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In order to investigate the long-term fate of petroleum hydrocarbons in salt marsh sediments in Wild Harbor (West Falmouth, MA) impacted by the Florida spill of 1969, 26 sediment cores were collected and analyzed for total petroleum hydrocarbons (TPH). The results from this effort indicate that the distribution of petroleum hydrocarbons is spatially heterogeneous, oil compounds are generally located at sediment depths of 4 to 20 cm in areas closest to the banks of the marsh, and ∼ 100 kg of petroleum residues can be found to persist in intertidal sediments that were originally the most impacted.
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Environmental Forensics, 6:273–281, 2005
Copyright C
Taylor & Francis Inc.
ISSN: 1527–5922 print / 1527–5930 online
DOI: 10.1080/15275920500194480
The West Falmouth Oil Spill: 100 Kg of Oil Found to Persist
Decades Later
Emily E. Peacock,1Robert K. Nelson,1Andrew R. Solow,1Joseph D. Warren,2Jessica L. Baker,3
and Christopher M. Reddy1
1Woods Hole Oceanographic Institution, Woods Hole, MA, USA
2Southampton College, Long Island University, Southampton, NY, USA
3GeoNet Systems, Bournedale, MA, USA
In order to investigate the long-term fate of petroleum hydrocarbons in salt marsh sediments in Wild Harbor (West Falmouth, MA)
impacted by the Florida spill of 1969, 26 sediment cores were collected and analyzed for total petroleum hydrocarbons (TPH). The
results from this effort indicate that the distribution of petroleum hydrocarbons is spatially heterogeneous, oil compounds are generally
located at sediment depths of 4 to 20 cm in areas closest to the banks of the marsh, and 100 kg of petroleum residues can be found
to persist in intertidal sediments that were originally the most impacted.
Keywords: Florida spill, West Falmouth, No. 2 fuel oil, petroleum hydrocarbons, sediments
For the past three decades, the West Falmouth oil spill has in-
fluenced and shaped our understanding of post-spill environ-
mental impacts and developed the science of oil spill research
in the marine environment (Blumer et al., 1970, 1971; Blumer
and Sass, 1972a, 1972b; Burns and Teal, 1979; Frysinger et al.,
2003; Hampson and Sanders, 1969; Krebs and Burns, 1977;
Reddy, 2004; Reddy et al., 2002; Sanders et al., 1980; Slater et
al., 2005, Teal et al., 1978, 1992; White, Reddy, et al., 2005).
This spill occurred when the barge Florida went aground near
West Falmouth, Massachusetts, and released 700,000 l of No.
2 fuel oil into Buzzards Bay on September 16, 1969 (Figure 1).
Immediately after the spill, scientists at Woods Hole Oceano-
graphic Institution began to analyze samples from impacted
sediments and biota using state-of-the-art analytical technol-
ogy, mainly packed-column gas chromatography (Blumer et al.,
1970). These analyses revealed that petroleum hydrocarbons
could be acted upon by a series of weathering processes in-
cluding evaporation, water-washing, and microbial degradation
but also could persist for at least several years in salt marsh
sediments (Blumer et al., 1972b).
The environmental fate of the spilled oil was intensively stud-
ied for the first seven years after the spill (Blumer et al., 1970,
1971; Blumer and Sass, 1972a, 1972b; Burns, 1975; Burns and
Teal, 1979; Michael et al., 1975; Teal et al., 1978) and then
Received 3 January 2005; accepted 23 May 2005.
Address correspondence to Christopher Reddy, Department of
Marine Chemistry and Geochemistry, Woods Hole Oceanographic In-
stitution, Woods Hole, MA 02543, USA. E-mail:
some sites were revisited 20 (Teal et al., 1992) and 30 years
(Frysinger et al., 2003; Reddy et al., 2002) later. All of these
studies demonstrated that petroleum hydrocarbons did persist for
many years in the intertidal salt marsh sediments of Wild Harbor
(Figure 1), where no human intervention or cleanup was done
after the spill except for water-based emulsifiers applied imme-
diately after the spill. While investigating intertidal marsh sedi-
ments collected in 2000 at the M-1 site in Wild Harbor (Figure
1), Reddy et al.(2002) were also able to provide a highly re-
fined inventory of existing petroleum hydrocarbons using com-
prehensive two-dimensional gas chromatography (GC ×GC).
This novel technology showed that after three decades of expo-
sure to in situ degradative processes, only the n-alkanes were
completely degraded. However, despite some degradation, all
other compound classes typical of No. 2 fuel oil could still be
identified in the sediments at this site (Reddy et al., 2002). Be-
cause of the potential fears associated with the long-term haz-
ards of petroleum hydrocarbons in the marine environment, the
latter results attracted attention by the mainstream media and
comment by the scientific community. Owens (2003) criticized
this work (Reddy et al., 2002) by stating that only one loca-
tion (M-1) from the whole impacted area was investigated and
that likely much of the original cargo had dissipated. Reddy
et al. (2003) responded to Owens’s comments by stating that
their study was originally focused on only sediments at the
M-1 site because it was one of the most studied and contam-
inated sites. Nevertheless, Owens was correct that additional
sediment cores from a wider area would need to be collected
and analyzed before drawing conclusions about the long-term
fate of the total amount of petroleum released from this
274 E. E. Peacock et al.
Figure 1. Map of general area near the grounding of the Florida.
To address Owens’s comments as well as to continue to
study this oil spill, we surveyed Wild Harbor marsh sediments
for petroleum hydrocarbons. Twenty-six cores from intertidal
marsh sediments on the west and east sides of the Wild Harbor
River were collected and analyzed for petroleum hydrocarbons
(Figure 2). These analytical results were evaluated horizontally
and vertically in order to characterize the spatial distribution
of remaining petroleum in the impacted marsh sediments. The
Figure 2. Map of the study area. Marker size represents the maximum
TPH content (mg g1) found at each sample location, which was generally
at 12–16 cm. All of the core locations are within the intertidal zone.
data were then analyzed using two independent models aimed at
quantifying the volume of petroleum remaining in these sed-
iments. Finally, these results were compared to the volume
of petroleum released during the spill in order to estimate what
percentage of petroleum originally released persists in these im-
pacted sediments.
Sediment Collection
From November 2002 to March 2004, 26 sediment cores were
collected from intertidal Wild Harbor marsh sediments. Methods
for collecting and splitting sediment cores from this marsh have
been discussed previously (Reddy et al., 2002). Briefly, a 9.5-cm
diameter PVC tube was pushed into the sediments. The area
around the tube was cleared with a shovel and then the tube
was removed and capped. The core was returned immediately to
the laboratory and frozen at 40C. After a brief thaw, the core
wasextruded at 4-cm intervals from 0–4 to originally 44–48 cm.
(However after analyzing several of the first cores collected and
finding that oil was usually limited to depths of 0 to 24 cm, we
then only analyzed sections in the 0–4 to 20–24 cm horizons.)
The outer one centimeter of each core was discarded in order
to avoid cross-contamination. Each sample was placed in pre-
combusted glass jars with Teflon-lined caps and frozen until
Total Petroleum Hydrocarbons (TPH) Analysis
Three to nine grams of air-dried sediment were spiked with
40 µgofhexatriacontane (n-C36) and extracted with a 9:1
dichloromethane (DCM):methanol mixture by pressurized fluid
extraction (100C, 1000 psi). Extracts were reduced in volume,
solvent exchanged into hexane, and charged onto a glass col-
umn (9 cm ×0.4 cm) packed with fully activated silica gel
(100–200 mesh). The column was eluted with 12 ml of a 3:1
mixture of hexane: DCM. The extract was then treated with ac-
tivated copper to remove elemental sulfur and dried with sodium
sulfate. Finally, the extract was spiked with stearyl palmitate (40
µg) and analyzed on a Hewlett-Packard 6890 Series gas chro-
matograph with a cooled injection system (CIS) and interfaced
to both a Hewlett Packard 5973 mass spectrometer and flame
ionization detector (FID). A 1-µL sample was injected splitless
into the CIS, which was temperature programmed from 40 (0.1-
min hold) to 350Cat720min1(8 min hold). Compounds
were separated on a glass capillary column (J&W DB-5MS,
60 m, 0.32-mm i.d., 0.25-µm film thickness) with He as the
carrier gas at a constant flow of 1.5 mL min1. The GC oven
temperature was programmed from 40 (1-min hold) to 80Cat
20min1and then from 120 to 320Cat5
hold). The TPH were quantified by integrating the total FID
area of the unresolved complex mixture (UCM) and using re-
sponse factors determined from No. 2 fuel oil standards. The
carbon range of the UCM was variable but always existed be-
tween decane (n-C10) and hexacosane (n-C26), which excludes
The West Falmouth Oil Spill Decades Later 275
most of the larger, biogenic hydrocarbons. Because a subsample
of the original Florida cargo oil is no longer available, we used
the Marine Ecosystem Research Laboratory (MERL) No. 2 fuel
oil as a calibration standard (Reddy et al., 2002). We believe
that the uncertainty of using a fresh oil as a calibration stan-
dard for a weathered oil is minimal, as an FID is based on the
mass of carbon combusted, which should be relatively insensi-
tive to the chemical nature of hydrocarbons (Reddy and Quinn,
1999). In addition, we assume that most, if not all, of the hydro-
carbons in our operationally defined term for TPH is from the
Florida spill. Laboratory blanks of combusted sand were free of
petroleum compounds. Recoveries of No. 2 fuel oil spiked into
combusted sand and analyzed were 70 to 115% with an average
of 95%. Precision, based on the preparation and analysis of four
duplicate pairs of samples, ranged from +0.1 to 10%. Our esti-
mated method detection limit is 0.015 mg of TPH per gram of
dry sediment (Reddy et al., 2002).
Results and Discussion
Overall of Results
To determine the extent and distribution of TPH in Wild Harbor,
we chose to study the boxed area in Figure 1, which is magni-
fied in Figure 2. All of the cores were collected in the intertidal
regions of the marsh. We chose to investigate this area in Wild
Harbor based on historical results (Teal et al., 1992) and un-
published work from our laboratory, which showed that only
sediments from intertidal, and not subtidal, areas has detectable
petroleum hydrocarbons. As the study continued over more than
ayear, additional core locations were selected for analysis based
on our available data. It was found early in this survey that the
TPH content in marsh sediments farther from the Wild Harbor
River channel were minimal so more emphasis was placed on
areas nearest to the shoreline. Because of the sporadic distribu-
tion of the contamination, it is possible that some contaminated
pockets of the marsh were missed. However, based on 30 years
of historical data and all of the new data from numerous sta-
tions that had not been previously sampled, we believe all of the
hot spots have been included in this study. In total, 150 sed-
iment samples were analyzed from 26 sediment cores. (Please
note that only data for 22 cores are shown in Figure 2. The four
other cores were outside the study area shown in Figure 2 and
contained very little or no TPH). In terms of TPH content, the
values vary widely between locations and had a UCM eluting
in the range of n-C10 and n-C26,which is typical of partially
weathered No. 2 fuel oil. Core F (Figure 2) had no detectable
TPH (i.e., no detectable oil residues). Thirteen cores contained
sediments with TPH concentrations greater than 1 mg per gram
of dry sediment (mg g1). Of those, six sediment cores had max-
imum TPH values ranging from 1 to 4 mg g1and the remaining
seven sediment cores had TPH values that ranged from 4.6 to
14.1 mg g1. Core H, which was collected in the same vicinity
of the historical sampling site M-1, had a very similar TPH con-
tent as a core collected at M-1 in August 2000 (Reddy et al.,
Spatial Trends
Spatially throughout the marsh on the west side of the river,
sediments from cores in closer proximity to the water contained
higher TPH concentrations than the sediments obtained from
cores farther from shore (Figure 2). For example, sediments
from core G contained TPH concentrations about an order of
magnitude less than sediments from core H, while sediments
from core F had no detectable TPH (Figure 2). This difference
in TPH content at three sites occurs over a short distance of
only 10 meters indicating that oil contamination has not spread
laterally since the spill. The best supporting evidence for this
conclusion are photographs of the marsh taken immediately after
the spill. The photos reveal that a 2-wide band of oil had sorbed
to the intertidal marsh sediments closest to the banks of the river.
Hence, areas that were the most contaminated shortly after the
spill continue to be the most impacted three decades later. On
the east side of the river, a similar trend was observed. Cores N,
P, Q, T, and S outline a localized hot spot with higher TPH values
in sediments collected closest to the channel. In this area, which
had not been previously sampled, there is a visible depression
in the marsh surface. Assuming this depression existed at the
time of the spill, finding elevated TPH concentrations in these
sediments is consistent with the hypothesis that the horizontal
distribution of sedimentary TPH concentrations is related to the
original deposition of oil in this area.
Vertical Trends
Ve r tically, the maximum TPH value for each sediment core was
consistently between 4 and 20 cm below the surface (see Figure 3
to view four down-core profiles) and most frequently observed
in the 8–12 or 12–16 cm horizons. These depths are reasonably
consistent with the timing of the spill (1969) and an estimated
sedimentation rate of 0.35 cm yr1(White, Reddy et al., 2005).
The concentrations of TPH that were found in sediments above
(i.e., in surface 0 to 4 cm) and below (20–24 cm) the mid-core
maximums were relatively minimal. Several of the initial cores
were analyzed to a depth of 48 cm, and no oil was detected be-
low 20 cm. The analysis of subsequent cores was then limited
to a depth of 24 cm, despite the presence of oil in the 20–24 cm
horizon in some samples. The maximum depth of detectable
TPH varied, which could be attributed to either a difference in
marsh conditions or compaction of sediments during sampling.
The shape of the UCM and the presence of resolved peaks on
the UCM hump (Figure 4) varied substantially with depth be-
tween cores, suggesting a depth-dependent variance in the nature
of the petroleum hydrocarbons in these sediments. Preliminary
GC-MS and GC ×GC analysis of some samples indicate that the
composition of the UCM differs as depicted by the shape of the
UCM hump, thus supporting our hypothesis. Mechanistically,
we believe the latter results from post-depositional movement
of oil compounds based on their different abilities to partition
between the pore water and sediment organic matter, a hypoth-
esis that is evaluated and discussed elsewhere (White, Xu et al.,
276 E. E. Peacock et al.
Figure 3. Typical down-core concentration profiles of TPH at Wild Harbor
from locations denoted in Figure 2 as: (a) Core H, (b) Core S, (c) Core E,
and (d) Core D.
Estimating the Total Oil Remaining in the Marsh
The main objective in this study was to estimate the total amount
of oil remaining in the east and west sides of the marsh. To ac-
complish this task, the total amount of oil (identified as TPH)
present in each side of the channel was volumetrically integrated.
In order to account for the low statistical power caused by a less
than ideal number of cores collected from the study area, two
independent approaches were developed and used to estimate
Figure 4. GC-FID chromatograms of Wild Harbor marsh sediment extracts
from Core E: (a) 0–4 cm, (b) 4–8 cm, (c) 8–12 cm, (d) 12–16 cm, (e) 16–
20 cm, and (f) 20–24 cm. The peaks annotated with * and ** are standards.
Besides the standards, compounds eluting after n-C26 are biogenic hydro-
carbons (see Reddy et al., 2002).
this value (Davis, 2002). Our reasoning is that by using inde-
pendent lines of evidence to arrive at the same objective, if these
two values are similar, we obtain a higher degree of confidence
in the calculated volume of petroleum remaining in these marsh
The first approach involved the use of a grid and three-
dimensional interpolation to calculate the volumes. First, all of
the data from the cores were entered into a three-dimensional
grid, which considered an area created by a multisided polygon
of the outer perimeter of the cores. Pixel sizes in the grid were
approximately 1m ×1m in the horizontal dimension and 0.02
minthe vertical. A three-dimensional, isotropic, linear interpo-
lation algorithm (MATLAB, The Mathworks, Inc.) calculated
the oil content at each point in the grid that did not have core
data. These data were then integrated volumetrically to produce
an estimate of 22 kg of TPH still present in the intertidal sedi-
ments on the east side and 15 kg of TPH remaining in the inter-
tidal sediments on the west side for the areas sampled. Unfortu-
nately, this method does not allow a means to confidently predict
The second approach involves a statistical method that in-
corporates our data set and allows for estimating the total oil
remaining and the uncertainty involved. First, the TPH con-
tent throughout each sediment core was integrated over a 24-cm
depth (Figure 5). We then assumed that the TPH (or oil) content
in each core was homogeneous within one square meter, which
we call Y(x)where xis the two-dimensional location of each
core. The total amount of material contained within our study
region R,the boxed regions in Figure 5, is:
Y(x)dx (1)
The West Falmouth Oil Spill Decades Later 277
Figure 5. Map of the study area with the TPH content (g m2) listed for
each sample location. This was accomplished by integrating the total oil
found in each core from 0 to 24 cm depth of each sample. Hence, Core
E (see Figure 2) was estimated to have 350 g of TPH per m2in the top
24 cm.
Interest centers on estimating YRfrom concentrations
Y1,Y2,...,Ynmeasured at sample locations x1,x2,...,xn.
To estimate YRefficiently and particularly to give some mea-
sure of uncertainty about it, we will assume that Y(x) has an ln
normal distribution with parameters µ(x) and σ2. These param-
eters represent the mean and variance of log Y(x). The corre-
sponding mean and variance of Y(x) are:
β(x)=exp µ(x)+σ2
τ2(x)=(exp σ21) exp[2µ(x)+σ2] (3)
It follows that an estimate of YRis given by:
exp ˆµ(x)+ˆσ2
2dx (4)
where ˆµ(x) and ˆσ2are estimates of µ(x) and σ2, respectively.
To estimate µ(x) and σ2,wewill assume that:
where µoand µ1are unknown parameters and |xxo|is the
distance between location xand an unknown location xo. Under
this model, which was chosen on the basis of some preliminary
analysis of the data, mean ln TPH content declines linearly—and
mean TPH content declines exponentially—with distance from
the location xo(Figures 5 and 6). The model can be written as:
log Y(x)=µo+µ1|xxo|+ε(x) (6)
where ε(x)isanormal error with mean 0 and unknown variance
σ2.Forfixed xo, this model can be fit by simple linear regression.
Let ˆµo(xo) and ˆµ1(xo)bethe corresponding regression estimates
of µoand µ1, respectively, and let RSS(xo)bethe corresponding
residual sum of squares. The final estimate ˆ
xois the value of
xothat minimizes RSS(xo) and the final estimates of µo,µ1,
and σ2are µo(ˆ
xo), µ1(ˆ
xo),and RSS(ˆ
xo)/(n2), respectively.
It is possible to go beyond point estimation of YRto provide a
measure of uncertainty. Specifically, provided the scale of any
Figure 6. Plot of the ln of TPH mass (mg) in each sediment core versus
distance from ˆ
xo: (a) west side and (b) east side of Wild Harbor marsh. The
TPH content in each core was calculated by multiplying the area of each
core barrel (0.0708 m2)bythe values shown in Figure 5 and converting to
278 E. E. Peacock et al.
spatial correlation in TPH content is small compared to the scale
of R:
Va r Y R
τ2(x)dx (7)
where τ2(x)isgiven in (3). An estimate ar YRof the variance
in (7) can be found by replacing µo,µ1, and σ2in the expression
for τ2(x)bytheir corresponding estimates.
The statistical method described above estimated that there is
52 and 45 kg of oil (as TPH) that can be found in the sediments
on the east and west sides, respectively, for the study region R.
The uncertainties for the east and west sides were very good and
were +2 and 6 kg, respectively. The location of ˆ
xois depicted
in Figure 5. Shown in Figure 6 is the fit of the model for the two
data sets. These two independent approaches for estimating the
mass of oil (as TPH) remaining in these marsh sediments give
values that are within the same order of magnitude. However,
the statistical model yielded estimates that were approximately
three times larger than the linear interpolation approach. One
factor for this discrepancy was the study region for the statis-
tical model was 200% larger than the linear interpolation ap-
proach because the former required a simple rectangular study
area whereas the latter used a multi-sided polygon that enclosed
and only considered the area within the core locations. Hence,
the linear interpolation approach assumed a zero TPH content
beyond the outer perimeter of the polygon. Nevertheless, both
results reveal that a small fraction of oil can be found compared
to the original 595,000 kg of original product that spilled in Buz-
zards Bay. (This mass was calculated by using a specific gravity
of 0.85 and volume of 700,000 l).
Fate of Oil in Wild Harbor Since the Spill
For further discussion, we have chosen to use the larger estimate
from the statistical model because it provided an uncertainty and
because some oil in the sediment may have been missed in our
field sampling. Hence, less than 0.02% of the total original cargo
that was spilled (100 kg for both sides) was found in the inter-
tidal sediments of Wild Harbor. It is important to note that the
amount of oil that initially entered Wild Harbor is not known and
a significant amount of the original product likely evaporated or
was transported offshore within the first few weeks of the spill
(Reddy and Quinn, 2001). For example, 20, 30, and 50% of
product evaporated days to months following spills of the Exxon
Valdez (Wolfe et al., 1994), Amoco Cadiz (Gunlach et al., 1983),
and Jessica (Kingston, 2002), respectively. In May 1970, eight
months after the spill, an estimated four tons of oil still remained
in Wild Harbor (Blumer et al., 1971). Although it is unclear how
this value was calculated, only about 3% of that is remaining; it is
difficult to accurately account for all of these losses. The major-
ity of oil was probably lost in the subtidal sediments, which were
originally heavily oiled but are now relatively free of residues
from this spill. However, some of the petroleum hydrocarbons
were also removed in the intertidal sediments and evidence of
this can be observed in traditional one-dimensional packed-
column GC-FID chromatograms of sediment extracts from the
early to mid 1970s (Burns, 1975; Burns and Teal, 1979). These
chromatograms document the loss of lower molecular weight
compounds, presumably from water washing/evaporation, and
resolved compounds from biodegradation. By assuming that
each compound in these chromatograms has a similar FID re-
sponse and comparing the vintage GC chromatograms to recent
GC chromatograms, we estimate that 20 and 10% of the mass
of hydrocarbons in the intertidal sediments were removed due to
water-washing/evaporation and biodegradation, respectively,
since 1970. Despite this large estimated decrease since 1970,
concentrations of petroleum hydrocarbons in leftover hot spots
in intertidal sediments, such as M-1, are similar to values de-
tected in the mid 1970s (although analytical methods may cause
slight differences) and suggest that the most oiled locations have
persisted the most. This is consistent with our work at M-1,
where we believe that the removal of phytane and potentially
other saturated, branched compounds has not significantly ad-
vanced in the last two decades (Reddy et al., 2002). Obviously,
these results also need to revolve around the subjects of scale and
recovery. Only a small amount of oil exists in a small area but
at high concentrations. Most of Wild Harbor and Buzzards Bay
does not contain any oil residues from the Florida spill. Blumer
et al. (1971) showed that 8km
2of Buzzards Bay was initially
oiled after the Florida grounding. Our recent study indicates that
0.001 km2of salt marsh (Figure 2) have detectable residues
three decades later, which corresponds to 0.01% of the original
area impacted. Visually, the marsh appears quite healthy, but
studies are now underway to determine whether any plants or
animals continue to be affected.
Why Do Petroleum Residues Continue to Persist
in Wild Harbor?
While other types of shorelines can retain petroleum residues
for several years after a particular oil spill (Hayes and Michel,
1999), numerous studies and reviews have revealed that marshes
are the most capable of long-term oil preservation (Kingston,
2002; Table 1). For example, Baker (1999) compared numer-
ous spills and different shorelines; she illustrated that sheltered
salt marshes, including Wild Harbor, have the longest recovery
times after an oil spill. Consider Winsor Cove marsh sediments,
which are just 4 km away from Wild Harbor and were contam-
inated in 1974 when the Bouchard 65 spilled an undetermined
amount of No. 2 fuel oil. Recent analysis of Winsor Cove shows
persistent contamination, with most of the oil residing in the
top 3 cm (Reddy, 2004). Crude oil spilled by the Amoco Cadiz
on March 16, 1978, was found in the Ile Grande salt marsh in
France after 13 years. The levels there were generally low, with
localized areas of higher amounts of weathered oil, also an at-
tribute of the remaining oil in Wild Harbor (Mille et al., 1998).
Long-term studies of the sheltered lagoon, Black Duck cove in
Chedabucto Bay, Nova Scotia, where the tanker Arrow spilled
The West Falmouth Oil Spill Decades Later 279
Ta bl e 1. Examples of oil spills with petroleum residues persisting for more than 5 years
Name of vessel Date of spill Location Type of coastline Type of oil Size of spill What is left
Florida September
Buzzards Bay,
Salt marsh No. 2 fuel oil 700,000 l After 30 years, TPH values are
similar to values observed in
mid 1970s (Reddy et al.,
2002). Only n-alkanes
completely degraded
(Frysinger et al., 2003).
Arrow February
Chedabucto Bay,
Nova Scotia,
Beach with sand
and cobbles
Bunker C 2 million l After 22 years, n-alkanes were
mostly lost, and target PAHs
were degraded. Triterpanes
and steranes remain (Wang
et al., 1994).
Metula August 1974 Straight of
Marsh and beach Light Arabian
50,000,000 l light
Arabian Crude
and 2,000,000
l Bunker C
After 24 years, lightly weathered
oil in one marsh and heavily
weathered in one marsh and
one beach, with most
compounds including
biomarkers showing some
degradation (Wang et al.,
Bouchard 65 October 1974 Buzzards Bay,
Salt marsh No. 2 fuel oil 42,000–140,000 l After 30 years, partially
weathered diesel fuel remains
with moderate biodegradation
(Reddy, 2004)
Amoco Cadiz March 1978 Ile Grande Salt
Marsh, North
Coast of
Salt marsh,
Rocky and
sandy beaches
Crude, Iranian,
and Arabian
223 million l After 13 years, hydrocarbon
levels were generally low, with
localized areas of highly
weathered oil in the marsh.
Biomarkers remain (terpanes,
steranes, and diasteranes)
(Mille et al., 1998).
Ruptured storage tank April 1986 East Coast of
Panama, near
seagrasses, and
coral reefs
crude oil
12–16 million l Exposed oil weathered rapidly,
while oil protected under
sediments retained most
compounds after 5 years
(Burns et al., 1994).
Exxon Valdez March 1989 Prince William
Sound, Alaska
Wide variety of
Alaskan North
Slope Crude
42 million l Boulders and cobbles continue to
protect oil in the intertidal
zone, inhibiting disturbance
and weathering (Hayes and
Michel, 1999).
Bunker C oil in 1976, found petroleum hydrocarbons at various
stages of degradation after 20 and 30 years (Lee et al., 2003;
Vandermeulen and Singh, 1994). A study done 22 years after
the Arrow spill found that biomarker compounds at this location
persist while other classes of compounds are at least partially
degraded (Wang et al., 1994). Weathered forms of light Ara-
bian Crude oil spilled into the Straight of Magellan from the
tanker Metula remain after 24 years in some protected marshes
and on one beach, while much of the coastline has been cleaned
by natural processes of the harsh climate (Wang et al., 2001).
Mangroves have also been found to retain oil residues in a way
similar to marshes with pockets of relatively high amounts of
petroleum residues (Burns et al., 1994). In a recent review article
assessing the Exxon Valdez oil spill after 14 years (Peterson et
al., 2003), the authors noted that sediments, which are physically
protected from wave action, disturbance, oxygenation, and pho-
tolysis, remain partially weathered oil for years. In addition to
exhibiting all of these characteristics, salt marsh sediments are
ideal for preserving petroleum hydrocarbons because they are
in temperate regions, have a high organic carbon content, and
become anoxic within the top one cm of the surface (Teal and
Teal, 1969). For example, n-alkanes were degraded four times
faster in tropical mangroves than a temperate salt marsh that
experienced below freezing temperatures in the winter (Burns
et al., 1994). The high organic carbon in salt marshes may aid
in preserving hydrocarbon residues for two reasons. First, many
other natural compounds are available and may be more labile
for microbes to respire. For example, 14C analysis of bacterial
phospholipids in a sediment core collected at the M-1 location
in Wild Harbor in 2001 have indicated that the bacteria in the
contaminated sections of the core were respiring recently pho-
tosynthesized material, which has contemporary 14Cvalues and
not petroleum, which has no detectable 14C (Slater et al., 2005).
Such a finding is consistent with the fact that the TPH in the
most contaminated sites in Wild Harbor only account for 10%
of the total organic carbon content (White, Reddy et al., 2005).
280 E. E. Peacock et al.
Second, the elevated organic carbon content allows for increased
partitioning into the sediment and out of the porewater, which in
turn reduces the bioavailibility. While evidence for anaerobic hy-
drocarbon degradation does now exist for select hydrocarbons in
No.2 fuel oil (Widdel and Rabus, 1999), there is no “real world”
data indicating that partially weathered hydrocarbon residues,
which persist in Wild Harbor, can be degraded.
Wild Harbor marsh continues to store petroleum residues
30 years after the Florida spill. Approximately 100 kg of the
original product can be found. The locations that were most heav-
ily contaminated continue to have the most persistent residues.
It is unfortunate that a more complete mass balance for the
spilled oil cannot be estimated, but it is likely that evaporation
and offshore transport of the fuel residing in the water column
days to weeks after the spill were major removal processes. The
results from this study should pave the way for future efforts
that focus on the geochemical and biological factors for contin-
ued persistence of petroleum hydrocarbons in a relatively small
area. Wild Harbor marsh is ideal for studies directed at gauging
whether any biological effects exist and whether the ecosystem
has recovered, which in turn may aid policy makers in decid-
ing when human intervention is necessary at other impacted salt
We wish to thank Mr. George Hampson, Ms. Helen White,
Mr. Bruce Tripp, Mr. Sean Sylva, Dr. Li Xu, Dr. John Teal,
Dr. James Quinn, and Dr. John Farrington for their advice and
comments related to this effort. Dr. Robert I. Haddad (Applied
Geochemical Strategies, Inc.) provided a very thorough review
of an earlier draft of this manuscript. Ms. Kristan Davison,
Ms. Danielle Rioux, Ms. Emily Hussey, Ms. Jennifer Webber,
Dr. Emma Teuten, and Mr. Erik Gura assisted with fieldwork.
This work was supported by grants from the National Science
Foundation (CHE-0089172), Woods Hole Coastal Ocean Insti-
tute, Environmental Protection Agency (R-830393), Petroleum
Research Fund Type G starter grant, and the Office of Naval Re-
search Young Investigator Award (N00014-04-01-0029). This is
WHOI contribution # 11405.
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... Studies found that petroleum hydrocarbons from marine oil spills have persisted for decades in anoxic sediments. 41,42 At Bon Secour and Fort Pickens, although deep water table and low moisture content likely created oxygen-adequate sediment environments for microbial activities, the lack of liquid likely limited the mobility of microorganisms. The relatively low (negative) matrix potential likely exerted physiological stress on microorganisms and limited their activity. ...
The 2010 Deepwater Horizon (DWH) blowout released 3.19 million barrels (435 000 tons) of crude oil into the Gulf of Mexico. Driven by currents and wind, an estimated 22 000 tons of spilled oil were deposited onto the northeastern Gulf shorelines, adversely impacting the ecosystems and economies of the Gulf coast regions. In this work we present field work conducted at the Gulf beaches in three U.S. States during 2010-2011: Louisiana, Alabama, and Florida, to explore endogenous mechanisms that control persistence and biodegradation of the MC252-oil deposited within beach sediments as deep as 50 cm. The work involved over 1500 measurements incorporating oil chemistry, hydrocarbon-degrading microbial populations, nutrient and DO concentrations, and intrinsic beach properties. We found that intrinsic beach capillarity along with groundwater depth provides primary controls on aeration and infiltration of near-surface sediments, thereby modulating moisture and redox conditions within the oil-contaminated zone. In addition, atmosphere-ocean-groundwater interactions created hypersaline sediment environments near the beach surface at all the studied sites. The fact that the oil-contaminated sediments retained near or above 20% moisture content and were also eutrophic and aerobic suggests that the limiting factor for oil biodegradation is the hypersaline environment due to evaporation, a fact not reported in prior studies. These results highlight the importance of beach porewater hydrodynamics in generating unique hypersaline sediment environments that inhibited oil decomposition along the Gulf shorelines following DWH.
... An exception has been the over 40-year study of the effects of the 1969 #2 fuel oil spill from the barge Florida off West Falmouth, Massachusetts (Cape Cod). Because of its location near the Woods Hole Oceanographic Institution and oil spill expertise and resources located there, the grounded oil in the West Falmouth salt marsh has been periodically monitored and its effects on biota analyzed, resulting in a number of seminal publications (Burns and Teal, 1979;Sanders et al., 1980;Teal et al., 1992;Reddy et al., 2002;Peacock et al., 2005). One of the most illuminating findings of this longitudinal study was the persistence of oil when it eventually became buried in marsh sediments to a depth where anoxic conditions exist. ...
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Following the Deepwater Horizon blowout, oil, degraded oil, oil mixed with dispersants, and management responses to the spill affected a variety of Gulf of Mexico organisms. This review provides examples of various documented impacts, common patterns, and trends across organisms and/or their environments, and discusses future implications as well as directions for future research. Organism effects are generally characterized as lethal and sublethal. Sublethal can be short term, long term, or permanent and multigenerational. We present individual examples of effects on behavioral response, olfaction, vision, cardiac function, and gene shift, based on research done in laboratories, mesocosm settings, and the field. Future research should emphasize collection and analysis of routine toxicological baselines and examine how and if molecular impacts cascade up to populations. This research will require development of rapid molecular tools and testing procedures to determine exposure compared to field-relevant exposure levels and to be able to extrapolate laboratory results to the field, especially given the mosaic of differing contaminant concentrations (below, at, or exceeding critical concentrations that result in lethal or sublethal effects) occurring in the environment. Recent chemical studies have identified a detectable suite of polycyclic aromatic hydrocarbon metabolites for which there are no toxicity data; further research is needed to determine their impacts on food webs.
... Although anaerobic biodegradation of petroleum hydrocarbons has been reported over the past 20 years, the rates are relatively slow compared to those commonly observed in the presence of oxygen under comparable experimental conditions ( [15,62,174]). Certainly, hydrocarbons from marine oil spills have persisted for decades in anoxic sediments (e.g., [40,122,138,168]), although they can also persist in aerobic environments (e.g., [88,134]). ...
Accidental oil spills in ocean may occur during exploration, production, transportation and use. The spilled oil frequently reaches shoreline where it may harm more or less the ecosystem depending on the physicochemical properties of spilled oil. Here, we review the physicochemical behavior of petroleum hydrocarbons, such as crude oil and refined products, on various types of shorelines under various environmental conditions. During migration to the shore, the oil characteristics can change by evaporation, photooxidation, partition and aggregation. The penetration, remobilization and retention of stranded oil on shorelines are affected by the beach topography and the natural environment. We also discuss the attenuation and fate of oil on shorelines from laboratory and field experiments.
... Although anaerobic biodegradation of petroleum hydrocarbons has been reported over the past 20 years, the rates are relatively slow compared to those commonly observed in the presence of oxygen under comparable experimental conditions ( [15,62,174]). Certainly, hydrocarbons from marine oil spills have persisted for decades in anoxic sediments (e.g., [40,122,138,168]), although they can also persist in aerobic environments (e.g., [88,134]). ...
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The distribution and persistence of oil within the matrix of a beach depends on the oil and beach properties, the presence of fines in the water column, and beach hydrodynamics and biochemistry. In this review, we attempted to provide an assessment of the journey of oil from offshore oil spills until it deposits within beaches. In particular, we addressed the disparity of spatial scales between microscopic processes, such as the formation of oil particle aggregates and oil biodegradation, and large-scale forcings, such as the tide. While aerobic biodegradation can remove more than 80% of the oil mass from the environment, its rate depends on the pore water concentration of oxygen and nutrients, both of them vary across the beach and with time. For this reason, we discussed in details the methods used for measuring water properties in situ and ex situ. We also noted that existing first-order decay models for oil biodegradation are expedient, but might not capture impacts of water chemistry on oil biodegradation. We found that there is a need to treat the beach–nearshore system as one unit rather than two separate entities. Scaling down large-scale hydrodynamics requires a coarser porous medium in the laboratory. Unfortunately, this implies that microscopic-scale processes cannot be reproduced in such a setup, and one needs a separate system for simulating small-scale processes. Our findings of large spatio-temporal variability in pore-water properties suggest that major advancements in addressing oil spills on beaches require holistic approaches that combine hydrodynamics with biochemistry and oil chemistry.
... Aeppli et al. 18 concluded from analysis of SRBs collected between 2011 and 2017 along Gulf shores that the persistence of oxyhydrocarbons limited the overall crude oil hydrocarbon depletion in these MC252 agglomerates to 42% (1 SD = 12%) after 7 years, which equates to approximately half of the 76 to 83% depletion estimated by our in-situ experiment for that time period. MC252-SRBs continue to wash up onto Gulf beaches to the present day, and a possible explanation for this discrepancy could be the formation of SRBs from oil that was temporarily embedded in sublittoral sediments 60 where protection from oxygen substantially reduced degradation rates and preserved some of the n-alkanes and PAHs as also found after the Falmouth oil spill 42,61,62 . Lines depict percent quantity remaining versus time. ...
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Sediment-oil-agglomerates (SOA) are one of the most common forms of contamination impacting shores after a major oil spill; and following the Deepwater Horizon (DWH) accident, large numbers of SOAs were buried in the sandy beaches of the northeastern Gulf of Mexico. SOAs provide a source of toxic oil compounds, and although SOAs can persist for many years, their long-term fate was unknown. Here we report the results of a 3-year in-situ experiment that quantified the degradation of standardized SOAs buried in the upper 50 cm of a North Florida sandy beach. Time series of hydrocarbon mass, carbon content, n-alkanes, PAHs, and fluorescence indicate that the decomposition of golf-ball-size DWH-SOAs embedded in beach sand takes at least 32 years, while SOA degradation without sediment contact would require more than 100 years. SOA alkane and PAH decay rates within the sediment were similar to those at the beach surface. The porous structure of the SOAs kept their cores oxygen-replete. The results reveal that SOAs buried deep in beach sands can be decomposed through relatively rapid aerobic microbial oil degradation in the tidally ventilated permeable beach sand, emphasizing the role of the sandy beach as an aerobic biocatalytical reactor at the land-ocean interface.
... The result shown in Table 3 depicts kerosene with the lowest surface tension, density (σ = 22.5 mN/m, ρ = 810 kg/m 3 ) have low absorption for the CIP, while the crude oil surface tension and density (σ = 31.7 mN/m, ρ = 937 kg/m 3 ) have higher absorption. These results are the same as the study of Peacock et al. (2005). Hence, the above results prove that oil absorption capacity depends on not only the cellulose percentage, cellulose length, but also the petroleum product type. ...
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Recently, Oil spill incidents from maritime activities and port operation have been causing the serious ocean environment pollution, these problems are said to be the negative effects on the natural environment, social economy, marine species, and human health. Due to the high costs of treating oil spills and oil slick in comparison with a low-income country like Vietnam, many incidents related to the oil spill and oil slick have not been thoroughly processed. Cellulose components from Vietnamese agricultural residues used to produce the absorbent materials are one of the most urgent issues and this is the research object of this work. In this study, two types of structural lengths of cellulose added into PU matrix foam are used to measure how much crude oil, fuel oil, diesel oil and kerosene can be absorbed. The absorbent materials are designed after adding cellulose with 5%, 15%, 25% of mass, respectively. The achieved results show that the oil absorption capacity of PU-cellulose implemented 5% cellulose with 500µm of cellulose structure length and 25% cellulose with 3000µm of cellulose structure length are highest for crude oil. These study results from this work provide a reasonable price for the protection of the marine environment in the strategies of recovery and treatment of oil spill and oil slick on the seawater surface.
... For example, the Gulf of Mexico, Deepwater Horizon oil spill in 2010 [18] resulted in 4.9 million barrels of crude oil, some of which contaminated the coastal lands [19]. It is welldocumented that crude oil trapped in porous media such as sands, soils, and sediments can persist for several decades after an oil spill [20][21][22][23][24][25][26], one apparent reason being that the porous-mediatrapped oil cannot be readily weathered [26][27][28][29]. Surfactants are applied to the bulk oil spill in open water to break the oil droplets into smaller sizes by reduction of interfacial tension [30][31][32]. ...
Abstract In this work, an oil-soluble surfactant was studied to enhance crude oil mobilization in a cryolite packed miniature bed. The cryolite packed bed provided a transparent, random porous medium for observation at the microscopic level. In the first part of the paper, oil-soluble surfactants; Span 80 and Eni-surfactant (ES) were dissolved directly into the crude oil. The porous medium was imbued with the crude oil (containing the surfactants), and deionized water was the flooding phase, in this experiment, the system containing ES had the best performance. Subsequently, Sodium Dodecyl Sulfate (SDS), a hydrosoluble surfactant was used to solubilize the ES, with the SDS acting as a carrier for the ES to the contaminated porous media. Finally, the SDS/Eni Surfactant micellar solutions were used in oil-removal tests on the packed bed. Grayscale image analysis was used to quantify the oil recovery effectiveness for the flooding experiments by measuring the white pixel percentage in the packed bed images. The SDS/ES flooding mixture had a better performance than the SDS alone. Keywords: Oil-soluble Surfactant; Micellization; Cryolite Packed-bed; Enhanced Oil Recovery; 14 Image Analysis; Dynamic Light Scattering, Interfacial Tension
... Other examples are illustrated by oil remaining at the West Falmouth and Arrow spill sites after 35 years (Peacock et al. 2005;Owens et al. 2008) and at the Metula incident in southern Chile 41 years later (Fig. 2, Gundlach 2017). In all cases, oil remains only where it is sheltered from physical, chemical, and biological degradation. ...
What light does nearly 25 years of scientific study of the Exxon Valdez oil spill shed on the fate and effects of a spill? How can the results help in assessing future spills? How can ecological risks be assessed and quantified? In this, the first book on the effects of Exxon Valdez in 15 years, scientists directly involved in studying the spill provide a comprehensive perspective on, and synthesis of, scientific information on long-term spill effects. The coverage is multidisciplinary, with chapters discussing a range of issues including effects on biota, successes and failures of post-spill studies and techniques, and areas of continued disagreement. An even-handed and critical examination of more than two decades of scientific study, this is an invaluable guide for studying future oil spills and, more broadly, for unraveling the consequences of any large environmental disruption. For access to a full bibliography of related publications, follow the Resources link at
Most oil tanker accidents occur near land. So when a marine oil spill occurs, it is usually not long before the spilled oil reaches shorelines. The shoreline is where the potential for harm to the environment and biological resources is the greatest, and where media attention and public concerns usually focus. Therefore, it is essential to determine the distribution, amount, composition, and fate of spilled oil on shorelines. This information forms the foundation for management decisions about cleanup during the early phases of the spill, assessments of long-term exposure and injury to biological resources, and long-term restoration strategies after the initial cleanup. In this chapter, we consider the fate of shoreline oil following the Exxon Valdez oil spill, beginning with oil coming ashore in Prince William Sound (PWS) in 1989. This chapter picks up where Chapter 3 left off, describing where the oil was deposited, why some locations were oiled more than others, and how oil disappeared over time and why, in a few isolated locations, it persisted.
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In 1970, approximately 2000 m3 of Bunker C crude oil impacted 300 km of Nova Scotia’s coastline following the grounding of the tanker Arrow. Only 10% of the contaminated coast was subjected to cleanup, the remainder was left to cleanse naturally. To determine the long-term environmental impact of residual oil from this spill event, samples of sediment and interstitial water were recovered in 1993, 1997 and 2000 from a sheltered lagoon in Black Duck Cove. This heavily oiled site was intentionally left to recover on its own. Visual observations and chemical analysis confirmed that substantial quantities of the weathered cargo oil were still present within the sediments at this site. However, direct observations of benthic invertebrate abundance suggest that natural processes have reduced the impacts of the residual oil. To confirm this hypothesis, sediment and interstitial water samples from Black Duck Cove were assessed with a comprehensive set of biotests and chemical assays.
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The largest amounts of, and the least weathered, oil found eight years after the Exxon Valdez oil spill occurred at depths of 25–50+ cm under the protective cover of a well-sorted cobble/boulder armor on intermittently exposed, coarse-grained gravel beaches within Prince William Sound, Alaska. In addition to the armoring, other factors enhancing the retention of the oil include flat slopes of the middle beach and a thick sediment veneer over a bedrock platform. Natural cleaning of the subsurface sediments was accomplished within three years on the finer-grained gravel beaches that have steeper slopes, a thin sediment veneer over the rock platform, and no surface armoring. Minor berm relocation was an effective technique for removing subsurface oil from the finer-grained gravel berms at the high-tide line. Extensive storm berm relocation caused disruptions to beach morphology and sediment distribution which lasted for up to six years.
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We have analyzed the two- and three-ring aromatic hydrocarbons from the Wild Harbor oil spill in September 1969 and the Winsor Cove oil spill in October 1974, in intertidal marsh sediments, using glass capillary gas-chromatographic and mass-fragmentographic analyses. Naphthalenes with 0–3 alkyl substitutions and phenanthrenes with 0–2 substitutions decreased in concentration with time in surface sediments. The more substituted aromatics decreased relatively less and in some cases actually increased in absolute concentration. The changes in composition of the aromatic fraction have potential consequences for the ecosystem and provide insight into geochemical processes of oil weathering. Key words: oil pollution, aromatic hydrocarbons; gas chromatography; gas chromatography–mass spectrometry; geochemistry; marsh; sediments; oil spills
A small spill of No. 2 fuel oil occurred near Wild Harbor, Massachusetts, in September 1969. The benthic fauna of the Wild Harbor Marsh, boat basin, and offshore area was sampled through the fourth and fifth years after the spill (1973, 1974). Sediment samples were analyzed for the presence of petroleum hydrocarbons. Gas chromatography produced evidence of hydrocarbons typical of weathered fuel oil in the sediments of the marsh, boat, basin, and two offshore stations. The numbers of benthic species at the offshore stations and the marsh were slightly, but significantly, lower than those found at control stations. Population densities were similar to control areas for the offshore stations but not in the case of the marsh. The boat basin was still heavily affected. Some stations were characterized by the presence of opportunistic species. The recovery process in terms of the total benthos has leveled off, but there was evidence for further recovery during the course of the study.
Oil contamination may persist in the marine environment for many years after an oil spill and, in exceptional cases such as salt marshes and mangrove swamps, the effects may be measurable for decades after the event. However, in most cases, environmental recovery is relatively swift and is complete within 2–10 years. Where oil has been eliminated from the scene, the long-term environmental impacts are generally confined to community structure anomalies that persist because of the longevity of the component species.
The Ile Grande salt marshes (Brittany coast) were polluted by petroleum hydrocarbons after theAmoco Cadizgrounding in 1978. Thirteen years after the oil spill, sediments were analysed for residual hydrocarbons in order to monitor the aliphatic and aromatic hydrocarbon signatures and to assess both qualitatively and quantitatively the changes in composition of theAmoco Cadizoil. Six stations were selected in the Ile Grande salt marshes and sediments were sampled to a depth of 20cm. For each sample, the hydrocarbon compositions were determined for alkanes, alkenes, aromatics and biomarkers (terpanes, steranes, diasteranes). Hydrocarbon levels drastically decreased between 1978 and 1991, but to different extents according to the initial degree of contamination. In 1991, hydrocarbon concentrations never exceeded 1·7g kg−1sediment dry weight, and in most cases were less than 0·1g kg−1sediment dry weight. Even though petroleum hydrocarbons are still present, natural hydrocarbons were also detected at several stations. Changes in some biomarker distributions were observed 13 years after the oil spill. Nevertheless, most of the biomarkers are very stable in the salt marsh environment and remain unaltered even after a 13-year period.
Introduction: In the aftermath of an oil spill, what should drive the cleanup response and when is it reasonable to stop cleaning? Further, which of the diversity of oil spill clean-up technologies as described in other chapters of this volume might be employed most effectively to achieve this elusive goal? These are complex questions involving chemical, ecological, socio-economic and political considerations and there are no simple answers. It is important to identify and build consensus for recommended clean-up protocols. These recommendations should be based on the considerable experience that has accumulated over the past 30 years. It is the intent of this paper to identify key points and issues with respect to ecological aspects, bearing in mind that these in turn commonly relate to socio-economic aspects.