm was transferred
to Andreasen pipette for gravitational sedimentation.
Stoke’s law was used for estimating the time required
for particles to settle 20 cm and samples representing the
sizes40,32,16,8,4,2and1μmweremeasured.
Sequential extraction was made in four steps based
on the improvement of the three-step method (Rauret
et al. 1999) described by Standards, Measurements and
Testing Program of the European Union. Air-dried sed-
iment (0.5 g) was first extracted with acetic acid
(0.11 M, 20 mL, pH 3) for 16 h; secondly, extracted
with hydroxylammonium chloride (0.1 M, 20 mL; pH
2) for 16 h; thirdly, extracted with hydrogen peroxide
(8.8 M, 5 mL) for 1 h, followed by extraction at 85
o
C
150 Page 4 of 15 Water Air Soil Pollut (2015) 226:150
for 1 h, followed by evaporation of liquid at 85
o
C,
subsequently the cooled solid fraction was extracted
with ammonium acetate (1 M, 25 mL, pH 2) for 16 h;
and fourthly, digestion according to DS259 on the re-
maining solid particles was made, following the descrip-
tion above. Measurement deviation was ±5-20 %.
2.4 PCA Modelling
In this study, SimcaP11 Software was used for PCA of
the sediment properties and pollutant levels. Since the
values of the descriptors of the sediments varied in
magnitude, the data were logarithmically transformed
and subsequently centred and scaled to unit variance in
the calculated PCA models. The number of significant
components was determined by cross-validation.
3 Results and Discussion
3.1 Pollutant Levels in Harbour Sediments
The concentrations of heavy metals, organic pollutants
and TBT in the studied sediments are given in Tables 2
and 3and are compared to the assessment concentra-
tions (BAC) of OSPAR. The concentrations of all PAH
components and PCB congeners are provided in sup-
plementary material (Table 7). The BACs are based on
statistical calculations in which there is a 90 % proba-
bility that the observed mean concentration will be
below the BAC when the true mean concentration is
equivalent to the background concentration (BC)
(OSPAR 2009). OSPAR recommends using
hydrofluoric acid in metal analysis (digestion) in order
to dissolve all metal in the sediment matrix. Nitric acid,
though not as effective as hydrofluoric acid, was used in
this study due to health, safety and environmental con-
siderations, and the true concentrations may thus be
higher than registered. The BAC values are none the
less used for assessing pollutant levels in the sediments.
The concentrations of As, Cr and Ni are well below
BAC levels in all of the sediments and are assumed to be
equivalent to igneous levels. The concentrations of the
other heavy metals (Cd, Cu, Hg, Pb and Zn) exceed the
BAC levels in some or all of the sediments with up to 17
times the BAC (Fig. 2). Concentrations of the organic
pollutants (PAH, Benzo(a)pyrene (B(a)P), PCB exceed
the BAC levels with up to 500 times for the organics
(Fig. 2) and 1800 times for TBT (Table 3).
The sediment quality criteria of OSPAR do not include
THC, which nonetheless has been included in Table 3
since it is related to the organic pollutants and/or the
organic matter in the sediments. The THC content in all
of the sediments is mainly related to the fraction C
16
–C
35
and may be phytogenic rather than petrogenic hydrocar-
bons. The highest level of THC in Hammerfest was found
in sample H4, which was sampled adjacent to the former
sewage discharge point in the harbour (Table 1). Generally,
higher levels of THC were found in Sisimiut with the
highest concentrations found in the sediments sampled
adjacent to the shoreline (points S1, S2 and S3 in Table 1).
Elevated concentrations of PAH and PCB were
observed in all sample points in the two harbours
(Table 3,Fig.2). In Hammerfest, the highest concen-
trations were found in H4 adjacent to the former
sewage outlet. The highest concentrations of organic
Tabl e 2 Heavy metal concentrations in the sediments
Sample As Cd Cr Cu Hg Ni Pb Zn
mg/kg
H_1 6.3±0.8 0.13±0.03 15.2±0.1 116±39 0.31±0.01 9.5±0.4 48.6±3.6 82.8±6.0
H_2 4.0±0.5 0.25±0.14 8.4±0.3 33.1±2.5 0.92±0.02 5.1±0.3 220± 10 64.4± 5.9
H_3 5.0±0.3 0.27±0.04 22.7±0.5 54.3±9.9 0.54±0.01 14.8±0.4 46.3±1.1 140±7.5
H_4 21.0±0.7 1.10±0.14 46.5±11 167±29 1.19± 0.03 23.0± 0.8 152±44 537±72
H_5 5.9±0.4 0.14±0.03 24.3±0.7 46.8±1.3 0.32±0.01 15.3±0.7 41.7±2.4 94.0±6.5
S_1 18.7±0.2 0.54±0.05 37.1±1.2 216±8.9 0.30±0.01 18.3±0.5 72.8±3.7 343±21
S_2 8.5±0.3 0.70±0.09 24.0±1.6 125±3.8 0.10±0.02 13.0±1.4 38.6±4.1 239±12.4
S_3 9.2±0.1 0.38±0.06 25.2±3.7 184±39 0.09±0.01 18.0±6.2 57.1±6.0 957±173
S_4 3.3±0.1 0.09±0.02 10.0±1.3 42.2±4.2 0.01±0.00 6.0±0.5 7.8± 3.3 81.8± 10.1
OSPAR BAC 25.0 0.31 81 27.0 0.07 36.0 38.0 122
Water Air Soil Pollut (2015) 226:150 Page 5 of 15 150
pollutants in Sisimiut harbour were found adjacent to
the former shipyard (S1), the shrimp factory (S3) and
the petrol station (S2).
The concentration of Hg is generally high in Ham-
merfest harbour, especially at H2 (petrol station), H3
(freshwater lake outlet) and H4 (sewage discharge).
The concentrations of Cd, Cu, Pb and Zn are high at
the sewage discharge, which could indicate either
urban origin or that heavy metals have higher affinity
for organic matter. The concentration of Pb is in addi-
tion high in the vicinity of the petrol station (H2),
which might be due to earlier use of leaded gasoline
(Fig. 1). In Sisimiut, the concentrations of heavy
metals are generally low at the marina (S4), while high
levels of Cu were registered in the remaining sampling
points of the harbour and a high concentration of Zn
Tabl e 3 Concentrations of organic pollutants and TBT in the sediments
Sample PAH B(a)P PCB THC TBT
mg/kg μg/kg
H_1 6.2±1.9 0.50±0.13 0.08±0.02 410±123 1,800±720
H_2 4.6±1.4 0.34±0.09 0.03± 0.01 240±72 290±116
H_3 8.9±2.7 0.66±0.17 0.28± 0.07 380±114 71±28
H_4 70.0±21 4.30±1.1 0.55±0.14 1000±300 110±44
H_5 9.1±2.7 0.71±0.18 0.08±0.02 340±102 32±13
S_1 38.0±11 2.00±0.50 0.18±0.04 2300± 690 590±236
S_2 7.6±2.3 0.52±0.13 0.22± 0.05 1800±540 220±88
S_3 13.0±3.9 0.74±0.19 0.14±0.04 1600±480 160±64
S_4 10.0±3.0 0.55±0.14 0.02±0.003 330± 99 14±5.6
OSPAR BAC 0.36 0.03 0.001 1.0
B(a)P benzo(a)pyrene
Fig. 1 Pollutant concentrations compared to BAC in sediments from Hammerfest (H) and Sisimiut (S)
150 Page 6 of 15 Water Air Soil Pollut (2015) 226:150
was registered at the petrol station. The concentrations
of Cd and Pb in Sisimiut around or slightly elevated
compared to the BACs.
In both harbours, PAH, PCB, TBT, Cu and Zn
exceeded the sediment quality criteria and in Hammer-
fest Cd, Hg and Pb also exceeded the criteria. These
pollutants were hence the focus of this study.
It is worth noting that although POPs and TBT have
been observed in sediments of pristine areas in the
Arctic, the concentrations are much lower than those
registered in this study (Evenset et al. 2007;Evenset
et al. 2004;Harrisetal.2011;Jiaoetal.2009; Strand
et al. 2006; Viglino et al. 2004). The concentrations of
As, Cd, Cr and Ni in the sediments from the two har-
bours are equivalent to those found in remote areas
(Evenset et al. 2007; Lu et al. 2013). The previous
studies found that parts of the metal content originate
from global dispersion; however, levels are not signifi-
cantly higher than background levels (Evenset et al.
2007; Evenset et al. 2004). The concentrations of Cu,
Hg, Pb and Zn observed in remote Arctic areas, al-
though affected by global sources, are lower than con-
centrations of Cu, Hg, Pb and Zn observed in parts of the
harbours. Even though long-range transport of pollut-
ants has occurred to pristine areas in the Arctic, local
sources appear to have had larger impact on pollutant
levels in Hammerfest and Sisimiut harbours.
3.2 Sediment Characteristics
Ranges of the sediment characteristic in the two har-
bours of Hammerfest and Sisimiut are summarised in
Table 4. In general, the ranges in the sediment charac-
teristics are larger in Hammerfest than in Sisimiut,
which is accentuated by the PCA scores plot (Fig. 2)
with a larger dispersion of the Hammerfest sediments.
The two first components in the plot explain 70 % of the
variation in the sediment characteristics. In addition, the
scores plot illustrates that sediments from the same
Tabl e 4 Sediment characteristic
ranges in the sediments from
Hammerfest and Sisimiut
Characteristic Units Hammerfest Sisimiut
Carbonate %0.7–59 0.7–9
Organic matter %4.8–15 2.4–8.5
TC %3.1–10 1.1–5.3
S%0.2–1.2 0.3–0.8
N%0.01–0.5 0.1–0.5
CEC meq/100 g 2.4–13 0.7–4.3
pH 7.0–8.4 7.0–8.0
Conductivity mS/cm 7.8–20 5.6–10
Grain size
Clay (<2 μm) %4.3–8.9 0.8–8.8
Silt (2–63 μm) 12.2–38 5.0–52
Sand (63–200 μm) 54–77 38–90
Gravel (>200 μm) 0.3–22 0.6–4.0
Chloride mg/kg 6400–14,100 5700–7900
P645–3100 790–2900
Al 1900–8700 2500–6600
Ba 59–1340 42–160
Ca 4500–17,1000 6000–14,200
Fe 4300–18,600 5000–14,500
K950–4400 740–2300
Mg 4600–9000 1900–6000
Mn 40–130 40–110
Na 3800–15,500 2500–7200
V15–80 15–70
Water Air Soil Pollut (2015) 226:150 Page 7 of 15 150
harbour do not necessarily exhibit the same variation in
sediment characteristics.
The accompanying loadings plot (Fig. 2)illustrates
which sediment characteristics have strong contribu-
tions to the variations in the scores plot. All parameters
apart from Ba have an influence in the dispersion of the
first component (p1) whilethe strongest contributions to
the second component (p2) is related to grain size, Ca,
carbonate, Mg and C, as they are found far from the
origin in either dimension. The clustering of Al, Fe, K,
Mn, Na and chloride close to organic matter and silt
indicates a relation between these variables. The clus-
tering of Ca and carbonate close to gravel may be related
to shells and corals larger than 2 mm.
3.3 Distribution of Pollutants Related to Sediment
Characteristics
For both harbours loading plots (Fig. 3) show that the
major part of the target pollutants is clustered around
organic matter and/or finer grain sizes (silt/clay). In
Sisimiut, Zn may differ slightly from this trend,
which would be in line with the much higher level
registered adjacent to the petrol station (S3 in Ta-
ble 2). In Hammerfest TBT, Hg and Pb deviate from
the general trend which may be related to pollutant
sources and/or different binding patterns to the sedi-
ment. TBT is known to have higher affinity for or-
ganic matter, accordingly the deviation from this
trend in Hammerfest may be related to specific pol-
lutant sources rather than sediment properties, which
is in line with the highest concentration of TBT being
found adjacent to the former shipyard (H1); the ele-
vated concentrations of TBT in other parts of the
harbour (Table 3) may be due to general boat traffic.
Even though the use of TBT as a biocide in anti-
fouling was completely banned in 2008, TBT can
remain in eco-systems for many years; hence remain-
ing an environmental issue for the aquatic environ-
ment of harbours for many years to come.
Fig. 2 PCA score and loading
plot of sediment characteristics
150 Page 8 of 15 Water Air Soil Pollut (2015) 226:150
The loading plot for Hammerfest implies that PAH is
related to the organic matter in the sediments, and the
pollutant levels (Fig. 1) further support a point sourceof
PAH which may be related to sewage discharge (H4). In
Sisimiut, the same trend is not apparent, which may
indicate that the PAH pollution origins from several
diffuse sources such as harbour activities, urban run-
off, and to a lesser extent from long-range atmospheric
transportation. In both harbours, PCB is not closely
related to the content of organic matter indicating that
the PCB pollution in the sediments may be due to
several point sources as well as diffuse sources such as
urban run-off and to a lesser degree long-range atmo-
spheric transportation. A point source in Hammerfest
may be Storvatn, in which high levels of PCB have
previously been found in the sediments (Akvaplan-Niva
2008); high PCB levels were found adjacent to the
freshwater outlet in the harbour (H3 in Table 3).
In this study, the binding of heavy metals in the
sediments was assessed by determining the metal
partitioning by sequential extraction of the exchange-
able (including carbonates), reducible, oxidisable and
residual fractions. In order to investigate the possible
correlations between the heavy metals in each sedi-
ment fraction, PCAs were conducted applying the
metal/heavy metal concentrations in each fraction and
relevant sediment characteristics. Carbonate and CEC
were included in the exchangeable fraction and the
organic matter, TC, S and N were included in the
oxidisable fractions. The loading plots of metal con-
centrations in each fraction (not shown) did not reveal
any correlations between sediment characteristics and
metal concentrations, apart from carbonate and Ca and
to a lesser extent Mg.
Plotting of the different metal concentrations
against each other for each sediment fraction showed
correlations between some of the metals. Metals
which were correlated were different in the two har-
bours as well as in the different fractions and were
related to the mineral composition. It is interesting to
a b
cd
Fig. 3 PCA score and accompanying loading plots of sediment characteristics and pollutant levels in Hammerfest (aand b) and Sisimiut (c
and d)
Water Air Soil Pollut (2015) 226:150 Page 9 of 15 150
note that for both harbours correlations between Al,
Fe, K, Mg, Mn, Cr and Ni were found as exemplified
by Al-Ni correlation in the Hammerfest sediments
(Fig. 4). In addition, no correlations between major
elements and Cd, Cu, Hg, Pb and Zn were found
indicating different binding patterns in the sediment
implying that besides igneous content, these heavy
metals may also stem from anthropogenic sources.
This is also in line with the high concentrations found
in the sediments (Fig. 2). Based on PCA alone, it is
however not possible to evaluate the potential pollut-
ant sources. The environmental investigations howev-
er indicated that heavy metal pollution in both har-
bours is related to diffuse sources from both land-
and sea-based activities.
3.4 Distribution of PAH
The preliminary assessment of the PAH pollution in the
sediment indicated a point source in Hammerfest and
several, diffuse sources in Sisimiut. The ratios of the
selected PAH components have been widely used to
identify pollution sources in sediments (Countway et al.
2003;Fengetal.2014; Soclo et al. 2000; Yunker et al.
2002). In cases of mixed PAH pollution derived from
diffuse sources, the PAH ratios can be used for evaluat-
ing predominant sources, if such exist. The PAH ratio
antracene/(anthracene/phenantrene) has previously
been used as an indication for petrogenic (<0.1) and
pyrogenic (>0.1) sources (Soclo et al. 2000); the sedi-
ments from Hammerfest and Sisimiut all have values
above0.1 indicatingpyrogenic source(s) of PAHpollu-
tion (Table 5). The PAH ratios fluoranthene/(fluoran-
thene+pyrene) and indeno(123-cd)pyrene/
(indeno(1,2,3-cd)pyrene+ benzo(ghi)perylene) can in
addition indicate whether pyrogenic sources originate
from liquid fossil fuel combustion (0.4-0.5/0.2-0.5) or
coal/biomass combustion (>0.5/>0.5) (Feng et al.
2014). Calculations of these ratios (Table 5)giveam-
biguous results with no clear indication of combustion
sources,whichcouldbe due tomixed pollution sources,
for instance combustion from incineration plants and
fuel combustion from vehicles/vessels. It appears that
the PAH pollution in Sisimiut stems from mixed com-
bustion sources to a larger extent than in Hammerfest
(Table5).
Fig. 4 Correlation between the Al and Ni concentrations in the following fractions of the sediment: aexchangeable; breducible; c
oxidisable and dresidual
150 Page 10 of 15 Water Air Soil Pollut (2015) 226:150
To further assess the possible PAH sources, PAH ratios
of petrogenic and combustion sources based on data from
(Yunker et al. 2002) were compared to the PAH ratios of
the sediments (Fig. 5). The plot of the fluoranthene/(fluo-
ranthene+pyrene) ratio versus the indeno(123-cd)pyrene/
(indeno(1,2,3-cd)pyrene+ benzo(ghi)perylene) ratio indi-
cates that sources of the PAH pollution in the sediments of
both Hammerfest and Sisimiut are combustion of coal/
biomass rather than liquid fossil fuels.
According to Statistics Norway, the main sources of
PAH air emissions in 2012 were aluminium industry
(50 %), fuelwood (23 %) and traffic (15 %) (SSB2014),
and since the production of aluminium does not take
place in Hammerfest, it is not unlikely that the biggest
source of PAH pollution is from the combustion of
wood, and may partly include components from the
burning of Hammerfest town in 1944. In Sisimiut, the
pyrogenic sources may stem from present and past
incineration of waste and combustion of fuel from ve-
hicles or household heating by oil boilers.
3.5 Distribution of PCB
The preliminary assessment of the PCB pollution in
both harbours indicated diffuse sources such as urban
run-off and/or long range atmospheric transport. PCB is
expected to constitute part of the waste cycle for years to
come since PCB is still present in products and mate-
rials; e.g. cable insulation, thermal insulation materials,
paint, plastics, transformers, hydraulic oil; produced
before the production and use of PCB was prohibited
on a global scale more than 10 years ago. In addition,
several studies have revealed inadvertent production of
PCB congeners in the manufacturing of paint pigments
(Anezaki and Nakano 2014; Guo et al. 2014;Huand
Hornbuckle 2009; Shang et al. 2014).
In this study, seven of the 209 PCB congeners were
analysed (Table 6). Since the seven analysed PCB con-
geners in this study represent tri- (28), tetra- (52), penta-
(101, 118), hexa- (138,153) and hepta- (180)
chlorobiphenyls, the composition of these congeners
may reveal difference in the diffusive sources of PCB
pollution in the sediments. The PCA score plot of the
variation in the seven congeners of the sediments in
Hammerfest and Sisimiut (Fig. 6) reveals that H4 and
S4 stand out compared to the clustering of the sediments
Tabl e 5 PAH ratios of Hammerfest and Sisimiut sediments
An/(An+Phe) (Fl/Fl+ Py) Ip/(Ip+Bghip)
Ratio Source Ratio Combustion Ratio Combustion
H1 0.23 Pyrogenic 0.55 Coal/biomass 0.46 Fuel
H2 0.21 Pyrogenic 0.56 Coal/biomass 0.47 Fuel
H3 0.30 Pyrogenic 0.52 Coal/biomass 0.45 Fuel
H4 0.29 Pyrogenic 0.57 Coal/biomass 0.45 Fuel
H5 0.24 Pyrogenic 0.56 Coal/biomass 0.43 Fuel
S1 0.23 Pyrogenic 0.59 Coal/biomass 0.50 Coal/biomass
S2 0.21 Pyrogenic 0.58 Coal/biomass 0.49 Fuel
S3 0.24 Pyrogenic 0.61 Coal/biomass 0.52 Coal/biomass
S4 0.26 Pyrogenic 0.61 Coal/biomass 0.52 Coal/biomass
An anthracene; Phe Phenantrene; Fl fluoranthene; Py pyrene; Ip ideno(1,2,3-cd)pyrene; Bghip Benzo(ghi)perylene
Fig. 5 Comparison of PAH ratios of petrogenic and pyrogenic
sources; and the studied sediments. Petrogenic and pyrogenic PAH
ratio data from Yunker et al. 2002
Water Air Soil Pollut (2015) 226:150 Page 11 of 15 150
Fig. 6 PCA score plot of seven
PCB congeners in the
Hammerfest and Sisimiut
sediments
Tabl e 6 Composition of seven
PCB congeners in the harbour
sediments as well as in Aroclor,
Clophen, Svovol and Kanechlor
PCB mixtures calculated as per-
centage of the total PCB7, based
on data from (Hop et al. 2001;
Takasuga et al. 2005;USDepart-
ment of Health and Human
Services 2000)
AC Aroclor; KC Kanechlor
PCB mixture PCB28 PCB52 PCB101 PCB118 PCB138 PCB153 PCB180
H1 1 12 11 9 30 24 13
H2 1 12 10 6 29 26 16
H3 039 5312922
H4 159 5322918
H5 1138 7312614
S1 01619152718 6
S2 01021202518 5
S3 0172015211710
S4 32719191513 4
AC1016 65 35 0 0 0 0 0
AC1242 58 30 6 6 1 1 0
AC1248A 23 44 14 15 2 2 0
AC1248B 34 34 12 14 3 2 1
AC1254A 0 3 19 48 21 6 1
AC1254A 1 19 25 23 18 12 2
AC1260 0 1 10 2 21 29 37
Clophen A50 0 19 22 29 15 14 1
Clophen A60 0 3 13 8 28 29 19
Sovol 0 2 23 27 27 16 5
KC2001756118530
KC30085254220
KC400 22 42 16 12 4 3 0
KC500 1 13 26 19 23 17 1
KC1000 1 13 27 18 22 17 1
KC600 1 2 10 2 20 39 26
150 Page 12 of 15 Water Air Soil Pollut (2015) 226:150
with respect to the specific harbour. S4 has PCB pollu-
tion level a magnitude lower than registered in the other
Sisimiut sediments. The ratio of PCB180/PCB28 is
approximately 1 for S4 and 24–30 for the other sedi-
ments in Sisimiut indicating lower relative content of the
more highly chlorinated biphenyls.
As was the case with PAH, H4 displays different
variation in the composition of PCB indicating different
sources or sediment binding/degradation than for the
other sediments in Hammerfest. The preliminary assess-
ment revealed that there was not a clear relation between
organic matter and PCB, which could indicate that PCB
is dispersed differently than PAH, and there may be
additional sources to sewage discharge at H4. Disper-
sion from Storvatn could be a source, which would
explain that H3 (Storvatn outlet) is situated closer to
H4 in the PCA plot than the other sediments.
The commercially produced PCB mixtures contained
different compositions of PCB congeners according to
their use. The PCA has been used in several studies for
comparing specific PCB mixture compositions with
observed PCB pollution in sediments to assess which
commercial mixture(s) the PCB pollution may originate
from (Hartmann et al. 2004; Zhang et al. 2007). In this
study, the seven analysed PCB congeners in the nine
sediments were compared to the composition of the
following PCB mixtures (Table 6): Kanechlor
(manufactured in Japan), Aroclor (US, UK), Clophen
(Germany) and Svovol (Russia).
The PCA score plot of the commercial PCB mixtures
and the harbour sediments indicate that the PCB pollu-
tion in Hammerfest is mainly related to Clophen A60
and Sovol (Fig. 7). This is in line with a study of 64 PCB
congeners in Storvatn, in which the major part of the
PCB pollution (approximately 82 %) was found to be
related to Clophen A60, Aroclor 1254, Aroclor 1260
and Sovol (Akvaplan-Niva 2008). This further implies
that applying the seven PCB congeners in this study can
be used in PCA for qualitative indications of PCB
mixture sources. The PCB pollution in Sisimiut is clus-
tered in a different part of the PCA score plot (Fig. 7)
and appears to be related to Kanechlor 500, Kanechlor
1000, Sovol and Aroclor 1254. Whether the relation to
the Kanechlor and Sovol mixtures is due to long-range
atmospheric or local emissions of products
manufactured with the Russian/Japanese mixtures is
not clear and further analysis to confirm/rule out such
indications entails analysis of more PCB congeners.
4 Conclusion
The preliminary PCA assessment based on concentra-
tions of heavy metals, PAH, PCB and TBT and respec-
tively the sediment characteristics indicated different
sources and pollutant distribution in the two harbours.
One exception was TBT which was not found to be
related to sediment characteristics, indicating point
sources resulting in locally high TBT concentrations.
In both harbours, TBT concentrations were highest; up
to 1800 times the non-polluted level; in sediments adja-
cent to the former shipyards.
The in depth PAH, source analyses were based on
both a PAH ratio assessment and PCA and indicated that
Fig. 7 PCA score plot of the
seven PCB congeners of the
Hammerfest and Sisimiut
sediments compared to
commercial PCB mixtures
Water Air Soil Pollut (2015) 226:150 Page 13 of 15 150
the predominant source of PAH pollution in both har-
bours was pyrogenic coal/biomass. This was in line with
the second largest PAH air emissions in Norway being
related to wood combustion. PCA of PAH composition
indicated that the PAH pollution in the two harbours
may origin from diffuse as well as point sources such as
sewage discharge.
The PCB composition (seven congeners) in the sed-
iments was compared to commercial PCB mixtures in a
PCA plot. The PCB pollution in Hammerfest was found
to mainly be correlated to European, Russian and Amer-
ican manufacturers, while the PCB pollution in Sisimiut
was related to other PCB mixtures manufactured in the
US, Russia and Japan. PCA of the PCB congeners in the
sediments indicated several diffuse sources of pollution.
Although long-range transport of POPs, TBT and
metals has previously been established, the concentration
levels of pollutants in this study were higher than those
reported in pristine areas of the Arctic, indicating that
local sources were more significant than global sources.
The study showed that PCA can be used as an im-
portant tool, along with pollutant levels and mapping of
potential sources, for identifying pollutant sources and
differences in pollutant composition in relation to sedi-
ment characteristics.
Acknowledgments The Northern Environmental Waste Man-
agement (EWMA) project, which is funded by the Research
Council of Norway through NORDSATSNING (grant number
195160) and Eni Norge AS, is acknowledged for funding. Ham-
merfest municipality is acknowledged for providing boat and
assistance in sampling of sediments in Hammerfest. Tore Lejon
and Kristine B. Pedersen acknowledge The Arctic Technology
Centre at DTU for funding the trip to Greenland and in addition
the technical staff is acknowledged for assistance with sampling
and sediment analyses.
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