Pugef Sound Estuary Program
EVERETT HARBOR
ACTION PROGRAM:
Analysis of Toxic Problem Areas
TC-3338-26
FINAL REPORT
September 1988
Prepared by
PTI Environmental Services
and
TetraTech, Inc.
Prepared for
U.S. Environmental Protection Agency
Region X - Office of Puget Sound
Seattle, Washington
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TC-3338-26
Final Report
EVERETT HARBOR ACTION PROGRAM:
ANALYSIS OF TOXIC PROBLEM AREAS
for
U.S. Environmental Protection Agency
Reg-fon X, Office of Puget Sound
Seattle, WA 98005
September 1988
by
PTI Environmental Services
3625 - 132nd Avenue S.E., Suite 301
Bellevue, WA 98006
and
Tetra Tech, Inc.
11820 Northup Way, Suite 100
Bellevue, Washington 98005
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CONTENTS
Page
LIST OF FIGURES vi
LIST OF TABLES x
ACKNOWLEDGMENTS xii
EXECUTIVE SUMMARY xvi
INTRODUCTION 1
SITE DESCRIPTION 4
DRAINAGE PATTERNS 6
STUDY AREAS 7
METHODS 9
DECISION-MAKING FRAMEWORK 9
Overview 9
Chemical, Biological, and Toxicological Indices 12
Action Assessment Matrix 18
Action-Level Guidelines 20
Ranking of Problem Areas 22
Quantitative Relationships 25
Spatial Resolution of Effects 28
Source Evaluation 31
OVERVIEW OF FIELD STUDY DESIGN 31
Station Locations 31
Data Analysis Methods 38
SEDIMENT CHEMISTRY 45
Field Sampling 45
Laboratory Analysis for Metals 47
Laboratory Analysis for Semi volatile Organic Compounds 48
Laboratory Analysis for PCBs 51
Laboratory Analysis for Chlorinated Pesticides 53
Laboratory Analysis for Resin Acids and Chlorinated
Phenols/Guaiacols 54
Laboratory Analysis for Volatile Organic Compounds 59
Ancillary Analyses 59
Quality Assurance/Quality Control Results 60
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BIOACCUMULATION 69
Field Sampling 69
Laboratory Analysis for Mercury 70
Laboratory Analysis for PCBs/Pesticides 71
Quality Assurance/Quality Control Results 72
SEDIMENT BIOASSAY 73
Field Sampling 73
Laboratory Analysis 73
Quality Assurance/Quality Control Results 75
BENTHIC MACROINVERTEBRATES 75
Field Sampling 75
Laboratory Analysis 77
Quality Assurance/Quality Control Results 78
FISH ECOLOGY AND HISTOPATHOLOGY 78
Field Sampling 79
Laboratory Analysis 79
Quality Assurance/Quality Control Results 80
DATA MANAGEMENT 81
Data Organization 81
Data Analysis 82
Data Entry and Quality Control 82
RESULTS 84
SEDIMENT CHEMISTRY 84
Normalization of Chemical Concentrations 85
Bulk Sediment Characteristics 87
Sediment Chemistry: Metals 97
Sediment Chemistry: Organic Compounds 103
Comparison with Recent Historical Data 145
Summary 155
BIOACCUMULATION 157
Mercury in Dungeness Crabs 158
PCBs and Pesticides in Dungeness Crabs 158
Mercury in English Sole 160
PCBs and Pesticides in English Sole 162
Comparison with Recent Historical Data 163
Summary 163
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Benthic Infauna
Polychaete abundance
Crustacean abundance
Pelecypod abundance
Gastropod abundance
Fish Pathology
Lesion prevalence in livers of English sole.
The rationale for using the five general kinds of data is provided in Tetra
Tech (1985a,b). The available Puget Sound AET (Tetra Tech 1986c, 1987) were
used as sediment quality values to evaluate chemical data relative to
predicted biological effects (see below, Quantitative Relationships).
Although many other variables were evaluated throughout the decision-making
process, those shown above formed the basis for problem identification and
priority ranking.
Target Chemicals
A list of chemical contaminants analyzed for in sediments collected
during the Everett Harbor studies is given in Table 1. Most of the sub-
stances on this list have at least one of the following two properties:
they can bioaccumulate, possibly with adverse biological effects in the food
chain if bioaccumulated, or they can produce adverse biological effects even
when not bioaccumulated. EPA priority pollutants that may be currently or
historically discharged into the study area are included on the list.
Compounds not on the EPA list of priority pollutants also have been con-
sidered on the basis of their local significance. For example, resin acids
and chlorinated phenolic compounds may originate from pulp and paper mills
in the project area. In water and effluent bioassays, such compounds may
induce a variety of toxic biological responses, from sperm disfunction in
sea urchins (Cherr et al. 1987) to mutagenicity (e.g., Kinae et al. 1981)
and acute lethality in salmonids (e.g., Leach and Thakore 1973, 1975, 1977).
Bioaccumulation of chlorinated phenolic compounds has also been documented
(e.g., Landner et al. 1977). Tributyltin (TBT), an antifouling agent, was
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TABLE 1. LIST OF CONTAMINANTS AND CONVENTIONAL
VARIABLES FOR ANALYSIS IN EVERETT HARBOR PROJECT
Low Molecular Weight PAH
naphthalene
acenaphthylene
acenaphthene
fluorene
phenanthrene
anthracene
High Molecular Weight PAH
fluoranthene
pyrene
benz(a)anthracene
chrysene
benzofluoranthenes (b and k)
benzo(a)pyrene
indeno(l,2,3-c,d)pyrene
dibenzo(a,h)anthracene
benzo(g,h,ijperylene
Total PCBs
Neutral Halogenated Compounds
1,2-dichlorobenzene
1,3-dichlorobenzene
1,4-dichlorobenzene
1,2,4-tri ch1orobenzene
hexachlorobenzene (HCB)
2-chloronaphthalene
hexachlorobutadiene
hexachloroethane
Phthalate Esters
dimethyl phthalate
diethyl phthalate
di-n-butyl phthalate
butyl benzyl phthalate
bi s(2-ethy1hexyl)phthalate
di-n-octyl phthalate
Pesticides
p,p'-DDE
p,p'-ODD
p,p'-DDT
aldrin
chlordane
dieldrin
endrin
endosulfan I
endosulfan II
endosulfan sulfate
endrin ketone
heptachlor
hepachlor epoxide
alpha-HCH
beta-HCH
delta-HCH
gamma-HCH (lindane)
methoxychlor
toxaphene
Phenol and Alkyl-Substituted Phenols
phenol
2-methylphenol
4-methylphenol
2,4-dimethylphenol
4-chloro-3-methylphenol
Chlorinated Phenols/Guaiacols
2-chlorophenol
2,4-dichlorophenol
2,4,6-trichlorophenol
2,4,5-trichlorophenol
2,3,4,6-tetrachlorophenol
pentachlorophenol
3,4,5-trichloroguai acol
4,5,6-trichloroguaiacol
tetrachloroguaiacol
Resin Acids
abietic acid
dehydroabietic acid
12-chlorodehydroabietic acid
14-chlorodehydroabietic acid
dichlorodehydroabietic acid
isopimaric acid
neoabietic acid
sandaracopimaric acid
Nitrogen-Containing Compounds
N-nitrosodi-n-propylamine
N-nitrosodiphenylamine
nitrobenzene
2-nitrophenol
4-nitrophenol
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TABLE 1. (Continued)
2,4-dinitrophenol
4,6-dinitro-2-methylphenol
4-chloroaniline
2-nitroaniline
3-nitroaniline
4-nitroaniline
2,4-dinitrotoluene
2,6-dinitrotoluene
3,3'-dichlorobenzidine
Halogenated Ethers
bi s(2-chloroethy1)ether
bis(2-chloroisopropyl)ether
bi s(2-chloroethoxy)methane
4-chlorophenyl phenyl ether
4-bromophenyl phenyl ether
Miscellaneous Extractable Compounds3
2-methylnaphthalene
dibenzofuran
benzyl alcohol
benzoic acid
isophorone
hexachlorocyclopentadiene
Volatile Organic Compounds
acetone
benzene
bromodi ch1oromethane
bromoform
bromomethane
2-butanone
carbon disulfide
carbon tetrachloride
chlorobenzene
chloroethane
2-chloroethylvinyl ether
chloroform
chloromethane
di bromoch1oromethane
dichloromethane
1,1-dichloroethane
1,2-dichloroethane
1,1-dichloroethene
trans-1,2-dichloroethene
1,2-dichloropropane
cis-l,3-dichloropropene
trans-l,3-dichloropropene
ethyl benzene
4-methyl-2-pentanone
2-hexanone
styrene
1,1,2,2-tetrach1oroethane
tetrachloroethene
1,1,1-trichloroethane
1,1,2-trichloroethane
trichloroethene
toluene
total xylenes
vinyl acetate
vinyl chloride
Metals
antimony
arsenic
cadmium
chromium
copper
iron
lead
manganese
mercury
nickel
selenium
silver
zinc
tributyltin
Conventional Variables
total organic carbon
total solids
percent fine-grained material
total nitrogen
water-soluble sulfides
a Fifteen tentatively identified organic compounds were also analyzed and
are listed in the Results section.
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analyzed in samples from the Everett marina and Port Susan because of
high toxicity and association with marinas. Several conventional sediment
quality variables were measured [e.g., total organic carbon (TOC) content,
grain size]. These conventional variables provide a means of comparing
areas with different bulk chemical or physical properties. Also, observed
biological effects could result from a characteristic of the system unrelated
to the selected organic compounds or metals of concern (e.g., the deleterious
effects of sediment anoxia on benthic communities).
The target contaminants measured during the Everett Harbor project have
the potential to cause observed sediment toxicity or biological effects.
However, the ability to identify poorly-understood chemical interactions
(e.g., synergism and antagonism) is limited. Although interactive effects
may not be distinguishable from other kinds of effects, they may be measured
through the use of biological indicators explained below.
Biological Variables--
Selection of individual biological and -toxicological variables was
based on the following considerations:
Analysis of several levels of potential biological effects
Bioaccumulation at the tissue level
Pathology at the tissue level
Mortality of amphipods in sediment bioassays
Chronic effects on benthic communities
Use of each variable in past Puget Sound studies
Documented sensitivity of each variable to contaminants
Ability to quantify each variable within the resource and
time constraints of the program.
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Response variables were selected to characterize several important toxic
effects in resident organisms of Everett Harbor. Although a study of
effects on fish populations was beyond the scope of the current project, a
study of effects on individual fishes is possible through an assessment of
liver lesion prevalence. Benthic macroinvertebrates were selected because
of their sensitivity to sediment contamination, their importance in local
trophic relationships, and their ability to establish site-specific response
gradients relative to sediment contamination.
The use of Rhepoxvnius abronius to determine the acute lethality of
field-collected sediments has been documented by numerous authors (e.g.,
Swartz et al. 1982, 1985; Chapman et al. 1982a,b; Mearns et al. 1986). The
use of this amphipod species as an indicator of contaminated areas is
supported by its typical absence from natural populations in such areas
(Swartz et al. 1982; Comiskey et al. 1984), and by its response to contami-
nated sediments in laboratory studies (Swartz et al. 1985). Because of
potential concerns that uncontaminated fine-grained sediments may induce
amphipod mortality, the data collected during the "present study were
screened to ensure that statistically significant toxicity could not be
accounted for by grain-size effects alone.
Elevation Above Reference Indices--
Environmental quality indices were developed to rank areas based on
observed contamination and biological effects. The indices have the general
form of a ratio between the average value of a variable at a site in the
Everett Harbor system and the value of the same variable at a reference
site. The ratios are structured so that the value of the index increases as
the deviation from reference conditions increases. Thus, each ratio is
termed an Elevation Above Reference (EAR) index. For most variables, the
measured average value at the study site is divided by the average value at
the reference area to obtain the EAR. For benthic infauna, EAR are derived
as the inverse ratio of values (i.e., reference divided by Everett Harbor
site) to reflect the magnitude of depressed abundances of benthic organisms.
Chemical effects on infauna are expected to be manifested as decreases in
taxa abundance relative to reference. An increase in the EAR for infauna
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would therefore reflect a decrease in absolute value of the variable but an
increase in adverse effect relative to reference conditions.
It should be noted that these indices were not used in lieu of the
original data (e.g., contaminant concentrations), but in addition to these
data. The original data were used to identify statistically detectable
increases in sediment contamination, sediment toxicity, or biological
effects, and to determine quantitative relationships among these variables.
The EAR indices were used to reduce large data sets into interpretable
numbers that reflect the magnitudes of the different variables among areas.
Action Assessment Matrix
The environmental contamination and effects indices (i.e., EAR) were
organized into an Action Assessment Matrix used to compare study areas or
stations. A simplified hypothetical example of an Action Assessment Matrix
is shown in Table 2. This example matrix is presented to demonstrate how
information from multiple indicators can ' be .integrated for an overall
evaluation and prioritization of different study areas. For this example,
only general indices such as "sediment contamination", or "benthic macro-
invertebrates" are used. In the actual application of the approach,
multiple indices for specific types of sediment contamination were evalu-
ated, including separate measures for organic compounds and metals (see
Prioritization of Problem Areas and Contaminants). Similarly, the benthic
macroinvertebrates category was replaced by more specific measures of
benthic community structure.
Evaluation of information in this format enables the decision-maker to
answer the following questions:
Is there a significant increase in sediment contamination,
sediment toxicity,. or biological effects at any study site?
What combination of indicators is significant?
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TABLE 2. THEORETICAL EXAMPLE OF ACTION ASSESSMENT MATRIX3
EAR Values for Study Sites
Indicator
Sediment contamination
Toxicity
Bioaccumulation
Pathology
Benthic macroin vertebrates
A B
1,300
8.5
900
5.2
4.0
45
2.0
20
2.6
1.2
C D E Reference Value
800
10.0
1,100
8.0
5.0
75
4.5
200
2.8
1.3
8 1,000 ppb
2.2 10% mortality
13 10 ppb
2.0 5% prevalence
1.1 60 individuals/m^
a EAR values for indicator variables are shown for Sites A-E. Benthic macroinverte-
brate factors represent the reduction in numbers of individuals at the study site
relative to the reference site. Factors for all of the other indices represent
increases relative to the reference site values shown.
I 1 - Indicates 'indicator v.alue for the specified area is significantly different
from reference value.
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What are the relative magnitudes of the elevated indices
(i.e., which represent the greatest relative hazard)?
The term "significant" is generally used in this report to mean statis-
tically significant at the 99.9 percent confidence level (alpha = 0.001).
With the exception of sediment chemistry, significance of an EAR was based on
statistical comparisons of variables between contaminated sites and the
reference area. Because replicate data for sediment chemistry were not
collected at every station, an alternative criterion for significance was
developed. Following the approach used earlier in Commencement Bay and
Elliott Bay (Tetra Tech 1985a; PTI Environmental Services (PTI) and Tetra
Tech 1988), a significant elevation of a chemical concentration in sediments
was defined as exceedance of the maximum concentration of that chemical in
all Puget Sound reference areas.
Action-Level Guidelines
4 The decision to evaluate potential.sources of contamination and the need
for possible remedial alternatives applies only to those sites that exceed a
minimum action level. An "action level" is a level of contamination or
effects that defines a problem area. It is assumed that an area requires no
action unless at least one of the indicators of contamination, toxicity.- or
biological effects is significantly elevated above reference levels.
The action levels used to define problem areas in the Everett Harbor
system are shown in Table 3. The action-level guidelines are summarized as
follows:
Significant elevation above reference for THREE OR MORE
INDICES identifies a problem area requiring evaluation of
sources and potential remedial action
For ANY TWO INDICES showing significant elevations, the
decision to proceed with source and remedial action evalua-
tions depends on the actual combination of indices and the
degree to which they are site-specific
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TABLE 3. ACTION-LEVEL GUIDELINES
-Condition Observed
Threshold Required for Action
Any THREE OR MORE significantly elevated
indices3
TWO significantly elevated indices
1. 'Sediments contaminated, but below
HAET and 90th percentile PLUS:
Bioaccumulation elevated relative to
that at the reference area, OR
Sediment toxicity with no more than
40% mortality, OR
Benthic community structure indicates
altered assemblage, but less than
80% depression
2. Sediments contaminated but below
HAET and 90th percentile PLUS
elevated fish pathology
III. SINGLE significantly elevated index
1. Sediment contamination
2. Sediment toxicity
3. Benthic community structure
4. Fish pathology OR bioaccumulation
Threshold exceeded, continue with source
and remedial action evaluation.
No immediate action. Recommend site for
future monitoring.
Threshold for source evaluation exceeded
if elevated contaminants are considered
to be biologically available. If not,
recommend site for future monitoring.
If the magnitude of contamination exceeds
the 90th percentile for all study areas
or the HAET, proceed with source and
remedial action evaluation.
Greater than 40% response (mortality).
80% depression or greater.
Insufficient as a sole indicator.
Recommend site for future monitoring.
Check adjacent areas for significant
contamination, toxicity, and/or bio-
logical effects.
a Combinations of significant indices are from independent data types (i.e., sediment
chemistry, bioaccumulation, sediment toxicity, benthic infauna, fish pathology).
Significant indices are defined as follows:
Sediment Chemistry = Chemical concentration at study site exceeds highest value
observed at all Puget Sound reference areas.
Sediment Toxicity, Benthic Infauna, Bioaccumulation, and Pathology = Statistically
significant difference between study area and reference area (PO.001) at one or more
stations within area.
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When only a SINGLE INDEX is significantly elevated, a problem
area may be defined when additional criteria are met (i.e.,
the magnitude of the index is sufficiently above the signifi-
cance threshold to warrant further evaluation).
Significant sediment toxicity or biological effects may occur in areas
without apparent contamination by toxic substances. In such cases, it would
be important to evaluate the possibility that the observed conditions result
from variables not measured in the field studies. An attempt would be made
to distinguish the biological problem area from surrounding areas using
chemical characteristics, and to identify sources based on these distin-
guishing chemical characteristics.
The action-level guideline based on exceedance of the 90th percentile
concentration of a chemical in sediments was applied only to chlorinated
phenols/guaiacols and resin acids. None of these compounds has an estab-
lished AET. Application of the 90th percentile guideline to data for other
chemicals was considered inappropriate for problem area identification
because of availability of AET or relatively narrow concentration ranges
observed for a number of chemicals. For example, the 90th percentile values
for most metals were below or only slightly elevated above Puget Sound
reference conditions. Stations identified as problem areas based only on
exceedance of the 90th percentile concentrations for selected chemicals
(chlorinated phenols/guaiacols and resin acids) were designated as relatively
low-priority problem areas.
Ranking of Problem Areas
Ranking of problem areas was based on a systematic method of assigning
scores to sampling sites based on the significance and severity (i.e., EAR)
of the various chemical and biological variables. Criteria for scoring
problem areas in terms of priority for evaluation of sources and remedial
actions are shown in Table 4. Based on these criteria, higher priority
would be assigned to an area with many elevated indices (i.e., EAR) than to
an area with few. Because the values of the individual indices are assumed
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TABLE 4. SUMMARY OF SCORING CRITERIA FOR SEDIMENT
CONTAMINATION, TOXICITY, AND BIOLOGICAL EFFECTS INDICATORS
Indicator
Criteria
Score
Metals (one or more)
Organic Compounds
(one or more)
Toxicitya
Macroinvertebrates^
Bioaccumulation
(fish muscle)
Fish Pathology0
Concentration not significant
Significant; EAR <10
Significant; EAR 10-<50
Significant; EAR 50-<100
Significant; EAR >100
Concentration not significant
Significant; EAR <10
Significant; EAR 10-<100
Significant; EAR 100-<1,000
Significant; EAR >1,000
No significant bioassay response
Amphipod bioassay significant
>40% response in bioassay
No significant depressions
1 significant depression
2 significant depressions
>3 significant depressions
>95% depression for >1 variable
No significant chemicals
1 significant chemical
2 significant chemicals
>3 significant chemicals
EAR >50 for >1 chemical
No significant lesion types
1 significant lesion type
O f"TrtMTTH^'ni«4» I /* r» ^ AM -^ \ If* f*f*
J. .J I U I I I I I V*UI I l« I V*.J I VSI I I* ₯ M^*
2 significant lesion types
>3 significant lesion types
>5% prevalence of hepatic n
neoplasms
0
1
2
3
4
0
1
2
3
4
0
2
4
0
1
2
3
4
0
1
2
3
4
0
1
2
3
4
a Toxicity based on amphipod mortality bioassay.
b Variables considered were polychaete abundance, crustacean abundance, gastropod
abundance, and pelecypod abundance.
c Lesions considered were hepatic neoplasms, foci of cellular alteration
(preneoplastic nodules), and megalocytic hepatosis.
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to represent relative environmental hazards, areas with higher values of the
indices are scored higher. Two ranking schemes were used. The first used
sediment chemistry indicators only, primarily to characterize the extent and
magnitude of contamination. The second used all biological indicators to
measure the response to chemical contamination. For ranking based on
biological variables, scores for bioaccumulation and pathology were assigned
to each subtidal station based on trawl data for the corresponding area in
which the station was located. Biological scores for intertidal stations
were based only on the results of the amphipod bioassay since other biologi-
cal variables were not measured at intertidal stations. Scores assigned to
a station for individual biological indicators (i.e., bioassay, infauna,
bioaccumulation, pathology) were summed to obtain an overall biological-
effects score for the station. The total biological-effects score for a
station was normalized to the maximum possible score attainable with the
available data. This normalization step was necessary to avoid biasing
ranks for some study areas towards lower values just because certain data
were missing. The maximum possible score for biological effects when all
variables were measured was 16 (= sum of 4 for amphipod bioassay, 4 for
benthic macroinvertebrates, 4 for bioaccumulation, and 4 for pathology).
The range of possible normalized scores for biology was 0-100 (expressed as
a percentage). The various areas were then ranked according to the magni-
tudes of their overall biological-effects scores.
Similarly, scores assigned to the sediment chemistry indicators (i.e.,
metals and organic compounds) were summed and normalized to the maximum
possible score to obtain an overall chemical-contamination score for each
station. The maximum possible score for sediment chemistry was 8 (= sum of 4
for metals and 4 for organic compounds). A ranking of problem stations was
then developed based on their relative chemical-contamination scores.
Individual stations that exceeded action-level guidelines were grouped
into problem areas based on consideration of the following factors:
Chemical distributions (including data from recent historical
studies)
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Nature and proximity of potential sources
Geographic and hydrographic boundaries.
Historical stations with contaminant concentrations exceeding the highest AET
(HAET) were included in the problem areas. Historical stations showing
lowest AET (LAET) exceedances were included only if they were contiguous with
problem areas defined in the present study.
Total chemical and biological scores for each multi-station problem area
were calculated as the averages of the corresponding total scores for
individual stations within the area. If the final ranking based on biologi-
cal effects for a single station or a multi-station problem area differed
substantially from that based on sediment chemistry, then the higher-ranking
score was given precedence. Thus, some high priority sites were designated
strictly on the basis of chemical contamination (i.e., no corresponding
biological problems apparent) or strictly on the basis of biological
conditions ("i.e., no chemical contamination apparent).
Quantitative Relationships
The development of quantitative relationships among possible causative
factors, sediment toxicity, and benthic effects identifies threshold
concentrations above which changes in the biological indicators are detect-
able. The basic concept of increased biological effects or sediment
toxicity resulting from increased concentrations of a single chemical in
sediments is depicted in Figure 4. Four study areas that have statistically
elevated effects are shown in the figure. Although there is an elevati'on in
contamination relative to reference conditions at four of the remaining five
study areas, there are no statistically detectable increases in the effect
indicator above background conditions. Thus, the level of sediment contami-
nation corresponding to Area X (arrow) represents an apparent threshold
above which significant effects occur. The contamination of sediments by
multiple chemicals may result in a more complex relationship than the
example in Figure 4. Such.relationships are discussed in detail later (see
Contaminant, Toxicity, and Biological Effects Relationships).
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i
o
Area Z
- Area X
u
UJ
Area Y
Area W
o
A
A
A
O A
£V . Average Reference Index
._ _^.
Sediment Concentration
of Contaminant
O Reference
A Everett Harbor, not statistically significant
A Everett Harbor, statistically significant at
the 99.9% confidence level (a- 0.001)
Figure 4. Theoretical example of relationship between sediment
contamination and an effects index.
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AET have been identified using synoptic chemical and biological data
sets from throughout Puget Sound (Tetra Tech 1986c, 1987). Puget Sound AET
are used in this study to identify potential problem areas based on chemical
data collected in previous studies (e.g., U.S. EPA 1982; U.S. Department of
the Navy 1985) where appropriate biological data were unavailable. The
concept of AET and the data sets used in deriving AET are explained below.
The Everett Harbor data collected during this study are being compiled along
with other recent data from Puget Sound into the EPA Sediment Quality Values
database (SEDQUAL). This database will be used as part of an ongoing study
to update Puget Sound AET.
The focus of the AET approach is to identify concentrations of con-
taminants that are associated exclusively with sediments having statistically
significant biological effects (relative to appropriate reference sediments).
Thus, to generate AET values, chemical data are classified according to the
absence or presence of significant biological effects to determine concentra-
tions ' of contaminants above which statistically significant biological
effects would always be expected to occur. AET were originally developed to
identify problem sediments in the Commencement Bay Nearshore/Tideflats
Remedial Investigation (Tetra Tech 1985a). AET have been subsequently
revised with an expanded database (200 stations) and their accuracy has been
evaluated using biological and chemical data for geographically diverse
areas of Puget Sound (Tetra Tech 1986c, 1987). The AET method and accuracy
tests based on Puget Sound data are described in detail in those documents.
AET have been established for 64 organic and inorganic toxic chemicals
using matched chemical and biological data for several biological indicators
and embayments in Puget Sound. Because of patchy biological and chemical
conditions in the environment, it was important that chemical analyses be
performed on the same or nearly the same sediment that was used in bioassays
and benthic infaunal analyses. AET are available for predicting significant
effects based on the following biological indicators:
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Depressions in abundances of major taxonomic groups of
benthic infauna (i.e., Crustacea, Mollusca, Polychaeta,
and total abundance)
Amphipod mortality bioassay using Rhepoxvnius abrom'us
Oyster larvae abnormality . bioassay using Crassostrea
diaas
Microtox bioluminescence bioassay using Photobacter'ium
phosphoreum.
For each chemical, a separate AET was developed for each biological indi-
cator, resulting in four sets of AET. A list of the different AET generated
thus far for Puget Sound is provided in Table 5, along with the LAET and
HAET among these four indicators. The derivation of these AET is described
in more detail in Tetra Tech (1986c).
The AET method has been shown to be sensitive in correctly predicting
impacted stations in Puget Sound, but in doing so the approach also predicts
impacts at some stations that do not demonstrate adverse effects [i.e., the
approach is not completely efficient in identifying only impacted stations
(Tetra Tech 1986c)]. Because the objective for using AET in this study was
to identify potential problem chemicals and problem areas (in conjunction
with action level guidelines), the ability to correctly predict most
impacted stations (sensitivity) is more important than the ability to
predict only impacted stations (efficiency).
Spatial Resolution of Effects
Using the Action Assessment Matrix, contamination and effects were
analyzed at several levels of spatial resolution (e.g., study areas within
the project area or individual stations). Detailed examination of each
sampling station was necessary because spatial heterogeneity of sediment
contamination was relatively high. Quantitative relationships among
sediment contamination, sediment toxicity, and benthic macroinvertebrates
28
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TABLE 5. PUGET SOUND AET (DRY WEIGHT)a-b
(ug/kg dry weight for organic compounds; mg/kg dry weight for metals)
Chemical
Low molecular weight PAH
naphthalene
acenaphthylene
acenaphthene
f 1 uorene
phenanthrene
anthracene
High molecular weight PAH
fluoranthene
pyrene
benz( a) anthracene
chrysene
benzofl uoranthenes
benzo(a)pyrene
i ndeno( 1 , 2 , 3-c , d) pyrene
dibenzo(a,h)anthracene
benzo(g,h,i jperylene
Total PCBs
Total chlorinated benzenes
1 ,3-dichlorobenzene
1 , 4-di chl orobenzene
1 , 2-di chl orobenzene
1 , 2 , 4-tri chl orobenzene
hexachl orobenzene (HCB)
Total phthalates
dimethyl phthalate
di ethyl phthalate
di-n-butyl phthalate
butyl benzyl phthalate
bis(2-ethylhexyl ) phthalate
di-n-octyl phthalate
Pesticides
p,p'-OOE
p,p'-ODO
p,p'-ODT
Phenol s
phenol
2 -methyl phenol
4-methyl phenol
2,4-dimethylphenol
pentachl orophenol
2-methoxyphenol
Miscellaneous extractables
hexachl orobutadi ene
1 -methyl phenanthrene
2 -methyl naphtha 1 ene
biphenyl
dibenzothiophene
dibenzofuran
benzyl alcohol
benzole acid
N-ni trosodi phenyl ami ne
Amphipod
AET6
S.SOOg'IV1
2,400"''
560h i
980h.i
i.aooP1!
5.400h>' .
1.90Q9'"'1
38,00o{j'i
9,800*'!
ll.OOOP'!
3, flOOd'!
5,000"''
3,700
2,400. .
880!''1
sio;"'!
860h''
2.5001
6801
>170
260
>350
51
130 .
>5,20oi'.
>700£'!
>1,200"'1
>5,100
>470
>3,100.
>5901
IS
43
3.9
670h''
63
1,200
>72n.i
>140
930
290
310
670
260
240
540
73
>690
220
Oyster
AETa
5,200'
2,100
>560
500
540
1,500
960
17,000
2,500
3,300
1,600
2,800
3,600
1,600
690
230
720
1,100
400
>170
120
50
64
230
3,400'
160
>73
1,400
>470
1,900
>420
>6
420
63
670
29
>140
930
270
370
670
260
240
540
73
650
130
Benthic
AETe
6,100'
2,100.
640 '
500.
640]
3,200!
1,300'
>sr,ooo!
6,300!
>7,300!
4,500!
6,700]
8,000!
6,800!
>5,200!
1,200!
5,400'
1,100
400
>170
120
50
64
230
>70,0001
160. .
200"-'
>5,100
470
1,900.
>68,000'
9
2.
11'
1,200
>72
670
29
>140
930
270
370
670
270
250
540
73
650
75
Microtox
AETr
5,200
2,100
>560
500
540
1,500
960
12,000
1,700
2,600
1,300
1,400
3,200
1,600
600
230
670
130
170
>170
110
35
31
70
3,300
71
>48
1,400
63
1,900
--
1,200
>72
670
29
>140
930
120
370
670
270
250
540
57
650
40
LAET
5,200
2,100
560
500
540
1,500
960
12,000
1,700
2,600
1,300
1,400
3,200
1,600
600
230
670
130
170
110
35
31
70'
3,300
71
200
1,400
63
1,900
9
2
3.9
420
63
670
29
930
120
310
670
260
240
540
57
650
40
HAET
6,100
2,400
640
980
1,800
5,400
1,900
38,000
9,800
11,000
4,500
6,700
8,000
6,800
880
1,200
5,400
2,500
680
260
50
64
230
3,400
160
200
1,400
470
1,900
15
43
11
1,200
63
1,200
29
930
290
370
670
270
250
540
73
650
220
29
-------
TABLE 5. (Continued)
Chemical
Amphipod Oyster Benthic Microtox
AET6 AET3 AETe AEV LAET HAET
Volatile organics
tetrachloroethene >210. 140 140 140 140 140
ethyl benzene >50 37 37 33 33 37
total xylenes >160 120 120 100 100 120
Metals
antimony
arsenic
cadmium
chromium
copper
lead
mercury
nickel
silver
zinc
5.3
93
6.7
>130.
800]
700]
2.11
>120l
>3.7]
8701
26
700
9.6
>37
390
660
0.59
39
>0.56
1,600
3.2
85
5.8
59
310
300
0.88
49
5.2
260
26
700
9.6
27
390
530
0.41
28
>0.56
1,600
3.2
85
5.8
27
310
300
0.41
28
5.2
260
26
700
9.6
59
300
700
2.1
49
5.2
1,600
a ">" indicates that a definite AET could not be established because the highest concentration
occurred at a station without biological effects (hence, it is not clear from available data if
biological effects always occur above this concentration, as specified in the definition of AET).
For the purposes of problem identification in Elliott Bay, these values were excluded when LAET (low
AET) and HAET (high AET) were generated.
° The following data sets were used to generate the AET in this table:
1. Battelle (1986)
2. Chan et al. (1985", unpublished)
3. Comiskey et al. (1984)
4. Osborn et al. (1985)
5. Romberg et al. (1984)
6. Tetra Tech (1985a)
7. Tetra Tech (1986d)
8. Trial and Michaud (1985)
9. U.S. Department of the Navy (1985).
c Based on 160 stations.
d Based on 56 stations (all ,from Commencement Bay Remedial Investigation).
e Based on 104 stations.
f Based on 50 stations (all from Commencement Bay Remedial Investigation).
9 A higher AET (24,000 ug/kg for low molecular weight PAH and 13,000 ug/kg for anthracene) could be
established based on data from an Eagle Harbor station. However, the low molecular weight PAH
composition at this station is considered atypical of Puget Sound sediments because of the unusually
high relative proportion of anthracene. Thus, the low molecular weight PAH and anthracene AET shown
are based on the next highest station in the data set.
The value shown exceeds the Puget Sound AET established in Tetra Tech (1986c) and results from the
addition of Eagle Harbor Preliminary Investigation data (Tetra Tech 1986d).
30
-------
were examined to evaluate small-scale response gradients. AET were used to
predict the occurrence of. biological problems at stations where chemistry
data were available but biological data were not.
Source Evaluation
The objective of source evaluation is to identify sources of contamina-
tion, and in turn to guide remedial activities. A limited evaluation of
sources is presented in this report based upon the spatial distribution of
contamination, the geochemical properties of observed contaminants, and
characteristics of known or potential sources. A more complete evaluation
of sources will be presented in a separate report (Tetra Tech 1988b).
OVERVIEW OF FIELD STUDY DESIGN
The general design of the field study is described in this section. A
summary of data types and samples collected in the Everett -Harbor study is
shown in Tables 6 and 7. Port Susan was used as a reference area. All of
the Everett Harbor and Port Susan data for this study were collected during
late August-October 1986. A previous sampling of Port Susan occurred during
October 1985 as part of the Elliott Bay Toxics Action Program. Results of
the 1986 sampling were compared with the 1985 results and used to evaluate
.Port Susan as a reference area. Similar methods were used during both years
for Port Susan variables discussed in later sections of this report.
Station Locations
The locations of stations sampled during the Everett Harbor project are
presented in Figures 5 and 6. Subtidal stations for sampling of sediments
were located in shallow water [<50 m water depth] near shore, with the
s
exception of stations located in deep water (>100 m) near the pulp industry
wastewater outfall in eastern Port Gardner- Stations for sampling English
sole (Parophrvs vetulus) and Dungeness crab (Cancer maqister) were located
near areas sampled for sediments at water depths generally <20 m. Coordi-
nates and water depths [corrected to mean lower low water (MLLW)] of all
stations are listed in Appendix A.
31
-------
TABLE 6. SUMMARY OF FIELD STUDY DESIGN
Indicator
Primary Variables
Sample Type
No. Stations
No. Everett
Replicates Harbor Reference"
Sediment chemistry
Toxicity bioassay
Benthic infauna
Bioaccumulation
Fish histopathology
toxic chemicals and
conventional variables"
% mortal i ty
major taxa abundances
species abundances
PCBs, pesticides,
mercury
lesion prevalences
composite 0-2 cmc
composite 0-2 cmc
0.1 -nc grab
0.1 -irr grab
MuscleEnglish sole
(>23 cm) and
Dungeness crab
English sole liver
1
5
5
5
5
1
ld
57
29
16
16
10
10
3
3
3
3
1
1
The reference area was Carr Inlet for sediment chemistry and Port Susan for the other indicators.
See Tables 1 and 7.
Chemistry and bioassay samples were aliquots of the same composite sample.
60 fish.per sample.
32
-------
TABLE 7 SUMMARY OF SEDIMENT ANALYSES BY STATION
Station
ES-01
ES-02
ES-03
EW-01
EW-02
EW-03
EW-04
EW-05
EW-06
EW-07
EW-08
EW-09
EW-10
EW-11
EW-12
EW-13
EW-14
EW-15
NG-01
NG-02
NG-03
NG-04
NG-05
NG-06
NG-07
NG-08
NG-09
NG-10
NG-11
NG-126
NG-136
NG-146
NG-156
OG-01
OG-02
OG-03
OG-04
OG-05
OG-06
OG-07
PS-02
PS-03
PS-04
SD-01
SD-02
SD-03
Semivolati le
Organic
Compounds3
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
Metal sb
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
Conventional sc.
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
- X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
Resin Acids and
Volatile Chlorinated
Organic , Phenolic
Compounds" Compounds
X
X
X
X
X
X
X
X
X
X
X
X
f
_
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
4
,
X
X
X
X
X
X
X
X
X
X
Amphipod
Bioassay
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
Benthie
Infauna
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
33
-------
TABLE 7. (Continued)
Station
SR-01
SR-02
SR-03
SR-04
SR-05
SR-06
SR-07
SR-08
SS-01
SS-02
SS-03
SS-04
SS-05
SS-06
Semi volati le
Organic
Compounds9
X
X
X
X
X
X
X
X
X
X
X
X
X
X
- ^^_^_____^__
Volatile
Organic
Metals" Conventional su Compounds"
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X X
X
X
X
X
X
X
X
X
X X
X
X
X
Resin Acids and
Chlorinated
Phenolic
Compounds
X
X
X
X
X
X
X
X
Amphipod
Bioassay
X
X
X
X
X
X
X
Benthic
Infauna
X
X
a EPA priority pollutant acid/base/neutral organic compounds, PCBs, and pesticides (see Table 1 for complete
list of target chemicals).
EPA priority pollutant metals, except beryllium and thallium. Tributyltin was analyzed at Stations SR-07 and
PS-02 only.
c Total organic carbon, total nitrogen, water-soluble sulfides, and grain-size composition.
EPA priority pollutant volatile compounds.
e Intertidal station.
34
-------
Site Vicinity Map
Weyerhaeuser Company, Everett, WA
0 1/2
e
Scale in Miles
J-2395-02
4/89
-------
STATIONS SAMPLED IN
PORT SUSAN DURING THE
EVERETT HARBOR SURVEY
Figure 5. Locations of sampling stations for sediment chemistry,
amphipod bioassay, and benthic macroinvertebrates.
35
-------
Figure 6. Locations of trawl transects in Everett Harbor and
Port Susan.
36
-------
The rationale for station locations is provided in the sampling and
analysis plan for the Everett Harbor Toxics Action Program (Tetra Tech 1986h)
and sections below. Briefly, stations were selected to:
Fill data gaps from previous studies
Define known areas of contamination more precisely
Determine large-scale gradients of contamination and bioef-
fects in relation to known sources
Detect localized areas of contamination and bioeffects near
potential sources.
Note that the triad of sediment chemistry, amphipod bioassay, and benthic
infauna was sampled at selected sediment stations in all study areas except
Ebey Slough, Steamboat Slough, upstream portions of the lower Snohomish
River, and -the deepwater outfall site in offshore Port Gardner. Assessment
of effects on benthic infauna in these areas would have required extensive
sampling of additional reference conditions to match, their characteristic
salinities or water depths. Such sampling was considered beyond the scope
of this project. Moreover, stations in the Snohomish River, Ebey Slough,
and Steamboat Slough were not sampled for benthos because of the likelihood
of estuarine gradients in community composition that would confound
interpretation of the data (Tetra Tech 1986h). Additional cost savings were
realized by collecting data on amphipod bioassay mortality and benthic
infauna only at selected stations sampled for analysis of sediment chemistry.
Stations selected for analysis of the full triad of sediment quality
indicators were typically located near known sources of contaminants.
In nearshore areas of Everett Harbor and in the Snohomish River, station
locations were determined by line-of-sight fixes on stationary shoreline
features. In offshore areas of Everett Harbor and in Port Susan, LORAN C
navigational coordinates were recorded for each station. Wherever possible,
a variable range marker was used with LORAN C to determine ranges between
37
-------
two reference points, or to determine distances to shore objects. In
addition, photographic records of all position alignments and ranges were
made at all stations, and depth soundings were recorded. Station positioning
methods were sufficiently accurate to define locations within a 15-m radius
at most stations and within a 8-m radius at stations that were located in
areas where the vessel could be tied to a stationary object. The vessel was
anchored at the stations whenever possible during the survey, and station
locations were always verified before each sample was collected.
Data Analysis Methods
Chemical Contamination
The magnitude and spatial extent of sediment contamination was deter-
mined by comparisons of chemical concentrations among Everett Harbor study
areas and with reference conditions in Carr Inlet and Port Susan. Averaged
data from six Carr Inlet stations sampled in 1984 were used whenever possible
to calculate EAR for Everett Harbor sediments. Recent Carr Inlet data were
used as the basis for calculating EAR for the following reasons:
The most complete reference data set is available for Carr
Inlet, including synoptic data for metals, a wide range of
organic compounds, grain size, organic carbon, and other
conventional variables
The lowest detection limits for most substances of concern in
Puget Sound embayments are available for Carr Inlet
Elevations above reference for other urban embayments (e.g.,
Commencement Bay, Elliott Bay) have been calculated with
these data, and therefore, will be directly comparable with
the values calculated for this study
38
-------
In almost all cases where chemicals were detected in multiple
reference areas, the Carr Inlet samples had comparable or
lower values and on this basis appear to be reasonably repre-
sentative of Puget Sound reference conditions.
For chemicals not measured in Carr Inlet (Tetra Tech 1985a), such as resin
acids, most tentatively identified organic (TIO) compounds, and chlorinated
guaiacols, data from Port Susan were used. Not all TIO compounds were
detected in Port Susan. Because detection limits are typically unavailable
for TIO compounds, reference concentration of 20 ug/kg dry weight (DW) was
assigned as a reasonable detection limit (twice the detection limits for
many semivolatile organic compounds in Port Susan) to generate EAR for TIO
compounds. EAR values for TIO compounds were used for comparison purposes
during data analysis, but were not used during problem area identification
and ranking.
Because replicate data for sediment chemistry were not collected at
every station, tests for statistically significant differences between
Everett Harbor samples and reference area samples could not be conducted.
Instead, chemical data from a wide range of Puget Sound reference areas
(collected from 1976 to 1986, including the Port Susan data from the present
study) were used for determining whether elevations above reference were
"significant" (i.e., whether the contamination exceeded all Puget Sound
reference conditions). Port Susan data from this study were added to
reference data compiled previously (Tetra Tech 1985a). If a chemical was not
detected in a reference area sample, detection limits were used to define
reference conditions for that chemical. Detection limits greater than
50 ug/kg DW for organic compounds were excluded from the reference area
concentration ranges to minimize the bias resulting from less sensitive
chemical analyses. Such detection limits observed in other studies were
previously excluded from Puget Sound reference area data (Tetra Tech 1985a).
In general, high detection limits were reported infrequently in this
study and did not impede data analysis. However, the maximum chemical con-
centrations for certain compounds (e.g., certain chlorinated benzenes and
pesticides) were relatively low and were in some cases exceeded by maximum
39
-------
detection limits. In order to generate 50th percentile (median) and 90th-
percentile concentrations that were most representative of chemical condi-
tions in the study area, detection limits greater than 100 ug/kg DW for
semivolatile organic compounds or greater than 25 ug/kg DW for single
component pesticides were not used in determining percentile concentrations
in the study area.
In samples analyzed for chlorinated phenols/guaiacols as well as
acid/base/neutral (A/B/N) compounds, data were generated by two different
procedures for certain chlorinated phenols (i.e., 2-chlorophenol,
2,4-dichlorophenol, 2,4,5- and 2,4,6-trichlorophenol, and pentachlorophenol).
Because detection limits for the dedicated chlorinated phenol analyses were
in most cases considerably lower than for the full-scan A/B/N analyses (in
extreme cases, by well over two orders of magnitude), only the results for
the dedicated analyses were used in data analysis.
For a small proportion of the chlorinated phenol data, detected results
for the dedicated analyses were greater than or roughly equal to (within a
relative difference of 50 percent) detection limits reported for the full-
scan analyses. In these cases, inclusion of the full-scan detection limits
would have had virtually no effect on reported data. In three cases,
concentrations reported for dedicated analyses were notably greater than
full-scan detection limits (i.e., with a relative difference of »50 per-
cent): 2,4-dichlorophenol at Station EW-01 [320 ug/kg DW (dedicated) vs.
U20 ug/kg DW (full-scan)]; 2,4,6-trichlorophenol at Station EW-01 [290 ug/kg
DW (dedicated) vs. U100 ug/kg DW (full-scan)]; and pentachlorophenol at
Station EW-04 [460 ug/kg DW (dedicated) vs. U200 ug/kg DW (full-scan)]. The
full-scan detection limits in these cases may be underestimates [e.g., by
not fully accounting for analytical recoveries (6-10 percent, recovery for
the three cases cited above) or for extraction efficiency (the acetic acid
used in dedicated analyses may have enhanced extraction efficiency relative
to the full-scan analyses)]. Regardless, favorable quality assurance/
quality control (QA/QC) results for the dedicated analyses (Tetra Tech
1988a) and strong correlations among chlorinated phenol concentrations (see
Sediment Chemistry in Results section) support the use of the dedicated
results over the full-scan results for these compounds. Preferably,
40
-------
additional sampling will be conducted in the East Waterway to resolve the
few discrepancies between, reported values for dedicated analyses and
detection limits for full-scan analyses.
Pairwise Pearson correlations were performed (using detected data only)
to examine covariance in the distribution of selected contaminants.
Scatterplots of all correlations cited in text were examined. Based upon
relatively strong correlations (e.g., r>0.8) among most individual polycyclic
aromatic hydrocarbons (PAH), PAH were treated as two compound groups [low
molecular weight PAH (LPAH) and high molecular weight PAH (HPAH)] during data
analysis. Detection limits were included in these PAH sums.
Biological Effects--
Selected biological variables (i.e., amphipod bioassay, benthic infauna,
and liver histopathology) were used to test for statistical differences
between study area stations and the reference area (Port Susan). Use of
statistical criteria ensured that between-site differences were judged
objectively- The statistical design used to test for significant differences
between control and test stations adjusted the individual error rate for
multiple comparisons. This reduced the probability of a Type I error (i.e.,
that the null hypothesis being tested was not falsely rejected). The null
hypothesis was that the mean value of a variable at the test station was
equal to the mean value of that variable at the reference station. This
null hypothesis was tested vs. several alternative hypotheses, depending on
the biological variable being tested. In environmental studies, control of
the Type I error rate becomes increasingly important as the regulatory and
legal consequences of incorrectly identifying a difference between mean
values become important.
Correction of the error rate for multiple comparisons was necessary
because the repetitive use of data collected at a control station results in
non-independence among the pairwise comparisons (Winer 1971). If the
individual error rate for each comparison is not corrected, then the
probability of falsely identifying a significant difference between the test
and reference stations increases with the number of pairwise comparisons
41
-------
made. For example, if the selected pairwise significance level is
alpha=0.05, and 20 hypotheses are tested (each using the same reference
data), then the probability that all of the significant differences identi-
fied in the 20 comparisons are correct is (0.95)20, or 35.8 percent. This
probability decreases as the number of tests increases.
In these studies, the number of pairwise comparisons varied from 11 to
29 among the four biological variables. Selecting an experimentwise error
rate of alpha=0.05, and dividing that rate by the number of comparisons would
have yielded individual error rates between alpha=0.005 to alpha=0.002.
However, a pairwise comparison error rate of alpha=0.001 was selected for all
four variables, for three reasons. First, a significance level of
alpha=0.001 was sufficiently conservative to assure with 97.1 to 98.9
percent probability that all identified significant differences were true
differences. Second, use of the same error rate for tests of all four
biological variables ensured comparability among the test results. Third,
an error rate of alpha=0.001 was consistent with the pairwise comparison
error rate used in the Elliott'Bay and Commencement. Bay studies.
For benthic macroinvertebrate data, an unpaired two-sample t-test was
used to test for a statistically significant difference (P<0.001) between
each study site (n=5) and the pooled reference site (n=15 for the three
stations combined). Before applying the parametric tests, the Fmax test was
used to determine whether the sample variances were homogenous for each
paired comparison. Because the variances were heterogeneous in most of the
pairwise comparisons, the abundances of infaunal taxa (i.e., polychaetes,
crustaceans, pelecypods, and gastropods) used to test for between-site
differences were log-transformed [log^o (x+1)]. If the variances of the
log-transformed data remained heterogeneous between the study site and the
reference site (Fmax test; P<0.05), an approximate t-test was applied to the
data (Sokal and Rohlf 1981).
Comparisons of benthic infaunal assemblages between stations in Everett
Harbor and Port Susan, and other reference areas within Puget Sound are also
described. Based on species-level data for all stations within the Everett
Harbor study area, faunal similarities among stations were determined using
42
-------
a normal classification analysis. All data were log transformed [Iog10
(x+1)] prior to analysis. The classification analysis involved two steps.
First, similarity values were generated for all possible pairs of stations
included in the analysis using the Bray-Curtis Similarity Index (see Boesch
1977). This index uses both species composition and the abundances of the
individual species to estimate between-site similarity. The group average
clustering strategy was then applied to the matrix of similarity values to
generate a dendrogram of stations, from which groups of stations (i.e.,
stations that are most similar in species composition and abundance) were
determined.
For the amphipod (Rhepoxvnius abronius) bioassay data, a two-sample
analysis of variance (ANOVA), which is statistically equivalent to a t-test,
was used to test for a significant difference (P<0.001) between each study
site station (n=5) and the pooled reference stations (n=10 for two stations
combined). Station PS-02 was excluded from the reference area data set
because of excessive mortality (see Sediment Bioassays in Results section).
Following the approach of Mearns et al. (1986), the data were transformed
using an arcsine transformation only when the variances were heterogeneous.
Homogeneity of variances was tested using the Fmax test (P<0.05). The mean
mortality and 95 percent confidence limits for reference area samples from
Port Susan were compared with similar statistics for other reference areas
used during previous studies.
There is evidence that the R. abronius bioassay is subject to limited
grain-size effects and attempts have been made to quantify and compensate for
these effects (DeWitt et al. 1988). The present data were examined using
simple linear regression to test for a predictive relationship between
amphipod mortality and grain-size (percent fine-grained material).
Lesion prevalence and male proportion (i.e., an index of fish sex ratio)
were compared between each transect in Everett Harbor and the Port Susan
transect using the G-test of independence (P<0.001) with Williams' correction
factor (Sokal and Rohlf 1981). Before testing for a difference in lesion
prevalence, the age distribution of fish sampled for histopathological
analyses was compared between each transect in Everett Harbor and the Port
43
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Susan transect using the Mann-Whitney U-test. When the age distributions
were significantly different (P<0.05). adjustments were made to the data set
for the Everett Harbor trawl site by removing data for individuals of an
extreme age class until the age distributions were no longer different. The
similarity among the prevalences of all three lesions across all transects
was determined using Kendall's coefficient concordance (W). Within Everett
Harbor, the proportion of males having each kind of hepatic lesion was
compared with the corresponding proportion of females using the G-test of
independence with Williams' correction factor. Positive association between
the prevalence of each kind of lesion and fish age was tested using Spear-
man's coefficient of rank correlation (rs). Length-at-age was compared
between fish with and without hepatic lesions using the Mann-Whitney U-test.
Otoliths were available for age determination for 650 of the 660
(98 percent) English sole sampled in Everett Harbor and Port Susan. Ages of
the 10 fish not having corresponding otoliths were estimated from age-length
keys based on the 650 fish of known age, stratified by sex (Ricker 1975).
Once age determinations were made, fish younger than 3 yr old (n=66) were
excluded from subsequent analyses. The goal of this study was to focus on
individuals >3 yr old (i.e., those most likely to be afflicted with serious
idiopathic hepatic lesions).
For bioaccumulation, qualitative comparisons of polychlorinated
biphenyl (PCB) and mercury concentrations in tissues of English sole and
Dungeness crabs were made among stations. Pesticides data were not tested
statistically because pesticides were not detected in any tissue samples.
No statistical tests were performed to determine among-station differences
in contamination of Dungeness crab because replicate samples were not
collected at stations other than Station EW-91. Limitations of PCB data due
to low analytical recoveries (see below, Bioaccumulation, Quality
Assurance/Quality Control Results) precluded statistical treatment of PCB
data for English sole. Statistical tests were not performed on mercury data
for English sole because reference-area concentrations were highest in the
study.
44
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SEDIMENT CHEMISTRY
Field Sampling
Full details of the sampling design and techniques are provided in the
"Sampling and Analysis Design for Development of Everett Harbor Action
Program" (Tetra Tech 1986h) and the "Quality Assurance Project Plan for Field
Investigations to Support Development of the Everett Harbor Action Plan"
(Tetra Tech 1986f). Field collection procedures followed the recommendations
of the Puget Sound Estuary Program (PSEP) (Tetra Tech 1986g).
Sediment samples were collected between 2 and 29 October 1986 using a
chain-rigged van Veen grab sampler with a cross-sectional area of 0.1 nr-
Following deployment, the closed grab was retrieved and placed in a sampling
tray. The hinged lids of the van Veen sampler were opened to inspect the
sample.
Care was taken to ensure recovery of an intact surface sediment layer,
with four major criteria used for rejection of a sample:
Overflowing sediments, with sediment touching the top of the
closed cover
Water leaking from the sides or bottom (i.e., indicating that
the interstitial water in the sample was being flushed with
overlying seawater), or visible scour of the sediment surface
near the edges of the sampler
Turbid water overlying the sediments
Insufficient penetration depth.
After the field supervisor determined maximum penetration depth and
sample acceptability, qualitative observations were recorded on field log
sheets for sediment color, odor, texture, and the presence of recognizable
45
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organisms. An HNu photoionization detector was used to monitor all sediment
samples for harmful vapors.
When it was determined that the grab triggered incorrectly, that the
sample was disturbed, or that some of the sample was lost, a new sample was
taken. More than one grab at the same station sometimes was necessary to
obtain an acceptable depth of penetration. In medium to coarse sand, a
minimum penetration depth of 5 cm was considered acceptable'. In fine sand
and sandy silt, a penetration depth of 7 cm was the minimum acceptable
depth. When attempts to sample a station were unsuccessful, another nearby
station was selected and documented. Standardized collection data (i.e.,
collection date and time, station location, depth, and replicate number)
were recorded for each sample.
Once onboard, samples were held in a vertical position by blocks and the
overlying water was carefully drained off by an aspirator. Subsamples for
volatile organic analyses were taken by placing 1.5-oz glass jars (dupli-
cates) at the undisturbed sediment surface and filling them using a stain-
less-steel spatula. These s.ample jars were tightly sealed using Teflon
tape, with no headspace remaining. Jars for volatile analysis were filled
as tightly as possible, eliminating obvious air pockets. Subsamples for
sulfide analysis were immediately removed from the sampler and placed in a
tared plastic container with 50 ml of sulfur antioxidant buffer.
The remaining subsamples were taken from a homogenized sample. Each
sampling horizon from the upper 2 cm of sediment away from the edge of the
van Veen sampler was carefully removed with a stainless steel spatula, trans-
ferred to a stainless steel bowl (which was pre-rinsed with site water and
methylene chloride), and homogenized by stirring with a stainless steel
spoon. Samples were stirred until uniform color and textural homogeneity
were observed. Subsamples for metals and semivolatile organic analyses were
removed with a stainless steel spoon and placed in precleaned glass jars with
polytetrafluoroethylene (PTFE)-lined lids. Subsamples for grain size
analysis were placed in polyethylene bags.
46
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Intertidal samples were collected from shore using a stainless steel
spatula. Otherwise, intertidal and subtidal sediment samples were processed
and analyzed in similar fashion.
Sample handling (including chain-of-custody procedures) and sample
storage are addressed in detailed quality assurance reports prepared for this
project (Tetra Tech 1988a).
Laboratory Analysis for Metals
The following 11 of the 13 EPA priority pollutant metals were analyzed
in 54 sediment samples: antimony, arsenic, cadmium, chromium, copper, lead,
mercury, nickel, selenium, silver, and zinc. The remaining two priority
pollutant metals, beryllium and thallium, were not analyzed because histori-
cal data did not suggest that these metals were of concern in the study
area. Iron and manganese were also analyzed in 54 samples and TBT was
analyzed in two samples. Analyses were performed at Battelle Northwest
Marine Research Laboratory in Sequim, Washington.
Samples were prepared by thawing the frozen sediment, and then homogen-
izing, freeze-drying, and grinding each sample. The sample was then either
subjected to a total acid digestion for atomic absorption analysis, or
pressed into a pellet for x-ray fluorescence (XRF) analysis. Total acid
digestion was performed by combining 1 mL of 4:1 nitric acid:perchloric acid
(HN03:HC104) with a 0.200-g sample in a PTFE bomb at 130° C for 4 h. After
the sample was cooled, 3 ml of hydrofluoric acid was added and the bomb was
heated overnight at 130° C. After cooling, 20 mL of 2.5 percent boric acid
^3603) was added and the bomb was heated again at 130° C for 8 h. After
the weight and volume of the digestate were determined, the solution was
analyzed for silver, cadmium, antimony, and selenium by Zeeman graphite
furnace atomic absorption (GFAA) using the method of standard addition for
calibration. Cadmium and silver were first concentrated into aminopyrolidine
dinitrocarbonate (APDC). Mercury was determined on aliquots by cold vapor
atomic absorption following preconcentration into APDC. The mercury
detector was calibrated with standard solutions.
47
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XRF was used to quantify arsenic, chromium, copper, iron, manganese,
nickel, lead, and zinc. Thin film standards (Neilson 1977) were used to
calibrate the XRF analyzer. Although the analysis of these metals by XRF
differs from routine EPA methods, the PSEP protocols (Tetra Tech 1986g)
specify that XRF may be used if accuracy and precision can be demonstrated
to the levels specified by the program.
TBT was analyzed by GFAA following extraction of organotin species into
methylene chloride, and back extraction of TBT into sodium hydroxide solution
(Homer and Dooley 1983).
Laboratory Analysis for Semi volatile Organic Compounds
The methods used for analysis of A/B/N semivolatile organic compounds
followed Tetra Tech (1986a). Analyses were performed at Enseco/California
Analytical Laboratories (CAL) in West Sacramento, California.
An 80-g homogenized sediment sample was spiked with the stable isotope-
labeled analogs of the target compounds (8 ug of base and neutral compounds
and 12 ug of acid compounds). The sediment was then Soxhlet-extracted with
methylene chloride/methanol (2:1, vol/vol). The resulting extract was
subjected to liquid-liquid partitioning with water and was dried by elution
through a sodium sulfate column. Elemental sulfur, a common interferant in
estuarine and marine sediments, was removed from the extract with metallic
mercury. Biological macromolecules were then removed from the extract by
gel permeation chromatography. The extract was subjected to reverse phase
column chromatography (bonded C^g solid phase) to reduce interferences from
unresolved paraffinic hydrocarbons prior to capillary gas chromatography/mass
spectrometry (GC/MS) analysis for A/B/N compounds using the isotope dilution
technique. Compounds without labeled analogs (Table 8) were quantified
using the nearest eluting, most chemically similar labeled compound as a
recovery standard. All reported concentrations were corrected for recovery
using the isotope dilution technique. Recoveries of isotope-labeled
standards were determined by the internal standard technique.
48
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TABLE 8. LABELED COMPOUNDS USED
WHEN ANALOG NOT AVAILABLE
d7-2-methylpyricline
aniline
dg-naphthalene
benzyl alcohol
2-methylphenol
4-methylphenol
N-nitrosodi-n-propylamine
b i s(2-ch1oroethoxy)methane
benzoic acid
4-chloroaniline
2-methylnaphthalene
dig-acenaphthene
2-nitroaniline
3-nitroaniline
4-nitroaniline
dibenzofuran
d^Q-phenanthrene
4-bromophenyl phenyl ether
d^-benz (a) anthracene
butyl benzyl phthalate
di2-benzo(g,h,i)perylene
i ndeno(1,2,3-cd)pyrene
dibenzo(a,h)anthracene
49
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The first batch of samples- extracted by the laboratory yielded consis-
tently lower, but acceptable recoveries of the isotope-labeled compounds
than the subsequent batches. The laboratory was unable to determine the
cause for this systematic phenomenon.
Lower limits of detection (LLD) were determined according to guidelines
specified in Tetra Tech (1986a). Based on the complexity of the extracts,
three levels of LLD were established. The data quality objective of 10 ug/kg
DW was met for the "cleaner" samples.
Tentatively Identified Organic Compounds--
TIO compounds were searched for in all extracts of Everett Harbor
sediments analyzed for A/B/N compounds by GC/MS. Analyses were performed at
Tetra Tech on a stand-alone Finnigan GC/MS data system with data stored on 9-
track magnetic tapes generated at CAL. The following procedure was used to
acquire data for TIO compounds:
.Preliminary, intensive searches were conducted on roughly 25
percent of the samples. Most samples were chosen from the
most contaminated areas (e.g., the East Waterway), but
representatives of all study areas were examined. Fifteen
chemicals that occurred most frequently and at the highest
concentrations were selected for routine searches in all
samples.
Routine searches for the 15 selected TIO compounds were
performed in all samples and in two method blanks.
Concentrations were estimated based on d1Q-phenanthrene (a
standard spiked in the sample at a known concentration) and
response factors that accounted for the variations in frag-
mentation between d,Q-phenanthrene and the TIO compounds.
TIO compound concentrations were recovery-corrected based
upon d.Q-phenanthrene. It is unlikely that djQ-phenanthrene
recovery was applicable across the chemically diverse range of
50
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TIO compounds. For compounds similar to phenanthrene (e.g.,
retene), recoveries were likely similar to d,Q-phenanthrene.
For more polar compounds such as fatty acids, the recovery
correction was likely an underestimate. Thus, recovery
corrections were "conservative" overall. All detected values
were qualified as estimates and assigned an "E" qualifier.
Undetected TIO compounds were reported as U (without a
detection limit). Sufficient information was not available to
determine detection limits.
Several compounds were found at low levels in blanks. Any
compound found in a sample at a level less than five times
the highest concentration found in any blank was reported as
a B (with no accompanying value).
Laboratory Analysis for PCBs
The extraction and cleanup procedures were performed according to Tetra
Tech (1986a) with the following notable exceptions:
40 g of sediment were extracted and none of the extract was
split for A/B/N analysis
No isotopically labeled A/B/N compounds were added [the
isotope dilution technique described in Tetra Tech (1986a)
applies only to A/B/N compounds].
Analyses of PCBs in extracts were performed at CAL by two instrumental
methods: gas chromatography/electron capture detection (GC/ECD) and GC/MS
with limited mass scanning. Only GC/ECD analyses were originally planned
for these analyses. However, review of the data generated by GC/ECD
indicated that sample interferences detracted from the reliability of
qualitative and quantitative results. GC/ECD results for two matrix spike
samples and two sediment standard reference materials were low (10 to
55 percent recovery for the matrix spikes and 9 to 32 percent of accepted
51
-------
values for the reference materials), whereas recoveries for spiked blanks
(without sample interferences) were considerably better (70 to 80 percent).
To address the apparent problems with interferences, samples with reported
values greater than 50 ug/kg (DW) or detection limits greater"than 50 ug/kg
(DW) were re-analyzed by GC/MS with limited mass scanning. Two samples had
reported GC/ECD results of less than 50 ug/kg (Samples NG-08 and SD-03) and
thus did not require re-analysis by GC/MS. All other positive PCB results in
the database were generated by GC/MS.
GC/ECD Analysis--
The instrumental and quantification methods described in Tetra Tech
(1986a) were followed with several exceptions. Most notably, external
standard quantification was used rather than the recommended internal
standard method, peak heights were used rather than peak areas, and a
single-point calibration was used rather than a five-point calibration. A
peak-by-peak, modified Webb-McCall technique was used to quantify PCBs.
Relative response factors for 25 resolved peaks in a PCB- standard containing
Aroclors 1242, 1254, and-1260 (the range of congeners expected in environ-
mental samples) were determined by measuring the individual peak concentra-
tions by GC/MS and then using dilutions of the same standard for initial and
ongoing GC/ECD calibrations. Dual capillary column analyses were performed
with a 30-m DB-5 column (for quantification) and a 30-m DB-1701 column (for
confirmation) (J & W Scientific).
GC/MS Analyses
GC/MS analyses were performed with a 30-m DB-5 fused silica capillary
column (J & W Scientific); the GC oven was temperature-programmed from 50° C
(held 1 min) to 320° C at 6° C/min. The internal standard was d1Q-phenan-
threne. The following ions were monitored for each chlorination level: m/z
222, 224 (dichloro-); m/z 256, 258 (trichloro-); m/z 292, 290, 294, 222
(tetrachloro-); m/z 326, 328, 256 (pentachloro-); m/z 360, 362, 292 (hexa-
chloro-); m/z 394, 396, 398, 326 (heptachloro-); and m/z 430, 428, 360
(octachloro-). Thus, for more chlorinated congener groups that might co-
52
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elute with less chlorinated congeners, (M-70)+ ions were used to ensure that
peaks were not double-counted or misclassified.
The congener standard containing representative compounds differed
slightly from the recommendations of Tetra Tech (1986a) and U.S. EPA
Method 680: 2,4-dichlorobiphenyl was used rather than 2,3-dichlorobiphenyl;
2,4,6-trichlorobiphenyl was used rather than 2,4,5-trichlorobiphenyl;
2,2' ,3,4',5,6'-hexachlorobiphenyl was used rather than 2,2',4,4',5,6'-
hexachlorobiphenyl; 2,2',3,4,5,6,6'-heptachlorobiphenyl was used rather than
2,2'" ,3,4' ,5,6,6'-heptachlorobiphenyl; and 2,2' ,3,3' ,5,5' ,6,6'-octachloro-
biphenyl was used rather than 2,2',3,3',4,5'.S.S'-octachlorobiphenyl. A
different congener standard was used to establish retention time windows for
scanning with selected ions.
Only single-point calibrations were used for GC/MS and GC/ECD standards
(although five-point calibrations were specified to the laboratory); hence,
the results must be considered estimates only.
Laboratory-AnaIvsis for Chlorinated Pesticides
The method originally specified is described in Tetra Tech (1986a).
This procedure calls for extraction of a 100-g wet weight sample with
removal of 20 percent of the extract for GC/ECD analysis of pesticides and
PCBs. For this project, the pesticide/PCB fraction was extracted separately
from the A/B/N extract to be analyzed by GC/MS. A sample of 40 g (wet
weight) was extracted and processed according to protocol.
The original statement of work submitted to CAL was verbally modified
at the request of CAL after they received the samples. Instrumentation was
modified from capillary column analysis to packed column analysis for both
quantisation and confirmation according to EPA Contract Laboratory Program
(CLP) procedures. A mixed phase 1.50 percent SP-2250 and 1.95 percent SP-
2401 was used for the quantisation column. The confirmation column used was
3 percent SP-2100.
53
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Most of the sample extracts were diluted to minimize interference from
non-target compounds. Dilution factors were 10, 100, or 200. Detection
limit specifications (0.1-5.0 ug/kg) were satisfied for samples not requiring
dilution but were exceeded for diluted samples.
Laboratory Analysis for Resin Acids and Chlorinated Phenols/Guaiacols
Standard procedures for analysis of resin acids and chlorinated phenols/
guaiacols in sediments are not available. Thus, dedicated analyses for these
compound classes were developed in conjunction with Laucks Testing Labora-
tories (Seattle, Washington) and were validated with initial performance
tests.
Extraction--
Wet sediment samples (roughly 40-50 g wet weight) were added to a
precleaned Soxhlet thimble. Recovery surrogates were spiked into the sample
prior to extraction: 0-methylpodocarpic acid (a resin acid surrogate)
[National Council of the .Paper Industry for Air and Stream Improvement
(NCASI) 1986] was added at 50 ug/sample and two phenolic surrogates,
2,6-dibromophenol and 2-bromo-4-chlorophenol, were added at 5 ug/sample. The
sediment was rinsed with a solution of 0.5-mL acetic acid/50 ml_ methanol to
remove as much water as possible and to reduce the extraction pH and thus
enhance recoveries of the organic acid analytes. The acetic acid/methanol
rinsate was stored for later use. The rinsed sediment was then Soxhlet
extracted for 24 h with a mixture of 3:2 (v/v) acetone/hexane (azeotropic
boiling point = 50° C).
Sample extracts were combined with the methanol rinsates and 200 mL of
pre-cleaned water (pH <2) in a separatory funnel and were subjected to
liquid-liquid extraction. After removal of the hexane layer, pentane and
ethyl ether were used for additional extractions of the aqueous phase.
Separatory funnel extracts were combined, dried with N32S04, and concentrated
to a volume of 10 ml with a Kuderna-Danish (K-D) apparatus. The extracts
were then split into two 5-mL aliquots for separate resin acid and chlori-
nated phenols analyses.
54
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Derivatization--
Resin acids were methylated and chlorinated phenolics were acetylated
before GC/MS analysis.
Resin Acids--Extract aliquots to be analyzed for resin acids were ex-
changed into ethyl ether, treated with 4 drops of methanol, and derivatized
with diazomethane (CH2N2) to generate methyl esters. Derivatized extracts
were exchanged to 1 ml of hexane for GC/MS analysis. Validation tests with
a spiked extract demonstrated that 4 min of methylation were required for
efficient methylation. When recovery of the surrogate compound (0-methyl-
podocarpic acid) suggested the possibility of inefficient derivatization,
extracts were rederivatized. Samples were re-extracted when rederivatization
had no apparent effect.
Chlorinated Phenols--Extract aliquots to be analyzed for chlorinated
phenols were derivatized to generate acetate derivatives, which were far more
amenabl-e to GC analysis than,the underivatized compounds. The 5-mL extracts
were reduced in volume (0.5 ml) and treated with sodium acetate (1 g) and
acetic anhydride (3 ml) in a 15-mL culture tube. After 1 h of heating at
60° C, the derivatized extracts were cooled and water (3 ml) and hexane
(3 mL) were added. The hexane layer was removed and the water was re-
extracted twice with 3 ml of hexane. The hexane extracts were combined,
dried with Na2SC>4, and concentrated to 1 ml for GC/MS analysis.
The efficiency of derivatization was monitored on a sample-by-sample
basis by including routine searches for the underivatized surrogate recovery
compounds during GC/MS analysis. Underivatized surrogates were detected in
three samples, but the areas of the underivatized compounds were always less
than 5 percent of the areas of the derivatized compounds. Thus, rederiva-
tization was considered unnecessary for these samples.
Instrumental Analysis
Resin acids were analyzed by full-scan GC/MS and chlorinated phenolics
were analyzed by GC/MS-SIM (selected ion monitoring).
55
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Resin Acids bv Full Scan GC/MS--Full scan analyses were performed with
a fused silica capillary column (0.25 mm ID x 30 m, DB-5, J & W Scientific).
The GC oven temperature was programmed from 35° C (held 5 min) to 300° C at
8° C/min (held at 300° C for 8 min). The injection internal standards were
d,Q-phenanthrene and d^-chrysene. Qualitative identification was based on
retention "times and evaluation of mass spectra. All mass spectra were
reviewed during QA evaluation.
Chlorinated Phenols bv GC/MS-SIM--Chlorinated phenols were analyzed by
GC/MS-SIM. This technique was chosen because full scan GC/MS analyses were
considered insufficiently sensitive for- analysis of chlorinated phenols.
Seven ion descriptor windows were used in the 26-min analysis, with two to
six ions per window. Two ions were scanned for each target compound. The
two ions selected for each compound were typically the two most intense ions
in their mass spectra; for a given compound, both ions represented the same
molecular fragment, but differed by two atomic mass units (AMUs) because of
the natural isotopic abundances of Cl and Cl. Such .chlorine isotope
peaks are characteristic -features of spectra of chlorinated organic
compounds. The spectra of the acetate derivatives were very similar to
those of the underivatized compounds, because the parent ions including the
acetate group were not predominant.'
Because GC/MS-SIM analysis does not yield mass spectra, qualitative
identification was based on comparison of retention times and chlorine
isotope peak ratios to those of authentic standards. A compound was
reported as undetected if its ion ratio in a sample differed by more than a
factor of 2 from that in the standard. This criterion, while somewhat
arbitrary, was based on the most extreme variations observed for the
injection internal standards (dg-naphthalene, d10-acenaphthene, and d1Q-
phenanthrene). In most cases, ratios in samples agreed very well with those
in standards and were well within a factor of 2. Co-eluting interferences
were assumed to be a predominant source of variation of ion ratios in sample
extracts. Of all analytes, 2,3,4,6-tetrachlorophenol most often had ion
ratios that deviated from standards by more than a factor of 2.
56
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Detection Limits--
Sample-specific detection limits for chlorinated phenols were based on
instrumental sensitivity (i.e., 0.1 ng on-column, the lowest concentration
standard used for initial calibration), final extract volume (1 ml), and
sample weight. Several sample chromatograms were examined and the baseline
noise was estimated in the retention time region of the target compounds.
Detection limits were above three times the signal:noise ratio. Compounds
reported between 0.05 and 0.1 ng on-column were qualified with an E, and
compounds reported by the laboratory at <0.05 ng on-column were reported as
undetected at the detection limit.
For resin acids, sample-specific detection limits were based on a 5 ng
on-column instrumental sensitivity, final extract volume (1 ml_), and sample
weight. Although the lowest standard concentration used during initial
calibration was 25 ng on-column, the laboratory analyzed a 5 ng on-column
standard and demonstrated linearity from 5 to 150 ng on-column and acceptable
mass spectra at 5: ng on-column. Hence, 5 ng on-column was considered a
reasonable basis for detection limits. "In fact, acceptable mass spectra were
observed in many samples for compounds detected at <5 ng on-column. Com-
pounds detected below the stated detection limits were reported with an E
(estimated value) unless area counts were lower than 1000 units, in which
case the compounds were reported as undetected. For all compounds except
abietic acid, an area of 1000 units corresponded to 0.3 to 1.6 ng on-column;
for abietic acid, the corresponding concentration was 4 ng on-column.
Initial Performance Tests-
Initial performance tests were conducted for resin acid and chlorinated
phenols analysis because the overall procedures were not standardized or
routine for the laboratory prior to this study. Results from spiked blank
analyses for resin acids and chlorinated phenols (Table 9) were considered
acceptable. The resin acid spiked blank analyses included a silica gel
column chromatography cleanup step that was not used during sample analysis.
57
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TABLE 9. RESULTS OF INITIAL PERFORMANCE TESTS
(SPIKED BLANKS)
Resin acids:
Sandaracopimaric acid
Isopimaric acid
Palustric acid
Dehydroabietic acid
Abietic acid
Neoabietic acid
14-Chlorodehydroabietic acid
12-Chlorodehydroabietic acid
Dichlorodehydroabietic acid
Chlorinated Phenols^:
2-Chlorophenol
2,4-Dichlorophenol
2,4,6-Trichlorophenol
2,4,5-Trichlorophenol
2,3,4, 6-Tetrachl orophenol
Pentachlorophenol
4,5,6-Trichloroguaiacol
Tetrachl oroguai acol
2,6-Dibromophenolc
4-Bromo-2-chl orophenol0
Spike
Level (ug)
1
1
1
1
2
2
1
1
1
0.04
0.04
0.04
0.04
0.04
0.04
0.04
0.04
0.10
0.10
Percent
Run 1
65
63
47
70
49
45
54
56
63
89
96
82
86
97
87
92
84
96
85
Recovery
Run 2
61
58
39
65
47
41
56
56
65
76
87
76
78
76
75
61
67
94
84
RPDa
6.3
8.3
19
7.4
4.2
9.3
3.6
0
3.1
16
9.8
7.6
9.8
24
15
41
23
2.1
1.2
a Relative percent difference.
b 3,4,5-Trichloroguaiacol was not added.
c Surrogate compound.
58
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Laboratory Analysis for Volatile Organic Compounds
Sample analysis followed a hierarchical procedure based on results for
selected samples. Thirty-five samples were delivered to Analytical Re-
source's, Inc. (Seattle, Washington). Ten samples were designated to be
analyzed only if target compounds were detected in specified associated
samples. None of the 10 contingency samples required analysis.
Samples were analyzed by EPA/CLP procedures for volatile organic
compounds (purge-and-trap GC/MS).
Ancillary Analyses
Grain Size--
Grain-size determinations were performed by Battelle Northwest Marine
Research Laboratory (Sequim, Washington). Approximately 25 g of homogenized
wet sediment was treated with hydrogen peroxide to remove organic material.
Sediment was then wet-sieved through a 0.0625-mm screen and the fines were
collected in a cylinder. Sand and gravel fractions (0.0625 to >2 mm) were
wet-sieved and then dried to constant weight at 90° C. The silt-clay
fraction (<0.004 to 0.0625 mm) was treated with a preweighed dispersant and
analyzed by pipetting 20 ml at 30-sec intervals for 10-in depth, and 59-min
intervals for 5-cm depth. Pipetted samples were dried at 90° C to constant
weight and then corrected for dispersant weight. Results were calculated
based on total weight of the eight fractions. The following size fractions
were evaluated:
gravel - >2 mm
very coarse sand - 1-2 mm
coarse sand - 0.5-1 mm
medium sand - 0.25-0.5 mm
fine sand - 0.125-0.25 mm
very fine sand - 0.0625-0.125 mm
silt - 0.004-0.0625 mm
clay - O.004 mm.
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Sulfides--
Water-soluble sulfides were measured by AmTest, Inc. (Redmond, Washing-
ton) according to the method described in Green and Schnitker (1974). In
this method, a 0.005 or 0.05 M Pb (0104)2 titrant was used for sample
titration.
Total Organic Carbon and Total Nitrogen--
Total organic carbon and nitrogen were analyzed by Weyerhaeuser
Analytical and Testing Services (Federal Way, Washington), using a Carlo-Erba
NA 1500 Elemental Analyzer and following PSEP protocols.
Quality Assurance/Quality Control Results
Reviews of sediment chemistry data were performed in accordance with
PSEP guidelines (Tetra Tech 1986g). QA/QC reviews of chemistry included
assessments of accuracy [using standard reference materials (SRM), matrix
spikes, and surrogate recoveries, when applicable], precision (using
analytical replicates), initial and ongoing calibration and tuning, blank
results, sample holding times, and initial performance tests or validation
data for certain non-CLP procedures.
Detailed QA reports were prepared for chemical analyses and were
compiled in a single document (Tetra Tech 1988a). These reports are not
reproduced here, but are summarized below.
Metals--
The sample results are considered acceptable as qualified. Because
precision control limits were exceeded for antimony, all positive antimony
data are considered to be estimated and were assigned an "E" qualifier.
Assessment of the Effect of Analytical Procedure on Metals Results-.Tho
analytical methods used to determine metals in this study were designed to
60
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measure the total concentrations of metals in sediments (including mineral -
bound components), in contrast to methods that rely on partial digestion. A
small study was conducted (PTI and Tetra Tech 1988) to examine the implica-
tions of using the "total metals" methods, especially when comparing results
to historical reference area data generated by "strong acid" methods (e.g.,
reference area data from Carr Inlet). The analytical methods used in the
present study were the same as those used by PTI and Tetra Tech (1988) and
analyses were performed by the same laboratory (Battelle Northwest Marine
Research Laboratory).
Two archived Carr Inlet samples collected during the Commencement Bay
Remedial Investigation (Tetra Tech 1985a) were analyzed in triplicate by
"total metals" methods used in the present study and by the "strong acid"
method (per EPA CLP) used during the Commencement Bay study. In addition,
selected samples collected during the Elliott Bay study (PTI and Tetra Tech
1988) were reanalyzed by the "strong acid" method for comparison purposes-.
The results are presented in Table 10.
Although differences were observed for a number of metals analyzed by
both methods, the consistently largest differences were observed for
chromium (Table 10). In both Carr Inlet samples, mean chromium concentra-
tions by "total metals" methods (in this case, XRF) were over 4 times the
mean concentrations determined by the "strong acid" technique. Samples with
higher overall chromium concentrations from Port Susan and Elliott Bay/
Duwamish River (PTI and Tetra Tech 1988) tended to have approximately a
factor of 2 difference between "total metals" and "strong acid" results.
Differences between antimony results by "total metals" vs. "strong acid"
methods could not be determined for Carr Inlet samples because antimony was
consistently undetected by the "strong acid" procedure (Table 10). However,
data reported for Samples CR-11 and CR-13 during the Commencement Bay
Remedial Investigation were roughly 15 times lower than the "total metals"
values in Table 10. Similarly, for Duwamish River Samples WW-12 and EW-15,
the "total metals" procedure (including hydrofluoric acid digestion and
analysis by GFAA) resulted in antimony concentrations roughly 10-20 times
higher than concentrations determined by the "strong acid" procedure. This
61
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TABLE 10. COMPARISON OF ANALYTICAL METHODS FOR SELECTED METALS
Reference
Area Samples
Elliott Bay/
Ouwamish
River Samples
CTi
ro
Sample
CR-11 (n=3)
CR-11 (n=3)
CR-13 (n=3)
CR-13 (n=3)
PS-01 (n=l)
PS-01 (n=3)
WW-12 (n=l)
WW-12 (n=2)
WW-12 (n=l)
EW-15 (n=l)
EW-15 (n=2)
EW-15 (n=l)
NH-04 (n=l)
NH-04 (n=l)
KG-06 (n=l)
KG-06 (n=l)
WW-14 (n=l)
WW-14 (n=l)
SS-09 (n=l)
SS-09 (n=l)
Technique
Total metal3
Strong acidc
Total metal
Strong acid
Total metal
Strong acid
Total metal
Strong acid
XRF"
Total metal
Strong acid
XRF
Total metal
XRF
Total metal
XRF
Total metal
XRF
Total metal
XRF
Antimony Arsenic
1.91 + 0.16b 4.47 + 0.79
U0.92 ± 0 2.07 ± 0.09
1.40 + 0.18 3.69 + 1.1
U0.92 + 0 2.48 + 0.52
2.66
DO. 92 + 0
1,200
59 + 6.6
240
150
14 + 1.2
32
504
120
192
27
1,370
217
680
547
Cadmium Chromium Copper
0.09 + 0.01 99 + 26 9.8 + 1.6
0.13 ± 0.01 19 ± 1.5 6.1 ± 0
0.19 + 0.02 84 + 10 12.6 + 0.36
0.22 ± 0.01 19 ± 1.5 6.73 ± 1.4
236 49.8
133 ± 2 43.3 ± 1.1
555 618
266 + 12 920 ± 33
223 176
115 ±.2.8 305 ± 33
Lead
4.4 + 1.2
3.6 ± 0.1
8.1 + 0.55
2.2 ± 0.60
10.4
5.6 ± 2.4
1,180
1,510 ± 69
210
330 ± 40
Nickel Silver
17.7 + 3.1 0.043 + 0
13.8 ± 1.3 0.027 ± 0.002
20.6 + 0.85 0.076 + 0.029
15.1 ± 1.3 0.022 ± 0.007
139
130 ± 2
100
87 ± 3.6
63.8
45.9 ± 2.7
Zinc
28.2 + 1.7
19.3 ± 0.58
34 + 2
19 + 0.6
a Methods used in the present study: digestion with nitric, perchloric, and hydrofluoric acids and analysis by AA (for antimony, cadmium, and silver) or x-ray fluorescence
(for arsenic, chromium, copper, lead, nickel, and zinc).
Mean + standard deviation. All concentrations are in mg/kg DW.
c EPA CLP procedure involving digestion with nitric acid and hydrogen peroxide.
X-ray fluorescence.
-------
marked discrepancy prompted reanalysis by an independent and more reliable
technique for antimony (i.e., XRF). Comparisons between XRF and the "total
metals" procedure used in this study were confounding (Table 10), but
suggest that antimony concentrations observed during this study could be
considerable overestimates (e.g., by a factor of approximately 5).
The XRF analysis of antimony aroused sufficient uncertainty about the
antimony concentrations reported in this study that antimony data were not
used to define or rank problem areas. However, antimony distributions are
discussed in the Results section because of their potential value in
assessing relative antimony contamination in Everett Harbor.
Semivolatile Organic Compounds
The data for A/B/N organic compounds are generally acceptable. The
laboratory followed specified protocols with the following exceptions:
The relative response factor for N-nitrosodiphenylamine was
outside control limits (25 percent difference) for 11 of the
15 daily standard analyses. Positive sample results for
N-nitrosodiphenylamine in all samples associated with the 11
standard analyses have been qualified in the database with an
"E" (estimated).
Benzoic acid levels in one of four blanks exceeded the PSEP
control limit of 2.5 ug total (Tetra Tech 1986g). Analyses
were not halted while investigating the cause of contamina-
tion. Therefore, benzoic acid values for the batch of
samples run with this blank were qualified with an "E" after
blank correction.
Method blanks were analyzed with each extraction batch. Phenanthrene,
pyrene, phenol, naphthalene, and 2-methylnaphthalene were detected at
relatively low levels in some blanks (Table 11).
63
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TABLE 11. METHOD BLANK SUMMARY
Lab ID
26987018
Date
Extracted
12/1/86
Date
Analyzed
1/1/87
Compound
Phenanthrene
Di-n-butyl phthalate
Pyrene
Bi s (2-ethyl hexyl ) phthal ate
Concentration3
(ug/kg DW)
4
26
3
46
CRDLb
10
10
10
10
27987036 12/8/86 1/14/87 Phenol
Naphthalene
Benzoic acid
Di-n-butyl phthalate
Bi s(2-ethylhexyl)phthalate
Di-n-octyl phthalate
32
2
160
160
48
4
25
10
10
10
10
10
26987054
12/10/86 1/19/87 Phenol
Naphthalene
Di-n-butyl phthalate
Pyrene
Bi s (2-ethyl hexyl ) phthal ate
Di-n-octyl phthalate
2-Methyl naphthalene
20
4
15
2
44
28
' 2
25
10
10
10
10
10
10
a Concentrations in blanks are based upon 80 g wet weight of sediment and an assumed
50 percent moisture. These values provide a means for comparison of blank contamination
to observed concentrations in sediment samples.
b Contract required detection limit.
64
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PCBs--
The PCB data are considered acceptable when qualified as estimates.
Qualification was necessary because only a single-point calibration was used
for quantification. All positive results above 50 ug/kg DW in the database
were generated by GC/MS analyses because of interferences encountered during
GC/ECD analyses. Precision (based on blind replicates), and accuracy (based
on matrix spikes and SRM) for these analyses were well within PSEP limits
except for the results of one matrix spike (EW-04MS), in which the PCB
concentration was considerably lower than in the unspiked sample. This
discrepancy was not explained. However, the relatively high concentration
in unspiked sample EW-04 was confirmed by re-extraction and re-analysis.
Extracts for GC/MS analysis were held longer than the 40-day holding time
specified by the EPA CLP. The extended extract holding time may have
resulted in an underestimate of original sample concentrations, although
degradation of PCBs in solvent is not expected because of the well-documented
stability of this class of compounds (e.g., Hutzinger et al. 1974).
'Chlorinated Pesticides--
Many chlorinated pesticide samples required dilution because of inter-
ferences, resulting in higher detection limits than those specified in the
"Quality Assurance Project Plan for Field Investigations to Support Develop-
ment of the Everett Harbor Action Plan" (Tetra Tech 1986f). In addition,
because of sample dilutions, no precision and accuracy data were obtained for
this sample set. However, the review of calibration data suggests that the
analytical instrument was operating within acceptable limits. PSEP protocols
were used to assess the acceptability of data and data qualifiers were not
assigned to pesticide results.
Resin Acids and Chlorinated Phenols/Guaiacols--
Overall, data for resin acids and chlorinated phenols/guaiacols are
considered acceptable. Palustric acid data were rejected based on 0 percent
recoveries in both matrix spikes; this was not an unexpected result, as this
compound is susceptible to isomerization and degradation during analysis
65
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(NCASI 1986). Data reported by the laboratory were changed to detection
limits during QA review if they did not exceed blank values by a factor of 5
or, for chlorinated phenols, if ion ratios in samples differed from those in
standards by a factor of 2 or more. Data were qualified with an "E" for
several possible reasons: 1) if data were reported at a concentration
corresponding to less than half the lowest calibration standard; 2) if data
were associated with an ongoing calibration that was outside PSEP limits; or
3) if mass spectra were only marginally acceptable (applicable to only a few
reported values).
In the two sets of duplicate analyses performed for resin acids,
precision exceeded the 100 percent PSEP control limit for three resin acids
in one set of duplicates (sandaracopimaric acid, isopimaric acid, and
abietic acid) (Table 12). Data were not qualified based on precision
because several lines of evidence suggested that the low precision for
several compounds in Station EW-07 (Table 12) was the result of heterogeneous
sample contamination and/or matrix effects rather than analytical error.
This argument is based on the following lines of evidence:
Duplicate spiked blank analyses (see Table 9) resulted in
precision of 0 to 9 percent for all resin acids (except
palustric acid, which was rejected)
Precision for matrix spikes of two relatively uncontaminated
samples was <11 percent for all resin acids (Table 13)
Precision for resin acids at Station SS-03 (Table 12), which
was a far less complex sediment matrix than Station EW-07 in
terms of contaminant assemblage and sediment texture (e.g.,
organic carbon content), ranged from 7.4 to 50 percent for
the three resin acids detected at Station SS-03 (the detected
resin acids included two of the three resin acids with >100
percent precision at Station EW-07).
66
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TABLE 12. PRECISION FOR RESIN ACIDS
Compound
Sandaracopi marie acid
Isopimaric acid
Palustric acid
Dehydroabietic acid
Abietic acid
Neoabietic acid
14-Chlorodehydroabietic acid
12-Chlorodehydroabietic acid
Dichlorodehydroabietic acid
Compound
Sandaracopimaric acid
Isopimaric acid
Palustric acid
Dehydroabietic' acid
Abietic acid
Neoabietic acid
14-Chlorodehydroabietic acid
12-Chlorodehydroabietic acid
Dichlorodehydroabietic acid
EW-07a
(ug/kg)
E350
E760
U500
6,300
3,200
E240
1,400
4,100
E640
SS-03
(ug/kg)
E34
E130
U170
E180
U170
U170
U170
U170
U170
EW-16a
(ug/kg)
3,800
6,200
U300
9,500
14,000
680
1,600
5,400
770
SS-03 Dup
(ug/kg)
E85
E140
U210
E300
U210
U210
U210
U210
U210
X
E2,100
E3 , 500
--
5,100
8,600
E460
1,500
4,800
E710
X
E60
E140
--
. .E240
--
--
--
--
--
RPDb
170
160
--
41
130
96
13
27
18
RPDb
86
7.4
--
50
--
--
--
--
--
a EW-07 and EW-16 were blind duplicates.
b Relative percent difference.
67
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TABLE 13. RESULTS OF MATRIX SPIKES - RESIN ACIDS
Compound
Sandaracopimaric acid
Isopimaric acid
Palustric acid
Dehydroabietic acid
Abietic acid
Neoabietic acid
14-Chlorodehydroabietic acid
12-Chlorodehydroabietic acid
Dichlorodehydroabietic acid
Spike
Level
(ug)a
50
50
50
50
100
100
50
50
50
Percent
SS-03
88
82
0
98
83
62
84
84
79
Recovery
PS-03
92
87
0
88
87
58
93
92
85
Average
Percent
Recovery
90
85
0
93
85
60
89
88
82
RPDb
4.4
5.9
0
11
4.7
6.7
10
9.1
7.3
a These spiking levels correspond to 1,300-1,800 ug/kg DW (twice these
concentrations apply for abietic and neoabietic acid).
b Relative percent difference.
68
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Volatile Organic Compounds--
The data for volatile organic compounds are acceptable with the
exception of data for methylene chloride (a common laboratory contaminant).
Methylene chloride values were rejected because of excessive blank contamina-
tion.
Ancillary Analyses--
The overall quality of sulfide data is acceptable. However, the 7-day
holding time limit recommended by PSEP (Tetra Tech 1986g) was exceeded for
51 of 64 samples collected. The effect of holding time exceedance is not
clear. Technical holding times have been established only for water
matrices. It is possible that sample integrity was compromised by biological
or chemical changes occurring in the sample. Sulfide concentrations can
decrease due to the degassing of hydrogen sulfide or the oxidation of
sulfides to elemental sulfur. The observation of undetected sulfide
(detection limit = 20 mg/kg DW) reported for Station EW-01. was probably an
analytical, error, based on the extremely strong sulfur odor that was
recorded in field notes during sample collection and processing.
Data for grain size, total organic carbon, and total nitrogen were
acceptable without qualification.
BIOACCUMULATION
Field Sampling
English sole (Parophrvs vetulus) were sampled at 10 transects in Everett
Harbor and at 1 transect at Port Susan, a nonurban reference area (see
Figure 6). Port Susan was used as a reference area because previous studies
have found that the area is relatively uncontaminated (Malins et al. 1982).
In addition, Malins et al. (1984) found no serious hepatic lesions in English
sole collected from that embayment.
69
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Sampling of English sole was conducted between 25 August and 2 September
1986. Fish were collected using a 7.6-m (headrope) Marinovich otter trawl
having a body mesh size of 3.2 cm (stretched) and cod-end liner mesh size of
0.8 cm (stretched). Trawling was conducted along each transect at a
constant vessel speed of approximately 2.5 kn during daylight hours
(0800-1730 h).
Five of 60 English sole (>220 mm) that were collected for histopatho-
logical analysis (see below, Fish Ecology and Histopathology) were selected
for analysis of PCBs, EPA priority pollutant pesticides, and mercury in raw
muscle tissue. After removal of liver and otoliths, each fish was wrapped
in aluminum foil and stored on ice until transfer to the freezer at -20° C.
In the laboratory, fillets of dorsal muscle tissue were excised and skinned
with a stainless steel spatula in preparation for analysis.
Dungeness crabs (Cancer maaister) were collected between 25 August and
21 October 1986 primarily from otter trawls conducted for fish sampling and
from crab pots deployed near the trawl stations. Crabs from the East
Waterway (Station EW-91) were obtained from a crab pot fisherman at Pier 1.
Male crabs were selected from the catch at each site, placed in polyethylene
bags, and stored live on ice. At the end of each sampling day, samples were
transferred to a freezer and stored at -20° C until analysis. In the
laboratory, crabs were thawed, and samples of cheliped tissue from eight
crabs were composited into a single sample per site. Two additional
replicate composite samples were analyzed for Station EW-91.
Laboratory Analysis for Mercury
Mercury was the only EPA priority pollutant metal analyzed in fish and
crab tissue because of its high potential for bioaccumulation. Digestion and
instrumental techniques followed PSEP protocols (Tetra Tech 1986g). Muscle
tissue was homogenized and subjected to nitric acid/perchloric acid digestion
at Battelle Northwest Laboratories (Sequim, Washington). The digestate was
analyzed by cold vapor atomic absorption spectrophotometry.
70
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Laboratory Analysis for PCBs/Pesticides
Extraction and Cleanup--
The analytical procedure used by Battelle Northwest Laboratories
(Sequim, Washington) was derived from Tetra Tech (1986b). Only the sections
relevant to analysis of PCBs and pesticides were followed. The procedure
involves Soxhlet extraction with CH2Cl2/MeOH (2:1, vol/vol), extract cleanup
by gel permeation chromatography (Biobeads S-X3; elution with CI^C^) and
alumina column chromatography, and capillary column GC/ECD. Several notable
exceptions to the Tetra Tech (1986b) procedure were cited in the laboratory's
cover letter:
Soxhlet extraction was carried out for 12 h rather than the
specified 24 h
Rotary evaporation was used fo'r extract concentration rather
than the specified K-D apparatus.
These two modifications did not appear to affect laboratory performance based
on results of initial laboratory performance tests with SRMs and spiked blanks
conducted by Battelle during a previous study (PTI and Tetra Tech 1988).
GC/ECD Analysis and Quantification--
Pesticides and PCBs were analyzed by capillary column GC/ECD with a DB-5
quantification column (0.25-mm i.d. x 30 m, J & W Scientific) and a SP-608
(Supelco, Inc.) confirmation column. The 80-min temperature program used
for these samples allowed for a high degree of chromatographic resolution
[roughly 76 peaks were resolved in a PCB standard consisting of Aroclor
1242:1254:1260 (1:1:1, wt/wt/wt)].
The quantification procedure used for PCBs is described in Tetra Tech
(1986b). The procedure involves peak-by-peak quantification using an
internal standard. Relative response factors for resolved peaks in a PCB
standard containing Aroclors 1242, 1254, and 1260 (the range of PCB congeners
71
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expected in environmental samples) were determined by measuring the indi-
vidual peak concentrations by GC/MS and then using dilutions of the same
standard for initial and ongoing GC/ECD calibrations.
Extracts containing pesticides identified on the DB-5 column were rerun
on the SP-608 confirmation column.
Quality Assurance/Quality Control Results
Reviews of bioaccumulation data were performed in accordance with PSEP
guidelines (Tetra Tech 1986g). QA/QC reviews included assessments of
accuracy (using standard reference materials, matrix spikes, and surrogate
recoveries, when applicable), precision (using analytical replicates),
initial and ongoing calibration and tuning, blank results, and sample
holding times.
Detailed QA reports were prepared for chemical analyses and were
compiled in a single document (Tetra Tech 1988a). These reports will hot be
reproduced here, but'are summarized in this section-.
Mercury Bioaccumulation
Mercury data exhibited accuracy and precision within the guidelines
established by PSEP (Tetra Tech 1986g). However, because the 28-day maximum
sample holding time recommended by PSEP was exceeded for all of the tissue
samples analyzed, sample results for mercury are considered to be estimates
and were assigned an "E" qualifier.
PCB/Pesticide Bioaccumulation--
All detected data for PCBs in tissue were qualified as underestimates
("G", or greater than) because of low analytical recoveries observed
throughout the sample case. Recoveries of the two surrogate compounds
[4,4'-dibromooctafluorobiphenyl (DBOFB) and isodrin] in most samples, and
PCB recoveries in all three tissue matrix spikes, were below PSEP limits of
50 percent for accuracy (Tetra Tech 1986g). An interlaboratory comparison
72
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with selected tissue samples and using a similar extraction/cleanup procedure
confirmed the low PCB recoveries for Battelle. The cause of the low
recoveries could not be identified and recoveries did not improve during re-
extraction and re-analysis of selected samples. In addition, an "E"
qualifier was assigned to samples associated with ongoing calibrations that
were outside control limits. Sample and extract holding times exceeded
PSEP guidelines; however, the target .analytes (particularly PCBs) are not
very susceptible to microbial or chemical alteration, particularly at the
reduced temperatures of storage. No additional qualification was considered
necessary to address holding time exceedances.
SEDIMENT BIOASSAY
Field Sampling
Sediment toxicity tests with Rhepoxvnius abronius were performed at 29
stations in the Everett Harbor system and three stations in the reference
area (Port Susan). A subsample of the composite sediment sample collected
for chemical analyses was tested for toxicity using the amphipod bioa-ssay.
Field collection methods for sediment samples are described above (see
Sediment Chemistry, Field Sampling).
The infaunal amphipod R. abronius was collected subtidally from West
Beach on Whidbey Island (Washington) using a bottom dredge. Amphipods were
maintained and transported in clean coolers with ice, and were returned to
the laboratory within 18 h of collection.
Laboratory Analysis
Following their arrival in the laboratory, amphipods were kept in
holding containers filled with fresh seawater (28 ppt salinity) and clean
sediment and maintained at 15+1° C under continuous light until used in
testing. Cultures were aerated but not fed during acclimation and were held
for not more than 10 days. Prior to testing, amphipods were sorted by hand
from sediments and identifications were confirmed using a Wild M5 dissecting
microscope. Damaged, dead, or unhealthy individuals were discarded.
73
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Interstitial salinities of all test sediments were measured before
testing. Of the 34 sediments tested (32 stations plus two field replicates),
10 had interstitial salinities less than 25 ppt: samples from Stations
ES-01, ES-02, ES-03, NG-12, NG-14, SR-01, SR-02, SS-01, SS-03, and SS-07. In
each case, interstitial salinity was elevated to at least 25 ppt by mixing
the sediment with water of- a sufficiently high salinity following methods
outlined by PSEP protocols (Tetra Tech and E.V.S. Consultants 1986).
Acute lethality of amphipods exposed for 10 days to whole, fresh (un-
frozen) sediments was measured using the methodology of Swartz et al. (1982,
1985) as amended by PSEP protocols (Tetra Tech and E.V.S. Consultants 1986).
A 2-cm layer of test sediment was placed in 1-L glass jars and covered with
800 ml of clean seawater (28 ppt salinity). Each beaker was seeded (randomly
and blindly) with 20 amphipods and aerated. Six replicates (20 amphipods
each) were run per test sediment. Five beakers served to determine toxicity,
while the sixth beaker served as a reference for daily measurement of water
chemistry (i..e., pH, dissolved oxygen, salinity, and temperature). Testing
was conducted at 15±1° C under constant light. Test containers were checked
daily to establish early trends in mortality and sediment avoidance, and
also to gently sink any amphipods that had left the sediments overnight and
become trapped by surface tension at the air/water interface. A negative
(clean) control sediment from the amphipod collection site at West Beach,
Whidbey Island was tested concurrently with each series of test sediments.
Following PSEP protocols (Tetra Tech and E.V.S. Consultants 1986), cadmium-
spiked (CdCl2) seawater was used as a positive control to verify that the
amphipods were responsive. Amphipod bioassays were initiated on all
sediments within a 2-week period following field collection of sediments.
Bioassay tests were terminated after 10 days, when sediments were sieved
(0.5-mm screen), and live and dead amphipods were removed and counted.
Amphipods were considered dead when there was no response to physical
stimulation and microscopic examination revealed no evidence of pleopod or
other movement. Missing amphipods were assumed to have died and decomposed
prior to the termination of the bioassay (Swartz et al. 1982, 1985).
74
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Quality Assurance/Quality Control Results
Mean mortality ranged from 4 to 10 percent in the clean sediment
(Whidbey Island) controls. A mean mortality of 10 percent is considered
acceptable for amphipod sediment bioassay controls (Swartz et al. 1985).
ANOVA indicated no significant differences (P>0.05) in mean mortality values
among the clean sediment controls. Mortality in cadmium-spiked seawater was
100 percent, which is consistent with the expected mortality rate. Intersti-
tial salinities in nine sediment samples were not acceptable according to
PSEP Protocols (Tetra Tech and E.V.S. Consultants 1986) and were adjusted
following the PSEP Protocols. Dissolved oxygen concentrations in water
overlying the sediments in the bioassay chambers were acceptably high.
The amphipod bioassay results are considered acceptable for use in
problem area identification. However, it should be noted that the data for
the following stations showed high variance (standard error >12), generally
due to an extreme outlier replicate: SR-07, EW-10, and OG-03.
BENTHIC MACROINVERTEBRATES
Field Sampling
Benthic macroinvertebrates were collected at 16 stations in the Everett
Harbor study area and three stations in the Port Susan reference area between
30 September and 15 October 1986 (see Figure 5). Station depths ranged from
3.4 m to 21.4 m among the 19 stations. Most of the stations were located at
depths of 7.9 m to 12.8 m, but it was not possible to sample within this
depth range at all stations because of differences in shoreline bathymetry.
Five replicate grab samples were collected at each station, for a total
of 95 samples. All samples were collected using a 0.1-m^ modified van Veen
grab sampler. In the field, samples were washed on a sieve with 1.0-mm mesh
openings and fixed with a 10 percent solution of buffered formalin. Sample
tracking records followed each sample through all stages of sample collection
and laboratory processing.
75
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The field sampling methods used to" collect benthic macroiinvertebrate
samples during the Everett Harbor survey are outlined in the PSEP protocols
(Tetra Tech 1986g) and the "Quality Assurance Project Plan for Field Investi-
gations to Support Development of the Everett Harbor Action Plan" (Tetra Tech
1986f). The following discussion summarizes those procedures.
Following deployment and retrieval of the van Veen grab, it was placed
in a sieve stand and the sediment sample was inspected carefully to determine
the acceptability of the sample. Samples were rejected if excessive leakage
or surface disturbance occurred. Samples were also rejected if they did not
meet or exceed the following minimum penetration depths:
Medium to coarse sand and gravel - 4 to 5 cm
Fine sand and sandy silt - 7 to 10 cm
Silt - 10 cm.
When a sample was judged to be acceptable, the following qualitative sediment
characteristics were recorded:
Penetration depth
Sediment texture
Sediment color
Presence and strength of odors
Degree of leakage and/or surface disturbance
Presence of debris or shell fragments.
After the foregoing observations were recorded, the sampler was opened
and the sediment was released into the top section of the sieving stand. The
sediment was then washed from above with a gentle spray of seawater, and the
76
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larger masses of sediment were broken apart. Sediment was rinsed into a
sieve box in the-lower level of the sieving stand. The sediment in the sieve
box was then completely washed until materials no longer passed through the
1.0-mm mesh screen. That portion retained on the screen was placed in a
plastic sample bag having external and internal labels. Samples were then
fixed in the field with a 10 percent solution of Borax-buffered formalin.
Laboratory Analysis
In the laboratory, benthic macroinvertebrate samples were washed on a
0.5-mm sieve and transferred to a 70 percent solution of isopropyl alcohol
for long-term preservation. Organisms retained on the sieve were sorted into
major taxonomic groups (e.g., polychaetes, molluscs, crustaceans, misc.) and
enumerated. Planktonic organisms that occurred in the samples were not
enumerated. Colonial organisms that occurred in the samples were noted as
"present" but also were not enumerated.
Quality' control checks of sample sorting were performed by resorting 20
percent of each sample. The 20-percent aliquot was taken after the entire
sample had been spread out on a sieve with 0.025-mm mesh openings. If the
20-percent re-sort indicated a calculated difference of 5.0 percent or
greater in total sample abundance for all taxa combined, the entire sample
was resorted. Tetra Tech also performed independent quality control checks
of sorting procedures (including checks of 20-percent aliquots) and checks of
abundance counts for the major taxonomic groups. Samples that failed either
quality control check were resorted completely.
Organisms in the samples from Everett Harbor and Port Susan (i.e., 19
stations) were identified to the lowest possible taxonomic level and
enumerated. Specimens of each species (or lowest possible taxon) that
occurred in the Everett Harbor study area were placed in reference museums
prepared by the taxonomists.
77
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Quality Assurance/Quality Control Results
QA/QC procedures resulted in an acceptable data set without qualifica-
tion. Quality control checks of sample sorting, organism enumeration, and
identification followed the guidelines recommended by PSEP protocols (Tetra
Tech 1986g) and the "Quality Assurance Project Plan for Field Investigations
to Support Development of the Everett Harbor Action Plan" (Tetra Tech 1986f).
FISH ECOLOGY AND HISTOPATHOLOGY
Field Sampling
Field sampling methods were described earlier (see Bioaccumulation,
Field Sampling). English sole larger than 220-mm total length (TL) were
selected for histopathological analysis. This size limit was used to ensure
that most fish were greater than 2 yr old. A selection criterion based
indirectly on age was used because English sole younger than 2 yr old have
substantially lower prevalences of hepatic lesions than older fish7 (Maiins
et al. 1982). The present study therefore focused on those fish most likely
to be afflicted with hepatic lesions.
Sixty English sole of appropriate length were collected at every
transect, yielding a total of 714 fish for the overall study. Immediately
after collection, each selected fish was sacrificed by a blow to the head,
measured to the nearest millimeter (TL), examined for grossly visible
external abnormalities (e.g., fin erosion, skin tumors, scoliosis, para-
sites), and transferred to the shipboard laboratory for liver removal.
In the shipboard laboratory, the liver of each fish was removed in its
entirety, cut into multiple sections, and examined for the presence of
grossly visible lesions. If lesions or discontinuities were noted, a
subsample was taken from the affected area for histopathological analysis.
If the liver appeared to be normal, a subsample was taken from the center of
the organ at its broadest point. Each subsample was fixed in 10 percent
neutral-buffered formalin. After the liver was removed from each individual,
78
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the sex of the fish was noted and the otoliths (sagittae) were removed for
subsequent age determination.
All fishes in the remainder of the catch at each transect were identi-
fied to species and counted. All English sole not selected for histopatho-
logical analysis were measured (nearest mm TL) and counted.
Laboratory Analysis
Each formalin-fixed liver was dehydrated in a graded series of ethanol,
cleared in xylene, and embedded in paraffin. Embedded livers were sectioned
at 4 urn using a rotary microtome and stained using hematoxylin and eosin
(H&E). Prepared slides were examined using conventional light microscopy.
Each slide was coded, so the pathologist did not know where the corresponding
fish was captured. Lesion identifications were confirmed by Mr. M.S. Myers
(Chief Pathologist, Northwest and Alaska Fisheries Center) to ensure their
consistency with the identifications made by Malins et al. (1980, 1982,
1984).
Three major kinds of idiopathic hepatic lesion were evaluated:
neoplasms, foci of cellular alteration, and megalocytic hepatosis. Briefly,
neoplasms include both benign and malignant tumors. Foci of cellular
alteration are discrete clusters of altered cells that have specific
staining characteristics and are suspected of being preneoplastic. Megalo-
cytic hepatosis is a specific degenerative condition characterized by a
marked increase in both nuclear and cellular diameters in the absence of
cellular inflammatory responses.
Prevalences of all three major lesions have been found to be elevated in
English sole from urban embayments of Puget Sound (e.g., Malins et al. 1984;
Becker et al. 1987). In addition, Myers et al. (1987) found consistent
patterns of co-occurrence of these lesions in English sole from Eagle
Harbor. Based on those patterns of co-occurrence and comparisons with
similar lesions induced in rodents following laboratory exposure to chemi-
cals, Myers et al. (1987) concluded that megalocytic hepatosis, foci of
cellular alteration, and neoplasms may be related sequentially in the
79
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progression towards hepatic neoplasia in English sole. In that scenario,
the following steps are thought to occur:
Megalocytic hepatosis and associated degenerative lesions are
induced'as the initial, subchronic to chronic manifestations
of the cytotoxic effects of hepatocarcinogens. These lesions
form the proper stimulus for a proliferative response.
In the above environment favoring proliferation, foci of
cellular alteration develop. Because these lesions are
selectively resistant to the cytotoxic effects of hepatocar-
cinogens, they have a growth advantage over normal hepato-
cytes.
Autonomous, neoplastic hepatocytes arise from the nonautono-
mous foci of cellular alteration to form neoplasms. This
final transformation is probably a complex, multistep process
of mutation followed by selection.
Quality Assurance/Quality Control Results
Lesion identifications were confirmed by Mark Myers of the National
Marine Fisheries Service. To ensure consistent identification of lesions
between the three pathologists for this project, each examined slides from
every station. For all three major kinds of lesions, the numbers of each
lesion identified by the three pathologists were very similar, implying
consistent diagnostic criteria. In addition, the relative prevalences of
neoplasms and foci of cellular alteration among stations and among lesion
types were similar to results from previous studies by the National Marine
Fisheries Service (Malins et al. 1980). Although the relative prevalences
of megalocytic hepatosis among stations were consistent with patterns
identified by Malins et al. (1980), the absolute values found during this
study were considerably lower than those found by Malins et al. (1980). The
pathologists were aware of this apparent discrepancy shortly after the
laboratory analyses began and therefore paid particular attention to
identifying the presence of this abnormality. In addition, a review of
80
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selected slides by M. Myers confirmed the relatively low prevalence of
megalocytic hepatosis. Therefore, it was concluded that the prevalences
observed in this study were accurate. .The final histopathology data were
considered acceptable without qualification.
DATA MANAGEMENT
To facilitate data storage, QC, and analysis; recent and historical
data from the Urban Bay Action Programs have been incorporated into a
microcomputer database. The database software performs a wide variety of
retrievals, reports, and analyses. It also allows data to be transferred
directly to other software (e.g., SPSS/PC+ and Lotus 1-2-3) for statistical
analyses and graphic displays. A library system is incorporated into the
database to document data sources, changes to data, and other information to
be linked to sample measurements.
Data Organization
Data are linked so that related kinds of information can be retrieved
together for interdisciplinary analyses. For example, sediment chemistry,
infauna abundances, and bioassay data can be retrieved into a single table,
based on common samples or stations. During data retrievals, data can be
summarized across laboratory replicates and field replicates as requested by
the user.
The database design requires that only actual measurements be recorded.
For example, if cadmium was measured at all stations but one during a survey,
no value for cadmium need be stored for that single station. This reduces
ambiguity and complexity of the database as well as storage requirements and
retrieval speed. For biological effects data, a distinction is made between
"not significant" (as compared to a reference area) and "not evaluated."
Each data value is associated with a single survey and station. The
survey identifies the sampling program responsible for data collection. The
station coordinates identify a unique geographic position sampled during that
survey. Stations are described by an identifier, latitude and longitude, and
81
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basin and subbasin codes. Samples collected at each station are further
identified by a unique sample ID, the date of collection, and field replicate
number. Data of any type can be retrieved by:
Date - all dates or a specified range
Survey - any survey or only data from one or more specific
surveys
Station - any station or only data from one or more specific
stations
Basin and subbasin - any basin/subbasin or only data from one
or more specific basin/subbasin.
These criteria allow any subset of the data to be retrieved or combined for
analysis.
Data Analysis
Procedures for summarization of data are programmed into the database,
providing consistent treatment and formatting of the data for analysis and
interpretation. These procedures include, for example, the ability to rank
observations by station or chemical; create new variables (such as sums of
HPAH and LPAH); construct species lists by replicate, sample, or station; and
compare data to AET or other sediment quality values. Statistical analyses
were carried out using SPSS/PC+, and Lotus 1-2-3 was used for other analyses
and data manipulations.
Data Entry and Quality Control
QC of data entry was based upon technical evaluation of the data,
automated error-checking procedures in the database, and consistent and
reliable automated procedures for retrieving and summarizing the data. All
additions of data and modifications to data were documented, and the appro-
priate document reference code linked to the affected samples. The date was
82
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automatically inserted in all permanent output from the database. Technical
review of the data was carried out before data entry and during analysis and
interpretation. Automated error-checking procedures were used to screen data
to preclude erroneous codes, duplicate data, and insufficiently or incor-
rectly identified data (e.g., measurements that are not assigned to a
previously defined station). All access to the database was carried out
through a series of menus and prompts, ensuring that all summaries and
analyses were carried out in a consistent and replicable manner.
83
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RESULTS
Results of field investigations in the Everett Harbor system and Port
Susan are presented in the following sections on sediment chemistry,
bioaccumulation, sediment bioassays, benthic macroinvertebrates, and fish
ecology and histopathology. An evaluation of data collected during the
present study and comparisons with recent data from previous studies is
provided in each section.
SEDIMENT CHEMISTRY
The following section provides a summary of chemical results for over
50 subtidal and intertidal sediment samples collected from the Everett
Harbor system and an additional three samples collected from the Port Susan
reference area. Not all target, chemicals were measured at all.stations. At
54 stations, chemical data were collected for !! EPA priority pollutant
metals, 54 acid/base/neutral EPA priority pollutant organic compounds, PCBs,
19 chlorinated pesticides (mostly EPA priority pollutants), 10 additional
Hazardous Substance List compounds, and 15 selected TIO compounds (see
Table 1). At 31 stations, including some of the 54 stations discussed
above, eight resin acids and nine chlorinated phenols and chlorinated
guaiacols were analyzed by dedicated procedures (see Table 1). Nineteen
samples were also analyzed for 35 volatile organic compounds (mostly EPA
priority pollutants). TBT was measured at two stations. In addition,
sediment conventional variables (e.g., grain size distribution and total
organic carbon content) were analyzed in all 60 sediment samples. The
objectives of this section are to:
Provide a chemical perspective of the Everett Harbor study
area, including the general distributions, concentration
ranges, and frequencies of detection of chemical contaminants
84
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Determine the magnitude of contamination relative to reference
area conditions and to determine the significance of this
contamination relative to Puget Sound reference areas
Summarize spatial correlations to define groups of chemicals
with similar distribution patterns
Interpret historical data to supplement the sediment chemistry
results of the present study.
All chemical data and sediment conventional data are presented in Appendix B.
Normalization of Chemical Concentrations
Sediment concentrations presented in this report are typically expressed
as the weight of contaminant per dry weight of sediment (e.g., ug/kg DW).
Normalization of sediment concentrations to other variables [e.g., percent
organic carbon or percent of fine-grained material (silt plus clay)] can aid
in the interpretation of contaminant distributions by focusing on the most
contaminated fractions of sediment, thus reducing the significance of
variations in less important components of sediment texture and composition.
The following is a brief description of each type of normalization.
Dry Weight Normalization--
Most sedimentary contaminants are associated primarily with the solid
material in bulk sediments, not with the interstitial water. Thus, dry
weight contaminant concentrations are preferred to wet-weight concentrations.
Use of dry weight concentrations precludes the possibility that variations
in sedimentary moisture content will obscure informative trends in chemical
data.
Total Organic Carbon Normalization--
Chemical concentration gradients, particularly of nonpolar, nonionic
compounds, have been observed to correlate well with sedimentary organic
85
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carbon content (e.g., Choi and Chen 1976). This observation is commonly
interpreted in one of two ways:
1. Organic matter is the "active fraction" of sediment and
serves as a sorptive sink for neutral, and possibly polar or
metallic, compounds
2. Carbon-rich particles may be an important transport medium
for contaminants [e.g., HPAH may be associated with soot
particles (Prahl and Carpenter 1983)].
The occurrence of multiple contaminant sources in a localized area can
obscure gradients of concentrations normalized to TOC content.
Strong correlations of dry weight chemical concentrations with TOC
content, a good indication of the appropriateness of TOC normalization, were
typically not observed in this study, even in the area with highly elevated
TOC concentrations (the East Waterway). Thus, TOC normalization is mentioned
infrequently in this - section. Notably, many .of the organic chemicals
observed in this study were ionizable (e.g., phenols). Such relatively
polar compounds do not conform well to the assumptions of organic carbon
normalization theory.
Normalization to Percent Fine-Grained (<63 urn) Particles--
On a limited spatial scale, contaminant concentrations are often
inversely correlated with particle size (e.g., Lee 1985). Thus, contaminants
(especially metals) may be concentrated in the fine-grained particles of
bulk sediments. This observation is often explained in terms -of surface
area, in that finer particles have greater specific surface area, and thus
greater sorption capacity, than larger particles. However, organic carbon
content also tends to vary inversely with particle size in natural sediments
(Choi and Chen 1976). Thus, normalizing to percent fines may be effectively
equivalent to normalizing to organic carbon content in natural sediments.
86
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Bulk Sediment Characteristics
Bulk sediment characteristics measured for this study included grain
size distribution (as percent sand, silt, and clay), TOC, nitrogen, and
water-soluble sulfides.
Grain Size--
Average percentages of fine-grained material in the seven study areas
and Port Susan are presented in Figure 7. Several general trends are
apparent. Sediments from Nearshore Port Gardner (Area NG) were the most
coarse-grained of all study areas, probably because fine-grained material
cannot accumulate under the existing current velocities and wave energies.
Four of the NG stations were intertidal. Sediments further offshore in
deeper water (Area OG) were more fine-grained. Sediments in Ebey Slough,
Steamboat Slough, and the Snohomish River Delta study areas were relatively
coarse. Most of the sediments collected from the Snohomish River were
relatively coarse (<20 percent fines); however, Stations SR-04 and SR-05 had
predominantly fine-grained sediments (>60 percent fine-grained material) and
Station SR-07 (located in a sheltered area of the Snohomish River, outside
the main channel) had the highest percentage of fine-grained material in the
study (96 percent). Fine-grained sediments at these three SR stations are
responsible for the elevated mean in Figure 7. Sediments in the East
Waterway were typically the most fine-grained in the study, probably
because of the proximity of sources of fine-grained material, and because of
relatively quiescent conditions within the waterway. Sediment texture of
Port Susan reference sediments collected during the 1986 Everett Harbor
survey was relatively coarse (<15 percent fine-grained material at all three
stations).
A more detailed summary of grain-size distributions in the East
Waterway is presented in Figure 8. The stations are arranged geographically
in Figure 8, with the eastern shore of the East Waterway at the bottom of
the figure and the head (i.e., north end) of the waterway on the right side
of the figure. Most sediments were predominantly fine-grained (>50 percent
fine-grained material) with the finest sediment texture at the head of the
87
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Ul
UL
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80-
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LEGEND
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NG OG EW SD SR SS ES
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S R Snohornish River
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STUDY AREA
Figure 7. Average percent fine-grained material (silt plus clay) in sediments from all study areas.
-------
en
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EW-09 EW-06 EW-03
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EW-15 EW-14 EW-13 EW-12 EW-10 EW-07 EW-04 EW-01
STATIONS
Figure 8. Percent fine-grained material (silt plus clay) in sediments
of the East Waterway.
89
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waterway (Stations EW-02 and EW-03, >90 percent fine-grained material).
However, sediment at Station EW-12 was unusually coarse relative to other
sediments along the east shore (<10 percent fine-grained material), and
sediments at Stations EW-14 and EW-15 near the mouth were also relatively
coarse (30 to 40 percent fine-grained material).
Total Organic Carbon--
Sediment TOC concentrations (Figure 9) displayed trends similar to
those observed for percent fine-grained material. The correlation between
percent fine-grained material and TOC was moderate (r=0.71, n=60, PO.05),
based on a regression that included all sediment stations. A comparison
between sediments collected from nearshore and offshore Port Gardner
illustrates this relationship. With the exception of a single station
(NG-09), the relatively coarse-grained sediments collected in Area NG had
less than 1 percent TOC content. The finer-grained offshore sediments
(Area OG) had higher levels of TOC (2 to 4 percent). The relatively coarse
sediments in Ebey Slough and Steamboat Slough displayed relatively low
levels of TOC (<1 percent), as did sediments from the Snohomish River (with
the exception of relatively fine-grained Stations SR-04, SR-05, and SR-07).
The fine-grained sediments in the East Waterway had extremely high levels of
TOC (mean of 11 percent, maximum of 29 percent).
A more detailed summary of TOC distributions in the East Waterway is
presented in Figure 10. TOC and fine-grained content of sediments did not
covary well within this waterway. Wastes rich in organic matter discharged
into the East Waterway likely account for the highly elevated TOC levels in
this area and for deviations from the inverse relationship between particle
size and TOC content often observed in natural sediments. The highest
levels of TOC were found at Stations EW-04 and EW-13 (23 to 29 percent), not
in the very fine-grained sediments near the head of the waterway.
Average molar organic carbon to nitrogen (C/N) ratios in the seven
study areas and Port Susan are summarized in Figure 11. The molar C/N ratio
can provide information about the type of organic matter in the sediments.
For example, marine phytoplankton are observed to have a C/N ratio of
90
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29.4
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LEGEND
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P S Port Susan
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OG Offshore Port Gardner
EW East Waterway
S D Snohomish River Delta
S R Snohomish River
S S Steamboat Slough
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STUDY AREA
Figure 9. Average total organic carbon (TOG) content (as percent dry weight) in sediments
from all study areas.
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STATIONS
Figure 10. Total organic carbon (TOC) content (as percent dry
weight) in sediments of the East Waterway.
92
-------
102
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STUDY AREA
Figure 11. Average carbon/nitrogen (C/N) molar ratios in sediments from all study areas.
-------
approximately 7, soil and participate material in rivers have C/N ratios of
10 to 15, and woods have considerably higher C/N ratios (e.g., between 150
and 550; Hedges et al. 1985, 1986). Average C/N ratios were relatively
consistent (between 15 and 25) among Everett Harbor study areas except for
East Waterway and' offshore Port Gardner, which had average molar C/N ratios
of approximately .40. Two stations in the East Waterway, EW-04 and EW-13,
exhibited anomalously high C/N ratios (69 and 100, respectively). These ele-
vated ratios are consistent with pulp mill activities in this area, although
other source materials (e.g., coals) also have relatively high C/N ratios.
Sulfides--
The distribution of water-soluble sulfide concentrations in sediments
is summarized in Figure 12. Because sulfide is indicative of sulfate-
reducing (poorly oxygenated) conditions, it is common for sulfide levels to
be high in areas that are rich in organic material and high in oxygen
demand. In general, this relationship was observed in this study. The
correlation between TOC and sulfides was moderate (r=0.61, n=60, PO.05).
Mean sulfide concentrations in Port Susan.and throughout most of the study
areas were relatively low (<120 mg/kg DW). The highest mean (3,000 mg/kg DW)
and individual (11,000 mg/kg DW) sulfide concentrations were found in the
East Waterway. The highest sulfide concentration at an individual station
outside of the East Waterway was 600 mg/kg DW observed at Station SR-07 in
the Everett marina.
A more detailed summary of sulfide concentrations in the East Waterway
is presented in Figure 13. With the exception of Station EW-01, sediments
near the head of the waterway contained the highest sulfide concentrations.
The undetected sulfide value reported at Station EW-01 (detection limit =
20 mg/kg DW) is probably an analytical error, based upon an observation of
an extremely strong sulfur odor that was recorded in field notes during
sample collection and processing. Sulfide concentrations decreased toward
the mouth of the waterway. The discharge of sulfite pulp wastes in the East
Waterway and sulfur-rich discharges from a storm drain in the northeast cor-
ner of the waterway are probably important sources of sulfur and relatively
high oxygen demand in this area (particularly at the head of the waterway).
94
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STUDY AREA
Figure 12. Average sulfide concentrations (mg/kg dry weight) in sediments from all study
areas.
-------
10.000 -i
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STATIONS
Figure 13. Sulfide concentrations (mg/kg dry weight) in sediments
of the East Waterway.
96
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Sediment Chemistry; Metals
Concentration ranges and detection frequencies for the 14 metals
analyzed in this study are presented in Table 14. All metals except
selenium and TBT" were detected in all samples analyzed. Concentration
ranges were broad for many of the metals, spanning two to three orders of
magnitude. Maximum values of most metals occurred in the East Waterway
(Table 14). This broad range in sediment metal concentrations can be
attributed to a single station (EW-14), at which the concentrations of
several metals (i.e., antimony, arsenic, copper, lead, zinc) were 5-25 times
higher than at all other stations in the study area. Chromium and selenium
were exceptions, displaying maximum concentrations at Stations NG-15 and
NG-01, respectively. Nickel was also an exception, displaying a maximum
concentration at Station SR-07. Chromium, selenium, and nickel concen-
trations at these stations were not substantially elevated relative to their
concentrations at other stations within the study area.
TBT was only measured at two stations, one in the Port Susan reference
area (Station PS-02) and the other near the Everett marina (Station SR-07).
The estimated concentration of TBT at Station SR-07 was elevated above the
single measured reference concentration (undetected at 0.006 mg/kg DW) by a
factor of 15.
Sediment Metals of Concern--
Metals of concern are metals that occurred at concentrations exceeding
those in Puget Sound reference areas. It is assumed that the range of
reference concentrations provides a reasonable measure of the possible
variability of concentrations in relatively uncontaminated sediments.
The range of trace metal concentrations in Puget Sound reference areas
is summarized in Table 15. Metal concentrations from Port Susan sediments
collected for this study (Stations PS-02 to PS-04) are included among the
reference values summarized in Table 15. Metals concentrations at Port
Susan stations (1986 data) were within the ranges observed for other Puget
Sound reference areas.
97
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TABLE 14. CONCENTRATIONS OF METALS AND
TRIBUTYLTIN IN SURFACE SEDIMENTS
OF EVERETT HARBOR AND PORT SUSAN
Chemical
Antimony
Arsenic
Cadmi urn
Chromium
Copper
Iron
Lead
Manganese
Mercury
Nickel
Selenium
Silver
Zinc
Range
(mg/kg dry wt)
El. 21
2.62
0.04
51
10.6
16,600
4.4
282
0.006
24.1
U0.20
0.007
38
- E203
- 685
- 7.94
- 271
- 1,010
- 90,600
- 517
- 1,050
- 0.776
- 69a
- 0.58a
- 1.03a
- 5,910
Detection
Frequency
54/54
54/54
54/54
54/54
54/54
54/54
54/54
54/54
54/54
54/54
17/54
54/54
54/54
Location of
Maximum
EW-14
EW-14
EW-14
NG-15
EW-14
EW-14
EW-14
EW-14
EW-14
SR-07
NG-01
EW-14
EW-14
Tributyl tin
U0.006 - 0.093
1/2
SR-07
a Maximum observed concentration in this study does not exceed the
maximum concentration observed among Puget Sound reference areas.
98
-------
TABLE 15. SUMMARY OF METAL CONCENTRATIONS IN SEDIMENTS
FROM PUGET SOUND REFERENCE AREAS
Chemical
Antimony
Arsenic
Cadmium
Chromium
Copper
Lead
Mercury
Nickel
Selenium
Silver
Zinc
Range (mg/kg dry wt)a
U0.1c-2.79 (E1.52C-E2.18)
1.9-17 (6.7-10.1)
0.047-1.9 (0.047-0.082)
9.6-E255 (89-232)
5-74 (13.6-16.7)
UO.1-24 (5.6-10.9)
0.01-0.28 (0.029-0.056)
4-140 (41.3-65)
UO. 1-1.0 (0.27-0.40)
UO.02-3.3 (0.020-0.027)
15-E102 (39.1-51.5)
Detection
Frequency
19/39
41/41
31/31
45/45
35/35
28/35
45/45
33/33
21/31
31/33
33/33
Reference
Sites5
1,2,3,4,7,8,9,10,11
1,2,3,4,7,8,9,10,11
1,2,3,4,6,9,10,11
1-11
1,2,3,4,5,6,9,10,11
1,2,3,4,5,6,9,10,11
1-11
1,2,3,4,5,9,10,11
1,2,3,4,6,9,10,11
1,2,3,4,5,9,10,11
1,2,3,4,5,9,10,11
a The range of Port Susan concentrations from this study (Stations PS-02 to PS-04) is
shown in parentheses.
5 Reference sites: 1. Carr Inlet 5. Port Madison 9. Sequim Bay
2. Samish Bay 6. Port Susan 10. Port Susan (1985)
3. Dabob Bay 7. Nisqually Delta 11. Port Susan (1986)
4. Case Inlet 8. Hood Canal
c U = Undetected at the detection limit shown.
E = Estimated value.
References:
(Site 1) Tetra Tech (1985a); Crecelius et al. (1975)
(Site 2) Battelle (1986)
(Site 3) Battelle (1986)
(Site 4) Crecelius et al. (1975); Mai ins et al. (1980)
(Site 5) Mai ins et al. (1980)
(Site 6) Mai ins et al. (1982)
(Site 7) Crecelius et al. (1975)
(Site 8) Crecelius et al. (1975)
(Site 9) Battelle (1986)
(Site 10) PTI and Tetra Tech (1988)
(Site 11) This study.
99
-------
Eight of eleven EPA priority pollutant metals analyzed in this study
had concentrations exceeding the highest Puget Sound reference concentrations
and are thus of concern. Nickel, selenium, and silver concentrations did
not exceed Puget Sound reference area values, and are thus not considered of
concern in this study. Chromium will not be considered further because only
one station (NG-15) had a chromium concentration that exceeded the maximum
Puget Sound reference concentration, and it exceeded it by only 17 percent.
In addition to the EPA priority pollutant metals, TBT exceeded the single
reference area measurement at the single study area station at which it was
measured. The limited number of samples tested for TBT does not allow for
interpretation of spatial distributions.
A summary of the distributions of the metals of concern is presented in
Table 16. In this table, EAR are used to describe chemical distributions.
An EAR is the ratio of the dry weight concentration of a chemical divided by
the average concentration determined for six Carr Inlet stations (Tetra Tech
1985a). Threshold EAR values (Table 16) are the EAR equivalent of the
maximum concentration in Puget Sound reference areas. Thus, EAR values
above the threshold value indicate exceedance of the maximum Puget Sound
reference concentration. The threshold EAR value is exceeded by a factor
of 10 only at Station EW-14. The most elevated concentrations for all metals
of concern were observed in the East Waterway, at Station EW-14 (Table 16).
Also shown in Table 16 is the maximum EAR excluding Station EW-14. With
this station excluded, the maximum concentrations measured in the study area
for metals of concern (except antimony) were elevated above threshold EAR
values by a factor of less than 4.
Mean EAR values for metals of concern in Everett Harbor study areas are
illustrated in Figure 14. The mean EAR values for the East Waterway
including Station EW-14 are denoted with a dashed line (Figure 14). Cadmium
and mercury concentrations exceeded maximum reference concentrations at only
four stations, all located in the East Waterway (maximum EAR values for
cadmium and mercury were 8.4 and 19, respectively). Copper concentrations
exceeded maximum reference concentrations in the East Waterway and at
Station SR-07 in the Snohomish River. Lead concentrations exceeded maximum
reference concentrations in the East Waterway, at Station SR-07, and at
100
-------
TABLE 16. RANGE IN EAR FOR METALS OF CONCERN
IN SEDIMENTS OF EVERETT HARBOR AND PORT SUSAN
Chemical
Antimony
Arsenic
Cadmium
Chromium
Copper
Lead
Mercury
Zinc
Rangeb
11-1,850
0.78-203
0.04-8.4
3.4-18
1.7-160
0.48-56
0.15-19
2.0-310
(240)
(8.0)
(4.8)
(18)
(15)
(9.6)
(12)
(14)
EAR3
Median
29
2.4
0.14
7.3
3.8
1.2
1.2
3.2
Threshold0
25
5.0
2.0
17
12
2.6
7.0
5.4
Areas where Threshold
Exceeded by 10
EW-14
EW-14
--
EW-14
EW-14
--
EW-14
Times*"
a Dry-weight concentration in study area sediments divided by the average
concentration measured in six Carr Inlet sediments (Tetra Tech 1985a).
b Value in parentheses is the maximum EAR value excluding Station EW-14.
c The threshold EAR is defined as the ratio of the maximum reference sediment
concentration in Puget Sound divided by the average for six Carr Inlet
reference sediments. Above the threshold EAR, the dry-weight concentration
of a study area sediment contaminant would exceed the maximum concentration
reported for any Puget Sound reference site listed in Table 15.
d The contaminant EAR values for the listed stations exceeded the threshold
level by at least one order of magnitude. The factor of 10 was arbitrary,
but was useful for indicating the areas of greatest contamination. Sediments
from the underlined stations had the highest observed concentrations.
101
-------
UI
U
n ANTIMONY (Sb)
EJ ARSENIC (As)
ui
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s 75 : ; .
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s to- 1^ :'
S ^ N T r « - r.-J M & (-t-n W pfc S
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ARSENIC
ELEVATION ABOVE REFERE
(dry waight)
7
/
/
LEGEND
' T T1 Includes Station EW14
PS
NG
OG
ew
so
SR
ss
ES
Excludes Station EW14
Port Susan
Nearshore Port Gardner
Offshore Port Gardner
East Waterway
Snohomisn River Delta
. Snonomisn River
Steamboat Slough
Ebey Slough
* THRESHOLD - equivalent to the
highest concentration in Puget
Sound reference areas.
IT
UI
I
> I
I
' 2. 3-
-«rnBESHO.O*(Pb)
2 -^ THOESHOIO* (Cd)
UI
UI
n
Reference (mg/kg DW) =. 0.11 (Sb),
3.4 (As), 19(Zn).6.4(Cu), 15 (Cr),
0.95 (Cd), 9.2 (Pb), and 0.04 (Hg).
PS
NG OG EW SD SR SS ES
STUDY AREA
Figure 14. Mean EAR of metals of concern from all study areas.
102
-------
Station ES-01. Zinc and arsenic concentrations exceeded maximum reference
concentrations in the East Waterway, at Station SR-07 and two other fine-
grained Snohomish River stations (SR-04 and SR-05), and at Station ES-01.
Antimony had' the greatest EAR of all metals measured in Everett Harbor
study areas. Mean EAR values for antimony exceeded threshold EAR values in
all study areas except Area NG (Figure 14). However, reported antimony
concentrations may be overestimates by a factor of 5 and were thus not
considered appropriate for problem identification and ranking (see Sediment
Chemistry. Quality Assurance/Quality Control Results in Methods section).
Antimony data are presented in Figure 14 for comparative purposes.
Sediment Chemistry: Organic Compounds
The concentration ranges (ug/kg DW) and detection frequencies of
semi volatile and volatile organic compounds detected at least once in the
study area are presented in Table 17. Among those organic compounds with
the highest detection frequencies and reported at the highest concentrations
were 4-methylphenol, dehydroabietic and abietic acids (among other resin
acids), PAH (naphtha-lene in particular), and several tentatively identified
compounds (most notably, a diterpenoid hydrocarbon, possibly dehydroabie-
tane). Maximum concentrations of all EPA priority pollutant PAH, all
measured resin acids, phenol and all alkyl-substituted phenols, all chlori-
nated phenols, all chlorinated guaiacols, PCBs, most TIO compounds, and all
detected volatile organic compounds occurred in the East Waterway, as did
the maximum concentrations of most metals of concern (Table 17). Within the
East Waterway, maximum concentrations of a number of compounds were observed
at Stations EW-01 (particularly chlorinated phenols and guaiacols), EW-04
(including certain resin acids, certain phenols, most TIO compounds, and
PCBs), EW-07 (most notably 4-methylphenol and naphthalene), EW-13 (certain
resin acids), and EW-14 (especially PAH and benzoic acid). Structures of
some of the compounds listed in Table 17 are depicted in Figure 15. Note
that some TIO compounds were identified by mass spectral characteristics
(e.g., base peak m/z 181) or structural characteristics deduced from mass
spectra (e.g., compound class); these compounds will be described in more
detail later in this section.
103
-------
TABLE 17. CONCENTRATIONS OF DETECTED SEMIVOLATILE AND
VOLATILE ORGANIC COMPOUNDS IN SURFACE SEDIMENTS
OF EVERETT HARBOR AND PORT SUSANa
Chemical
LPAH
naphthalene
acenaphthylene
acenaphthene
f 1 uorene
phenanthrene
anthracene
HPAH
fl uoranthene
pyrene
benz(a)anthracene
chrysene
benzof 1 uoranthenes
benzo( a) pyrene
i ndeno ( 1 , 2 , 3 -c , d ) pyrene
di benzo(a,h)anthracene
benzo ( g , h , i } pery 1 ene
Total PCBs
Resin Acids
abietic acid
dehydroabi'etic acid
12-chlorodehydroabietic acid
14-chlorodehydroabietic acid
dichlorodehydroabietic acid
isopimaric acid
neoabietic acid
sandaracopimaric acid
Phenols and Guaiacols
phenol
2-methyl phenol
4-methyl phenol
2, 4-di methyl phenol
2-chlorophenol
2,4-dichlorophenol
2 . 4 , 6-tri chl orophenol
2,4,5-trichlorophenol
2,3,4, 6-tetrachl orophenol
pentachl orophenol
3,4, 5-trichloroguaiacol
4,5,6-trichloroguaiacol
tetrachloroguaiacol
Chlorinated Benzenes
1 , 2-di chl orobenzene
1 , 4-di chl orobenzene
Phthalates
dimethyl phthalate
di ethyl phthalate
di-n-butyl phthalate
butyl benzyl phthalate
bis(2-ethylhexyl Iphthalate
di-n-octyl phthalate
Range .
(ug/kg dry wt)°
L36 28,000
B3 X17.000
1 800
2 - 5,200
6 - 4,300
3 - 8,100
1 6,100
L36 - 23,000
3 3,700
3 - 5,500
1 3,200
1 3,200
5 4,100
1 1,700
1 730
2 270
3 550
Ul - E9.600
U130 98,000
E20 83,000
£61 11,000
E46 3,400
U130 E710
E85 £11,000
E79 El 4, 000
E17 14,000
11 2,900
6 1,200
3 X98.000
U10 520
El 160
2 320
U2 290
El 120
U2 120
U2 E460
El 110
U2 48
U2 50
7 96
2 25C
8 26°
3 - llc
BIO 260C
U10 70
BIO 930
B3 4C
Detection
Frequency
54/54
46/54
41/54
45/54
24/54
50/54
51/54
54/54
53/54
49/54
54/54
54/54
48/54
50/54
42/54
29/54
46/54
7/54
21/31
29/31
19/31
10/31
5/31
20/31
8/31
21/31
49/54
3/54
50/54
2/54
11/60
21/60
22/60
18/60
6/31
22/60
11/31
6/31
4/31
4/54
14/54
2/54
5/54
20/54
6/54
39/54
3/54
Location of
Maximum
EW-14
EW-07
EW-14
EW-14
EW-14
EW-04
EW-14
EW-14
EW-13
EW-14
EW-14
EW-14
EW-14
EW-14
EW-14
EW-14
EW-14
EW-04
EW-13
EW-04
EW-04
EW-04
EW-04
EW-13
EW-13
EW-01
EW-10
EW-04
EW-07
EW-04
EW-04
EW-01
EW-01
EW-02
EW-01
EW-04
EW-01
EW-01
EW-01
EW-04
OG-02
NG-02
NG-02, SD-03
EW-13
EW-01
EW-14
SR-02, SR-03
104
-------
TABLE 17. (Continued)
Chemical
Range
(ug/kg dry wt)b
Detection
Frequency
Location of
Maximum
Pesticides
lindane (gamma-HCH)
p,p'-DDT
Nitrogen-Containing Compounds
N-ni trosodi phenylami ne
Miscellaneous Extractables and
Tentatively Identified Compounds
benzyl alcohol
benzoic acid
dibenzofuran
2-methylnaphthalene
1-methylpyrene
U0.5 lc
Ul 23
8 57
retene
a "
U10
E10
3
2
U
U
810
5,900
5,000
7,400
E240
E3.100
1/54
1/54
13/54
6/54
25/54
44/54
38/54
25/54
44/54
NG-04
SD-03
EW-01
EW-04
EW-14
EW-14
EW-07
NG-11
EW-04
cymene (unspecified isomer)
di benzothi ophene ,
l,2,4-trithiolaned
diterpenoid hydrocarbon
(base peak 255)
diterpenoid alcohol
(base peak 271)
hexadecanoic acid
hexadecanoic acid methyl ester*:
hexadecenoic, acid methyl ester
cholesterol IJ
campesterol
alkanol (unidentified).01
base peak 181, isomer #1^
base peak 181, isomer #2
U
U
U
U
U
U -
U
U
U
U
U
U
U
E2.900
E280
E5,800
E23,000
E8.600
E2.300
E4.300
£3,200
E630
El, 100
E2,200
£12,000
£6,500
41/54
19/54
31/54
41/54
42/54
27/54
53/54
53/54
51/54
20/54
43/54
44/54
45/54
EW-04
EW-14
EW-04
EW-04
EW-11
EW-10
EW-04
EW-04
EW-04
EW-04
EW-04
EW-04
EW-04
Volatile Organic Compounds
acetone
ethyl benzene
total xylenes
U6
U3
U3
230
E5C
39
4/19
2/19
4/19
EW-05
EW-09
EW-08
a Qualifiers:
U Substance undetected at the detection limit shown.
B - Blank corrected down to the detection limit shown.
X The surrogate recovery for this compound was low (<10 percent). Hence, the recovery
correction was at least a factor of 10.
L "Less than" the reported concentration is the mean of a detected value and a
detection limit or, for PAH sums, the sum includes detection limits.
E = Estimated value.
Maximum is the highest detected value even if maximum detection limits were higher.
c Maximum concentration does not exceed Puget Sound reference area concentrations.
Tentatively identified organic (TIO) compound detection limits for TIO compounds were
not assigned.
105
-------
OOOH
DEHYDROABIETIC ACID
COOH
NEOABIETIC ACID
DEHYDROABIETANE '
(a diterpenoid hydrocarbon)
TOTAROL*
(a diterpenoid alcohol)
RETENE'
COOH
CHLORODEH YDROABIET1C
ACID (12-or 14-chloro-)
COOH
OICHLORODEHYDROABIETIC
ACID
3 TIO (tentatively identified
organic compound) - (he
identity ot these compounds
was not confirmed with
authentic standards during
analysis. Dehydroabietane
and totarol are proposed
as possible identities based
upon mass spectral
characteristics, but other
diterpenoid hydrocarbons/
alcohols are possible.
COOH
ISOPIMARIC ACID
COOH
SANDARACOPIMARIC ACID
OCH3
CHLORINATED GUAIACOLS
3,4,5-trichloro-
4,5,6-trichlorc-
tetrachloro-
CHLORINATED PHENOLS
2-chloro-
2.4-dicnloro-
2,4,6-lrichloro-
2,4,5-lrichioro-
2,3,4,6-tetrachloro-
pentachloro-
Figure 15. Structures of selected organic compounds observed
in sediments.
106
-------
Several semi volatile organic compounds were detected infrequently
(three or fewer times), including 2-methylphenol, 2,4-dimethylphenol,
dimethyl phthalate, di-n-octyl phthalate, lindane, and p,p'-DDT. The three
detected volatile organic compounds were detected four or fewer times.
Semi volatile organic compounds that were searched for but not detected
in any samples included all halogenated ethers, all nitrogen-containing
compounds other than N-nitrosodiphenylamine, 1,3-dichlorobenzene, 1,2,4-
trichlorobenzene, hexachlorobenzene, 2-chloronaphthalene, hexachlorobuta-
diene, hexachloroethane, hexachlorocyclopentadiene, 4-chloro-3-methylphenol,
and isophorone (see Tables 1 and 17). Most target chlorinated pesticides and
volatile organic compounds were not detected (see Tables 1 and 17).
Organic Compounds of Concern--
As described for metals, chemicals of concern are those chemicals that
occur at concentrations exceeding the range of Puget Sound reference areas.
The range" of concentrations of organic comprounds in Puget Sound reference
areas are summarized in Table 18. Concentrations in Port Susan sediments
analyzed for this study (Stations PS-02 to PS-04) are included in Table 18.
Port Susan concentrations were typically well within the range of concentra-
tions for other Puget Sound reference areas, although the maximum 4-methyl-
phenol concentration in Port Susan (290 ug/kg DW) (this study) was consider-
ably higher than the maximum value reported in Carr Inlet (32 ug/kg DW)
(Tetra Tech 1985a).
Organic compounds that did not exceed the range of Puget Sound reference
concentrations in this study were 1,4-dichlorobenzene, dimethyl phthalate,
diethyl phthalate, di-n-butyl phthalate, di-n-octyl phthalate, lindane, and
ethylbenzene (Tables 17 and 18). These compounds are thus of relatively
minor concern and will not be discussed further.
Distributions of contaminants of concern are summarized in terms of EAR
values in Table 19. Summaries of distributions of organic chemicals with
EAR >1,000 are presented in Table 20. The distributions of organic chemicals
of concern are summarized below.
107
-------
TABLE 18. SUMMARY OF ORGANIC COMPOUND CONCENTRATIONS
IN SEDIMENTS FROM PUGET SOUND REFERENCE AREAS3
Chemical
LPAH
naphthalene
acenaphthylene
acenaphthene
fl uorene
phenanthrene
anthracene
HPAH
fluoranthene
pyrene
benz(a)anthracene
chrysene
benzo(b)fl uoranthene
benzo(k)fl uoranthene
benzo( a) pyrene
i ndeno ( 1 , 2 , 3-c , d ) pyrene
di benzo(a, hjanthracene
benzo(g,h,i jperylene
Total PCBs
Resin Acids
abietic acid
dehydroabietic acid
12-chlorodehydroabietic acid
14-chlorodehydroabietic acid
dichlorodehydroabietic acid
isopimaric acid
neoabietic acid
sandaracopimaric acid
Phenols and Guaiacols
phenol
2-methyl phenol
4-methyl phenol
2, 4-di methyl phenol
2-chlorophenol
2,4-dichlorophenol
2,4,6-tnchlorophenol
2,4,5-trichlorophenol
2,3,4, 6-tetrachl orophenol
pentachlorophenol
3,4, 5-trichloroguaiacol
4,5,6-trichloroguaiacol
tetrachloroguaiacol
Chlorinated Benzenes
1 , 4-di chl orobenzene
1,2-dichlorobenzene
Phthalate Esters
dimethyl phthalate
di ethyl phthalate
di-n-butyl phthalate
butyl benzyl phthalate
bi s( 2-ethyl hexyl Jphthal ate
di-n-octyl phthalate
. I
Range (ug/kg dry wt)D f
4-L71 (L36-L42)
U0.5-U40 (B3-U10)
U0.1-U40 (1-U10)
U0.1-U40 (U10)
UO.1-40 (U10)
4-170 (4-7)
U0.5-U40 (1-2)
34-L100 (L36-L48)
5-100 (5-7)
5-120 (5-7)
2-U40 (2-3)
4-U40 (4-5)
U5-94
E4.8-94
UO. 37-40 (1-3)
UO. 37-30 (1-U10)
U0.4-E10 (2-U10)
El. 2-20 (3-4)
3.1-U50d (U50)
U130-U180
E20-U130
U130-U180
U130-U180
U130-U180
U130-U180'
U130-U180
U130-U180
UO.5-626 (Z100-Z200)
U0.7-U50 (U20-U50)
UO. 8-290 (84-290)
U1-U14 (U10)
U0.5-U9.4 (U3)
U0.5-U43 (U3)
U0.5-U38 (E2-L3)
U3-U37 (U3-L3)
U3
0.1-U50d (U3)
U3
U3
U3
U0.06-U40d (U10)
U0.06-U40d (U10)
U0.5-U50 (U10)
4-18 (U10),
U20-760 (BIO)1"
U0.5-U25 (U10)
U0.5-U25 (B10-Z58)T
U0.5-E56 (B3-U10)
Jetectlon
:requency
13/13
12/27
2/27
4/27
7/28
18/24
11/24
13/13
24/29
23/29
15/24
15/24
15/25
15/25
16/21
10/19
3/12
8/13
7/22
0/3
2/3
0/3
0/3
0/3
0/3
0/3
0/3
5/17
0/11
7/11
0/13
0/13
0/13
2/13
1/11
0/3
1/10
0/3
0/3
0/3
1/23
1/22
1/12
4/8
3/5
3/12
0/5
4/12
Reference
Sites0
1,8,9
1,2,3,4,5,6,8,9
1,2,3,4,5,6,8,9
1,2,3,4,5,6,8,9
All
1,2,3,6,7,8,9
1,2,3,6,7,8,9
1,8,9
All
All
1,2,3,6,7,8,9
1,2,3,6,7,8,9
1,2,3,4,5,6,7,8
1,2,3,4,5,6,7,8
1,3,4,5,6,7,8,9
1,4,5,6,7,8,9
1,8,9
1,7,8,9
1,2,3,4,6,7,9
9
9
9
9
9
9
9
9
1,2,3,8
--
1,8,9
1,8,9
1,8,9
1,8,9
1,8,9
1,8,9
9
1,8,9
9
9
9
1,2,3,4,5,8,9
1,2,3,4,5,8,9
1,8,9
1,9
1
1,8,9
1
1,8,9
108
-------
TABLE 18. (Continued)
Chemical
Range (ug/kg dry wt)
Detection
Frequency
Reference
Sites0
Pesticides
p,p'-ODT9
lindane (gamma-HCH)
Miscellaneous Extractables
benzyl alcohol
benzoic acid
di benzofuran
2-methylnaphtha! ene
1-methylpyrene
retene!'
cymene .
di benzothi ophene .
1,2,4-trithiolane" .
diterpenoid hydrocarbon
diterpenoid alcohol
hexadecanoic acid
hexadecanoic acid methyl
ester
,n
hexadecenoic acid methyl
ester"
cholesterol!]
campesterol
alkanol"
base peak 181, isomer #lP
base peak 181, isomer #2
Nitrogen-Containing Compounds
N-ni trosodi phenylami ne
Volatile Organic Compounds
acetone
ethyl benzene
total xylenes
U1.0-U10 (U1-U10) 0/12
U0.5-U50 (U0.5-U50) 0/9
U3.4-U20*3 (U20-U200) 0/6
U7.2-430d (E10-U100) 4/6
U5-E14 (U10-11) 4/11
E0.3-U22 (2-U10) 10/17
U 0/3
U-E130 (U-1.6) 8/13
U-12 1/4
U 0/3
U 0/3
U 0/3
E1.2-E3.; 3/3
U-E35 1/3
E380-E480 3/3
E330-E380 3/3
E19-E37 3/3
U 0/3
U 0/3
U 0/3
U 0/3
U0.5-U10 (U10) 0/8
U6 0/3
U3-U16 (U3) 0/11
U3 0/3
1,8,9
1,8,9
1,9
1,8,9
1,8,9
,4,5,6,8,9
9
1,8,9
1,9
9
9
9
9
9
1,9
9
2,3,9
9
a This table includes only chemicals that were detected in the present study.
Qual i fiers:
L = "Less than" the reported concentration is the mean of a detected value and a
detection limit or, for PAH sums, the sum includes detection limits.
U = Undetected at the detection limit shown.
E = Estimated value.
8 = Blank-corrected down to the detection limit shown.
Z = Value is blank-corrected but exceeds detection limit.
The range of Port Susan concentrations from this study (Stations PS-02, PS-03, and PS-04)
is in parentheses.
c Reference sites:
1. Carr Inlet
2. Samish Bay
3. Oabob Bay
4. Case Inlet
5. Port Madison
6. Port Susan
7. Nisqually Delta
8. Port Susan (1985)
9. Port Susan (1986, this
study)
Detection limits for this chemical or chemical group that exceeded 50 ug/kg have been
excluded for the purpose of reference area comparisons; this is consistent with treatment
of reference area data in Tetra Tech (1985a).
e An anomalously high phenol value of 1,800 ug/kg dry wt was found at one Carr Inlet
station (Tetra Tech 1985a). For the purpose of reference area comparison, this value has
been excluded. Data from Port Susan (this study) were excluded because laboratory contami-
nation of phenol was observed during analysis of these reference area samples.
109
-------
TABLE 18. (Continued)
Data from Port Susan (this study) were excluded because laboratory contamination of this
phthalate was observed during analysis of these reference area samples.
9 Higher detection limits for single component pesticides (U25) were reported for Main
Sediment Quality Survey samples from Carr Inlet in Tetra Tech (1985a). However, these
detection limits were based on GC/MS analysis, which is less sensitive than GC/ECD and was
considered undesirable for characterizing reference areas. GC/ECD analyses for Carr Inlet
samples in the Preliminary Survey (Tetra Tech 1985a) were consistent with the U10 value.
Tentatively identified organic compound. Detection limits were not assigned when
tentatively identified compounds were not found during mass spectral searches of reference
sample extracts.
References:
(Site 1) Tetra Tech (1985a); Mowrer et al. (1977)
(Site 2) Battelle (1986)
(Site 3) Battene (1986); Prahl and Carpenter (1979)
(Site 4) Mai ins et al. (1980); Mowrer et al. (1977)
(Site 5) Malins et al. (1980)
(Site 6) Malins et al. (1982)
(Site 7) Barrick and Prahl (1987); Mowrer et al. (1977)
(Site 8) PTI and Tetra Tech (1988); Stations PS-01 through PS-04
(Site 9) This study.
110
-------
TABLE 19. RANGE"IN EAR FOR ORGANIC COMPOUNDS OF CONCERN
IN SEDIMENTS OF EVERETT HARBOR AND PORT SUSANa
Chemical
LPAH
HPAH
Total PCBs
Resin Acids
abietic acid
dehydroabietic acid
12-chlorodehydroabietic acid
14-chlorodehydroabietic acid
dichlorodehydroabietic acid
isopimaric acid
neoabietic acid
sandaracopimaric acid
Phenols and Guaiacols
phenol
2-methyl phenol
4-methyl phenol
2, 4-di methyl phenol
2-chlorophenol
2,4-dichlorophenol
2,4,6-trichlorophenol
2 , 4 , 5-tri chl orophenol
2,3,4, 6-tetrachl orophenol
pentachl orophenol
3,4,5-trichloroguaiacol
4, 5,6-trichloroguaiacol
tetrachloroguaiacol
Range
0.88
0.46
0.17
0.87
0.32
0.41
0.31
0.87
0.57
0.53
0.12
0.33
0.86
0.23
1.5
0.29
0.29
0.29
0.1
0.67
0.06
0.33
0.67
0.67
690
290
1,600
650
1,300
73
23
4.7
73
93
95
88
170
7,500
76
46
47
43
12
40
14
37
16
17
EARb
Median0
6.4
4.1
0.83
15
22
5.2
4.0
4.0
6.2
2.7
6.4
6.8
7.1
57
7.3
5.7
2.9
2.9
1.7
1.3
0.6
1.3
1.5
1.3
Threshol dd
1.7
1.3
8.3
1.2
2.1
1.2
1.2
1.2
1.2
1.2
1.2
1.9
7.1
22
2.1
2.7
6.3
5.6
3.7.
1.0
1.5
1.0
1.0
1.0
Areas where Threshold
Exceeded by 10 Times6
EH.NG.OG, SR
Si.NG, SR
EW.NG
EW,SR
fW.OG.SR
si
EW
EW
EW
EW
ES,EW,NG
EW
EW.NG
EW
EW
--
--
--
EJi
--
EW
EW.SS
EW
Chlorinated Benzenes
1,2-dichlorobenzene
Phthalate Esters
butyl benzyl phthalate
bis(2-ethylhexylJphthalate
Pesticides
p,p'-OOT
Miscellaneous Extractables and
Tentatively Identified Compounds
benzyl alcohol
benzoic acid
dibenzofuran
2-methylnaphthal ene
1-methylpyrene
retene
cymene (unspecified isomer)
dibenzothiophene
1,2,4-trithiolane
di terpenoi d hydrocarbon
(base peak 255)
diterpenoid alcohol
(base peak 271)
hexadecanoic acid
2.0 27
0.59 4.2
0.60 55
0.1 2.3
1.0
0.07
0.82
0.54.
81
41
1,400
2,000
12
120
240
14
290
1,200
UT 4,300
Uf 66
2.9
0.6
2.2
0.1
2.0
0.7
4.8
5.5
0.3
0.84
1.3
0.7
2.7
2.3
9.3
5.1
11
1.5
1.5
1.0
2.0
3.0
3.8
6.0
1.0
4.8
1.0
1.0
1.0
1.0
1.6
1.0
EW
EW
EW
EW.NG
EW.NG
NG
EW
EW,NG,OG
QL
EW
EW,OG
ES,EW.,NG,SR,SS
EW,NG,OG
111
-------
TABLE 19. (Continued)
Chemical
Range
EARb
Medianc
Threshold*1 Exceeded by 10 Times6
Miscellaneous Extractables and
Tentatively ^Identified Compounds (Continued)
hexadecanoic acid methyl ester
hexadecenoic acid methyl ester
cholesterol
campesterol
alkanol (unidentified)
base peak 181, isomer #1
base peak 181, isomer #2
Nitrogen-Containing Compounds
N-m trosodi phenylami ne
Volatile Organic Compounds
9.9
9.2
22
55
110
600
330
2.0 14
1.0
0.9
1.9
3.4
14
7.0
3.5
2.4
1.1
1.1
1.6
1.0
1.0
1.0
1.0
2.4
EW
EW
All (EW)
EW,OG,SD,SR
EW.OG.SR
ES,EW,NG,
OG,SD,SS
acetone
total xylenes
1 38
1 13
1.7
1.7
1.0
1.0
EW
EW
a Only chemicals with concentrations exceeding Puget Sound reference area levels in at least one
sample are included in this table.
Dry weight concentration in study area sediments divided by the average concentration measured in
six Carr Inlet samples (Tetra Tech 1985a). For chemicals not measured in Tetra Tech (1985a), such as
resin acids, most TIO compounds, and chlorinated guaiacols, data from Port Susan were used. For TIO
compounds- that were undetected in Port Susan, no detection limits were available. In order to
generate EAR values for such compourTds, a reference concentration of 20 ug/kg OW was assigned as a
reasonable detection limit (i.e., twice the detection limit for many semivolatile organic compounds
in Port Susan).
c Medians are based on data after exclusion of detection limits >100 ug/kg DW for semivolatile
organic compounds and >25 ug/kg OW for pesticides.
The threshold EAR is defined as the ratio of the maximum reference sediment concentration in Puget
Sound divided by the average for sediments in Carr Inlet (Tetra Tech 1985a) or Port Susan (see
footnote b). Above the threshold EAR, the dry weight concentration of a study area sediment contami-
nant would exceed the maximum concentration- (or detection limit) reported for any Puget Sound
reference site listed in Table 18.
e The contaminant EAR in sediments from at least one station in each listed area exceeded the
threshold level by at least one order of magnitude. The factor of 10 is arbitrary, but is useful for
indicating the areas of greatest contamination. It was not used in problem area identification or
ranking. Sediments in the underlined areas had the highest observed concentrations.
Detection limi.ts are not reported for TIO compounds. Hence, the lower end of the range is unknown.
112
-------
TABLE 20. SUMMARY OF ORGANIC COMPOUNDS
WITH EAR >l,000a
Compound Station
Naphthalene EW-04, EW-07, EW-13, EW-14
2-Methylnaphthalene EW-04, EW-07, EW-13, EW-14
Acenaphthene EW-14
Fluorene EW-14
Dibenzofuran EW-14
Dehydroabietic acid EW-04, EW-13
4-Methylphenol EW-04, EW-07, EW-10, EW-13, EW-14
PCBs EW-04
a TIO compounds are not included in this table because of the
uncertainty of reference conditions for certain compounds.
113
-------
Polvcvclic Aromatic Hvdrocarbons.--To facilitate data analysis and to
maximize comparability with data analyses performed in other Puget Sound
studies, the 16 individual EPA priority pollutant PAH were treated as two
groups: LPAH and HPAH. This grouping was considered to be a reasonable
data reduction method because the concentrations of individual PAH within
each group tended to correlate well. Pearson correlation coefficients (r)
among the six LPAH (using dry weight concentrations) ranged from 0.62 to
>0.99 with most values exceeding 0.8 (Appendix C). Correlations of naph-
thalene with other LPAH were typically the least strong. Correlations among
HPAH were strong overall, with correlation coefficients ranging from 0.79 to
>0.995 with most values exceeding 0.9. Grouping of LPAH and HPAH is also
valuable for potential source correlations, as relatively high concentrations
of LPAH are typically characteristic of petroleum-derived materials whereas
relatively high concentrations of HPAH are more characteristic of combustion-
derived materials (e.g., Readman et al. 1982; Prahl and Carpenter 1983;
Tetra Tech 1985a).
Mean EAR for LPAH and HPAH were'higher in the East Waterway than in any
other study area, and LPAH were considerably more elevated than HPAH in the
East Waterway (Figure 16). The mean EAR for LPAH in the East Waterway was
roughly 310 whereas mean EAR in other study areas were less than 20. Within
the East Waterway, LPAH concentrations exceeding EAR of 500 were observed in
two areas along the east shore (Stations EW-04 and EW-07, 25,000 and
23,000 ug/kg DW; and Stations EW-13 and EW-14, 24,000 and 28,000 ug/kg DW,
respectively) (Figure 17). Concentrations were considerably lower at
stations on either side of these two maxima, but EAR for LPAH nonetheless
exceeded 100 at Stations EW-10 and EW-15 (Figure 17). PAH concentrations
were lower (EAR=59 for LPAH) at Station EW-11 near the west shore of the
East Waterway (note that PAH were not analyzed in Samples EW-02, EW-03,
EW-05, EW-06, EW-08, and EW-09 because of the availability of recent data;
Figure 17).
The PAH composition in East Waterway sediments was variable, but
certain trends were apparent. LPAH concentrations throughout the East
Waterway were comparable to or greater than HPAH concentrations (LPAH/HPAH
ratios ranged from 0.7 to 4.2 with a mean of 1.8; n=9) (Figure 17). Such
114
-------
UJ
O
z
UJ
rr
UJ
u.
in
cc
300-
200 -
O)
O
CO
O
h-
UJ
_l
UJ
100 -
THRESHOLD
^
PS
PS
NG
OG
EVV
SD
SR
SS
ES
LEGEND
HPAH
Port Susan
Nearshore Port Gardner
Offshore Port Gardner
East Waterway
Snohomish Delta
Snohomish River
Steamboat Slough
Ebey Slough
' THRESHOLD - equivalent to the
highest concentration in Puget
Sound reference areas.
r^-pn
NG
OG
EW
SD
SR
SS
ES
AREAS
Relerence: L41 (ig/kg DW (LPAH) and L79 (ig/kg DW (HPAH).
Figure 16. Mean EAR of LPAH and HPAH in sediments from all study areas.
-------
300 -
200 -
100
'^THRESHOLD
NA
NA
NA
EW-11 EW-09 EW-06 EW-03
01
U
z
Ul
CC
01
O.
01
Ul O)
>'3>
O Z
00 ^
< ^
2^
g
<
>
01
_J
01
300
200 -\
100-
LTHRESHOLD*
700 -
600
500-
400 -
300 -
200 -
100 -
THRESHOLD *ek
NA
NA
NA
SW-08 EW-05 EW-02
v\
EW-1S EW-14 EW-13 EW-12 EW-10 EW-07 EW-04 EW-01
STATIONS
LPAH
K\] HPAH
L - '
NA Not analyzed
*THRESHOLD - equivalent to
the highest concentration in
Puget Sound reference areas.
Reference: L41 ng/kg DW (LPAH) and L79 (ig/kg DW (HPAH).
Figure 17. EAR of LPAH and HPAH at individual stations in the
East Waterway.
116
-------
PAH compositions suggest a source other than combustion of organic material.
Naphthalene was the predominant PAH compound in all East Waterway samples
except Station EW-01, where fluoranthene and pyrene concentrations slightly
exceeded the naphthalene concentration. Naphthalene concentrations exceeded
EAR of 1,000 at Stations EW-07 (17,000 ug/kg DW), EW-13 (12,000 ug/kg DW),
EW-04 (10,000 ug/kg DW), and EW-14 (7,000 ug/kg.DW) and roughly equalled or
exceeded EAR of 100 at the remaining East Waterway stations that were
analyzed for PAH. Notably, PAH assemblages dominated by naphthalene were
also observed in sediments near a pulp mill in Commencement Bay (Tetra Tech
1985a).
Outside of the East Waterway, PAH concentrations were most elevated in
Areas OG and NG (Figure 16). PAH concentrations throughout Area OG were
consistent among stations (LPAH = 750+150 ug/kg DW; HPAH = 640+180 ug/kg DW,
n=7). All OG samples had very similar PAH compositions; naphthalene was the
predominant PAH compound in all samples (as was observed in East Waterway
sediments). The LPAH concentration at Station OG-01 (nearest the East
Waterway) was at least 5 times lower them concentrations at the nearest East
Waterway stations (e.g., Station EW-15) but was more than 4 times the
concentration at intervening Station NG-01. Thus, based on the limited data
available, a gradient indicating LPAH transport out of the East Waterway was
not apparent.
In Area NG, PAH concentrations were most elevated at Stations NG-09 and
NG-11, and to a lesser extent, Station NG-10. PAH contamination at Stations
NG-09 and NG-11 was similar in terms of composition and concentration
(3,500-4,100 ug/kg DW of LPAH and 8,700-9,000 ug/kg DW for HPAH). Concentra-
tions were roughly 3 times lower at Station NG-10 than at Stations NG-09 and
NG-11, and at least an order of magnitude lower at other NG stations. PAH
compositions in Area NG were unlike those in Areas EW and OG, and had higher
relative proportions of HPAH (e.g., fluoranthene, pyrene, and chrysene).
Polvchlorinated Biphenvls--PCBs were seldom detected in this study
(detection frequency = 7/54) and occurred at concentrations above 50 ug/kg
DW (the maximum reference area detection limit) in only three samples.
Sample EW-04 in the East Waterway had a highly elevated concentration of
117
-------
PCBs (9,600 ug/kg DW; EAR=1,600). PCBs were detected at a far lower con-
centration at adjacent Station EW-07 (87 ug/kg DW) and were undetected at
all other EW stations at detection limits of 50 ug/kg DW or less. In Area
NG, Sample NG-09 had a reported PCB concentration of 5,500 ug/kg DW
(EAR=920). PCBs were undetected at detection limits of 50 ug/kg DW or less
at nearby NG stations.
Resin AcidsThe resin acids analyzed for this study include abietic
acid, dehydroabietic acid (DHA), isopimaric acid, neoabietic acid, sandara-
copimaric acid, 12- and 14-chlorodehydroabietic acid, and dichlorodehydro-
abietic acid (see Figure 15 for structures). Unchlorinated resin acids (or
tricyclic diterpenoid acids) are among the predominant constituents of
higher plant resins and supportive tissue, particularly in conifers (e.g.,
Simoneit 1986; Thomas 1970; Gough 1964). Dehydroabietic acid, typically the
predominant resin acid found in the environment, is derived from abietic acid
and is relatively stable as a result of its aromatic ring structure (e.g.,
Simoneit 1986). Although unchfarinated resin acids are naturally-occurring
compounds, they are highly concentrated by pulping processes. The occurrence
of resin acids, particularly DHA and abietic acid, has been well-documented
in sulfite pulp effluents (e.g., Leuenberger et al. 1985; Leach and Thakore
1977) and in kraft effluents (e.g., Leach and Thakore 1973, 1977). Resin
acids (e.g., DHA) have also been reported at elevated concentrations in
sediments near pulp mill discharges (e.g., Brownlee et al. 1977). DHA is
very persistent in sediments (a "half-life" of over 20 yr was estimated in
210
Lake Superior sediments that were dated with Pb) (Brownlee et al. 1977).
Chlorine bleaching processes used by the pulp industry have been
demonstrated to result in the formation of chlorinated resin acids (i.e.,
chlorinated DHA derivatives) in bleached sulfite and kraft effluents
(Leuenberger et al. 1985; Claeys et al. 1980; Leach and Thakore 1975, 1977).
Chlorinated derivatives of DHA are by far the predominant chlorinated resin
acids reported in bleached pulp effluents, presumably because the stability
of DHA relative to other resin acids enables it to survive the strong
oxidizing conditions of chlorine bleaching. Chlorinated resin acids,
because of their unique origin, are powerful geochemical tracers of pulp
mills that use chlorine bleaching processes. Many other chlorinated
118
-------
compounds can be produced by pulp mills, including many acid and neutral
semi volatile organic compounds (e.g., Carl berg et al. 1986; Leuenberger et
al. 1985; Kringstad and Lindstrom 1984; Claeys et al. 1980) as. well as high-
relative-molecular-mass organic material (M^l.OOO) of poorly defined
structure. This latter material can constitute the majority of organically
bound chlorine in spent chlorination and alkali extraction liquors from the
bleaching of softwood kraft pulp (e.g., Kringstad and Lindstrom 1984), but
is not amenable to typical GC/MS analysis.
Concentrations of all resin acids were most elevated in the East
Waterway. Mean EAR values for DMA and abietic acid, which were the most
concentrated and among the most frequently detected resin acids, were 310
and 120, respectively, in the East Waterway (Figure 18). These mean EAR
were over 13 times higher than those of other study areas (note that samples
in Areas NG and ES were not analyzed for resin acids). Similarly, mean EAR
values of other resin acids in the East Waterway were typically at least 8
times higher than in other study areas. Outside of the East Waterway, Areas
SR and OG typically had the next highest concentrations of resin acids
(e.g., Figure 18).
Distributions of DMA and abietic acid in the East Waterway are presented
in Figure 19. DMA and abietic acid were similarly distributed; however,
DHA maximized at Station EW-04 (83,000 ug/kg DW; EAR=1,300), whereas abietic
acid maximized at Station EW-13 (98,000 ug/kg DW; EAR=650). As was observed
for virtually all chemicals in the study, the maximum concentrations in
the East Waterway occurred along the east shore. Along this shore, a
bimodal distribution was apparent, with maxima at Stations EW-04 and EW-13
(Figure 19). The interpretation of this bimodal distribution was impeded by
the lack of data at Stations EW-10 and EW-12 (resin acids were not analyzed
at these stations) and by variations in sediment TOC content along the east
shore (see Figure 10). Nonetheless, TOC-normalized DHA and abietic acid
concentrations also appeared to follow a bimodal distribution. Although
concentrations of DHA and abietic acid at Stations EW-04 and EW-13 were
predominant in the East Waterway, concentrations were highly elevated
throughout the East Waterway; for DHA, EAR values of >100 were reported at
9 of the 13 stations in the East Waterway (Figure 19).
119
-------
ro
o
-1
LU
Q 300-
Z
UJ
DC
UJ
UJ
DC ^
UJ TO 20°
> '5
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ffl *
** £*
z """
O 100 -
^^ 1 Uv
1-
UJ
LU
UJ
THRESHOLD**-
U NA r^-j\S
I 1 1
PS NG OG
v/
(^
/
X
X
/ ,
/,
' /
//
A
\N
A
Vs
A
X
X
\\
A
o-
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PS
LEGEND
ABIETIC ACID
DEHYDROABIETIC ACID
Port Susan
N G Nearshore Port Gardner
O G Offshore Port Gardner
E W East Waterway
SD
SR
SS
ES
U
NA
Snohomish Delta
Snohomish River
Steamboat Slough
Ebey Slough
Undetected at detection
limit shown
Not analyzed
* THRESHOLD - equivalent to the
highest concentration in Puget
Pru
pr "a OUL
U ,_^\\ _^^ NA
1 I I
EW SD SR SS ES
nd reference areas.
AREAS
Relerence: UI50 ng/Kg DW (abielic acid) and L63 fig/kg DW (dehydroabielic acid).
Figure 18. Mean EAR of abietic
East Waterway.
acid and dehydroabietic acid at individual stations in the
-------
600
400 -
.200 -
L THRESHOLD*
k\
U
F/K\
EW-11 EW-09 EW-06 EW-03
UJ
o
z
cc
UJ
U.
UJ 0>
o I
CO ^
zS
O
UJ
UJ
SOO-i
i
400 -j
200-
^THRESHOLD
1400 -,
1200-
1000-
800-I
600-
400-
200-
THRESHOLD
X
EW-08 EW-05 EW-02
NA NA
/
EW-1S EW-14 EW-13 EW-12 EW-10 EW-07 EW-04 EW-01
STATIONS
THRESHOLD - equivalent to
the highest concentration in
Puget Sound reference areas.
{/A Abietic Acid
^\j Dehydroabietic Acid
U Undetected at detection limit shown
NA Not analyzed
Reference: U150 (ig/kg DW (abiotic acid) and L63 ng/kg OW (dehydroabietic acid).
Figure 19. EAR of abietic acid and dehydroabietic acid at individual
stations in the East Waterway.
121
-------
Distributions of other unchlorinated resin acids in the East Waterway
were similar to those of DMA and abietic acid, but several discrepancies are
noteworthy. Sandaracopimaric acid occurred at high concentrations at
Stations EW-04 and EW-13, but was most concentrated at Station EW-01
(14,000 ug/kg DW;. EAR=95) (Figure 20). Strong gradients were apparent for
sandaracopimaric acid along the east shore of the East Waterway (Figure 20).
However, it should be noted that sandaracopimaric acid concentrations in
duplicate analyses for Station EW-07 were not in close agreement (see
Sediment Chemistry, Quality Assurance/Quality Control Results in Methods
section). Isopimaric acid covaried with abietic acid in the East Waterway
(r=0.92, n=18, P<0.05; study-wide), with a maximum concentration at Station
EW-13 (11,000 ug/kg DW; EAR=73). Neoabietic acid also maximized at Station
EW-13 (14,000 ug/kg DW; EAR=93), although this concentration was over 18
times that of any other station in the East Waterway. In addition, the
detection frequency of neoabietic acid was low in the East Waterway relative
to those of other unchlorinated resin acids (46 percent for neoabietic acid
as compared to over 90 percent for other unchlorinated resin acids).
Like DMA, -12- and 14-chlorodehydroabietic acids had maximum concen-
trations at Station EW-04 (12-chlorodehydroabietic acid = 11,000 ug/kg DW,
EAR=73) (Figure 21). However, in contrast to the bimodal distribution
observed for DHA and abietic acid in the East Waterway, monochlorodehydro-
abietic acids had maxima toward the head of the waterway without a comparably
high concentration at Station EW-13. Dichlorodehydroabietic acid (not shown
in Figure 21) also maximized at Station EW-04 (710 ug/kg DW; EAR=4.7) but
had comparable concentrations at Stations EW-07 and EW-13 (EAR=4-5).
Dichlorodehydroabietic acid was detected at lower concentrations at two
other stations in the East Waterway (Stations EW-03 and EW-05) and was not
detected in any other study areas.
Resin acids were detected in Area OG, but at far lower concentrations
than were typically observed in the East Waterway. Concentrations of DHA
and abietic acid were the most elevated among the resin acids detected in
Area OG. Maximum concentrations of these resin acids occurred at Station
OG-03 (DHA=1,500 ug/kg DW; EAR=24; abietic acid = 1,700 ug/kg DW; EAR=11),
although concentrations were typically very consistent for all OG samples
122
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40-
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10-
0
.THRESHOLD'
100
90-
80-
70-
60-j
50-
40-
30-
20-
10-
THRESHOLD1
EW-11 EW-09 EW-06 EW-03
EW-08 EW-05 EW-02
NA
NA
EW-15 EW-14 EW-13 EW-12 EW-10 EW-07 EW-04 EW-01
STATIONS
U Undetected at detection limit shown
NA Not analyzed
*THRESHOLD - equivalent to
the highest concentration in
Pugel Sound reference areas.
Reference: U150 ng/kg DW.
Figure 20. EAR of sandaracopimaric acid at individual stations in
the East Waterway.
123
-------
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L« THRESHOLD*
30-
20-
10 -
^THRESHOLD*
80-1
70-
60-
50-
40-
30-
20 -
10 -
THRESHOLD
EW-11 EW-09 EW-06 EW-03
/
EW-08 EW-05 EW-02
NA
NA
_Z^
EW-15 EW-14 EW-13 EW-12 EW-10 EW-07 EW-04 EW-01
U
NA
STATIONS
12-Chlorodehydroabietic Acid
14-Chlorodehydroabietic Acid
Undetected at detection limit shown
Not analyzed
THRESHOLD - equivalent to
the highest concentration in
Puget Sound reference areas.
Reference: U150 |ig/kg DW (12- and 14-chlofodehydroabietic acid).
Figure 21. EAR of 12- and 14-chlorodehydroabietic acids at
individual stations in the East Waterway.
124
-------
analyzed (e.g., agreement within a factor of 2-3 among most stations and for
most resin acids). Concentrations at Stations OG-02 and EW-15, the most
closely spaced stations from Areas OG and EW that were tested for resin
acids, were very similar for most resin acids (typically well within a
factor of 2). However, it was not possible to discern whether resin acid
contamination in Area OG derived from the East Waterway or had dispersed
from the area near Station OG-03. Notably, chlorinated resin acids (12- and
14-chlorodehydroabietic acids) were detected in Area OG but at relatively
low concentrations (e.g., 12-chlorodehydroabietic acid was detected at all
5 OG stations tested at concentrations from 78 to 270 ug/kg DW, with the
maximum concentration at Station OG-06).
In the Snohomish River (Area SR), resin acid contamination was
most prevalent at Station SR-05 (DHA=3,500 ug/kg DW, EAR=56; abietic
acid = 2,300 ug/kg DW, EAR=15). Concentrations at adjacent Station SR-04
were roughly 5 times lower. The only detected chlorinated resin acid in the
Snohomish River occurred at Station SR-04 (12-chlorodehydroabietic acid,
61-ug/kg DW). In Steamboat Slough, resin acids were most frequently detected
at Station SS 02, although several resin acids were detected at less than.
250 ug/kg DW at Station SS-03. The highest resin acid concentration in this
area was for DMA (730 ug/kg DW at Station SS-02, EAR=12). No chlorinated
resin acids were detected in Steamboat Slough.
Phenol and Alkvl-Substituted PhenolsOf the compounds in this group
(phenol, 2- and 4-methylphenol, and 2,4-dimethylphenol), phenol and
4-methyl phenol were both frequently detected, but 4-methyl phenol
concentrations were by far the most elevated. 4-Methylphenol was detected
in over 90 percent of the samples in which it was analyzed and occurred at
the most elevated concentrations of any chemical measured in this study
(maximum EAR=7,500). Roughly 30 percent of 4-methylphenol concentrations
exceeded an EAR of 100 and roughly 9 percent exceeded an EAR of 1,000 (all
of the latter group were from the East Waterway). Of all the study areas,
the highest mean 4-methylphenol concentration was observed in the East
Waterway (mean = 25,000 ug/kg DW; EAR=1,900) (Figure 22). However, the mean
EAR in Area NG exceeded 100 (EAR=120) and the mean EAR in Area OG was 71.
125
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en
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1600
1400
1200
1000
800-
600-
400
200-
THR£SHOLD*0fc
D)
LEGEND
P S Port Susan
N G Nearshore Port Gardner
O G Offshore Port Gardner
EW East Waterway
S D Snohomish Delta
S R Snohomish River
S S Steamboat Slough
E S Ebey Slough
'THRESHOLD - equivalent to the
highest concentration in Puget
Sound reference areas.
PS
NG OG EW SD SR SS ES
AREAS
Reference; LI3 ng/kg DW.
Figure 22. Mean EAR of 4-methylphenol in sediments from all study areas.
-------
Within the East Waterway, the highest 4-methylphenol concentration was
observed at Station EW-07 (98,000 ug/kg DW; EAR=7,500) (Figure 23). Four
other stations along the east shore had EAR >1,000, with concentrations
ranging from 15,000 to 35,000 ug/kg DW (Stations EW-04, EW-10, EW-13, and
EW-14).. Concentrations decreased along the east shore moving in either
direction from Station EW-07. Contamination in the East Waterway toward the
west shore was not well characterized because only Station EW-11 in that
area was analyzed for A/B/N compounds. The 4-methylphenol concentration at
Station EW-11 was highly elevated (EAR=550).
Area NG also had elevated 4-methylphenol concentrations. However, the
highest concentrations were observed at Station NG-05 (9,700 ug/kg DW;
EAR=730) and nearby stations, not at stations near the mouth of the East
Waterway (e.g., Stations NG-01 and NG-12; U20 to 500 ug/kg DW). Hence, 4-
methylphenol contamination in Area NG did not appear to derive from the East
Waterway. EAR values >100 were observed at Stations NG-04, NG-09, NG-10,
NG-11, and NG-14 (all between 1,600 and 2,400 ug/kg DW). Concentrations
were somewhat patchy in this are/i, but did not exceed l.,000 ug/kg DW at any
other NG stations. '
4-Methylphenol concentrations were generally consistent among stations
in Area OG (EAR from 68 to 97 at Stations OG-01 to OG-05). Distributions of
4-methylphenol between the East Waterway mouth and OG stations nearest the
mouth did not suggest that 4-methylphenol contamination in Area OG derived
from the more contaminated East Waterway. The 4-methylphenol concentration
at Station OG-01 (nearest the East Waterway) was at least 5 times lower than
concentrations at the nearest East Waterway stations (e.g., Station EW-15)
but was more than double the concentration at intervening Station NG-01. In
other areas, high 4-methylphenol concentrations (EAR >100) occurred at
Station SR-05 (2,000 ug/kg DW) and Station ES-03 (1,400 ug/kg DW).
Phenol, like 4-methylphenol, was detected frequently (detection
frequency >90 percent) but at far lower concentrations than 4-methylphenol.
The mean EAR for phenol in the East Waterway (40) was greater than that of
any other study area (Figure 24); Areas NG, OG, and ES all had mean EARs
between 11 and 17. Laboratory contamination of phenol was observed for two
127
-------
3000-
2000
.1000 -
^ THRESHOLD
NA
NA
NA
EW-11 EW-09 EW-06 EW-03
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THRESHOLD
8000-;
7000-
6000-
5000-
4000-
3000-
2000-
1000-
THRESHOLD1
NA
NA
NA
EW-08 EW-05 EW-02
EW-15 EW-14 EW-13 EW-12 EW-10 EW-07 EW-04 EW-01
STATIONS
NA Not analyzed
*THRESHOLD - equivalent to
the highest concentration in
Puget Sound reference areas.
Reference: L13 ng/Kg DW.
Figure 23. EAR of 4-methylphenol at individual stations in the
East Waterway.
128
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7HRESHOLD **
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T
OG
LEGEND
EW
p s Port Susan
N G Nearshore Port Gardner
O G Offshore Port Gardner
E W East Waterway
SO Snohomish Delta
S R Snohomish River
S S Steamboat Slough
E S Ebey Slough
* THRESHOLD - equivalent to the
highest concentration in Puget
Sound reference areas.
ES
AREAS
Reference: L33 ng/kg DW.
Figure 24. Mean EAR of phenol in sediments from all study areas.
-------
blanks analyzed during this study (see Chemistry, Quality Assurance/Quality
Control Results in Methods section), although the level of contamination was
relatively minor. For the samples associated with the contaminated labora-
tory blank, laboratory contamination accounted for roughly 20 to 30 ug/kg
DW. All of these samples were blank-corrected.
Within the East Waterway, the maximum phenol concentration was observed
at Station EW-10 (2,900 ug/kg DW; EAR=88) (Figure 25). No clear concentra-
tion gradient was apparent along the east shore of the waterway on a dry
weight or TOC-normalized basis (Figure 25). The only sample analyzed near
the west shore of the waterway, Station EW-11, had a concentration comparable
to most stations on the east shore (1,200 ug/kg DW; EAR=36). Only one EW
sample required blank correction (Station EW-01; 1,600 ug/kg DW).
Phenol concentrations at certain stations in Area NG were comparable to
those in the East Waterway. The maximum concentration in Area NG was
observed at Station NG-09 (2,100 ug/kg DW, EAR=64). Overall, phenol concen-
trations were relatively patchy (Figure 26) and did not suggest dispersion
from a single source. Blank correction- was performed on concentrations for
Stations NG-06 and. NG-12 to NG-15. Phenol concentrations in Area OG were
consistent throughout the area (380+73 ug/kg DW; n=7, all values blank-
corrected). In Ebey Slough, phenol was detected at Station ES-03 at
1,200 ug/kg DW (EAR=36, blank-corrected). The other two ES stations were
blank-corrected down to detection limits (25 ug/kg DW).
2-Methylphenol and 2,4-dimethylphenol were seldom detected in this
study (the former compound was detected three times and the latter, twice)
(see Table 17). Both phenols occurred at Stations EW-04 and EW-07, with
maximum concentrations at the former station. 2-Methylphenol was reported at
1,200 ug/kg DW (EAR=170) at Station EW-04 and at 330 ug/kg DW (EAR=47) at
adjacent Station EW-07. Detection limits were somewhat high (200 ug/kg DW)
at nearby Stations EW-10 and EW-12, but did not greatly interfere with data
interpretation. 2,4-Dimethylphenol was detected at 520 ug/kg DW (EAR=76) at
Station EW-04 and occurred at 100 ug/kg DW (EAR=15) at Station EW-07.
2,4-Dimethylphenol was undetected throughout the rest of the East Waterway at
detection limits of 20-50 ug/kg DW.
130
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40 -
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30 -
20 -
C" 10 -
< THRESHOLD'
90 -
80 -
70 -
60 -
50
40 -
30 -
20 -
10 -
THRESHOLD* »
NA
NA
NA
EW-11 EW-09 EW-06 EW-03
NA
NA
NA
EW-08 EW-05 EW-02
EW-15 EW-14 EW-13 EW-12 EW-10 EW-07 EW-04 EW-01
STATIONS
NA Not analyzed
THRESHOLD - equivalent to
the highest concentration in
Puget Sound reference areas.
Reference: L33 ng/kg DW.
Figure 25. EAR of phenol at individual stations in the East Waterway.
131
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90 -
80 -
70 -
60-
50-
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THRESHOLDV
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LEGEND
P S Port Susan
N G Nearshore Port Gardner
O G Offshore Port Gardner
E W East Waterway
S D Snohomish Delta
S R Snohomish River
S S Steamboat Slough
E S Ebey Slough
B Blank-corrected down to
detection limit shown
* THRESHOLD - equivalent to the
highest concentration in Puget
Sound reference areas.
NG-02
NG-01
NG-10
NG-15
NG-07 NG-05
NG-14
NG-13
NG-12
STATIONS
Reference: L33 jig/kg DW.
Figure 26. EAR of phenol at individual stations in Area NG.
-------
Chlorinated Phenols and GuaiacolsCertain chlorinated phenols have
been commercially produced for various purposes (e.g., pentachlorophenol, or
PCP, has been used as a biocide); however, chlorinated phenols and chlori-
nated guaiacols are well-documented by-products of pulp bleaching processes
(e.g., Carlberg et al. 1986; Leuenberger et al. 1985, Kringstad and Lindstrom
1984, Claeys et al. 1980, Leach and Thakore 1975, 1977). Lignin, a primary
component of wood, is a natural polymer formed by the mixture of various
4-hydroxyarylpropenyl alcohols (e.g., Kringstad and Lindstrom 1984 and
references therein). The chlorine bleaching process, through various
substitution and dealkylation mechanisms, can depolymerize lignin and
generate various chlorinated phenols and guaiacols, among other phenolic
compounds (e.g., catechols) (Kringstad and Lindstrom 1984, Leuenberger et
al. 1985, and Claeys et al. 1980). Chlorinated guaiacols, like chlorinated
resin acids, are excellent geochemical tracers of pulp mills because of
their unique origin.
Chlorinated phenols and guaiacols (see structures in Figure 15) were
detected mqst often in the East Waterw§y and occurred at the highest
concentrations in that area.- For the 'nine chlorinated phenols/guaiacols
analyzed in this study (i.e., 2-chlorophenol, 2,4-dichlorophenol, 2,4,5-
and 2,4,6-trichlorophenol, 2,3,4,6-tetrachlorophenol, PCP, 3,4,5- and
4,5,6-trichloroguaiacol, and tetrachloroguaiacol), maximum EAR values within
the East Waterway ranged from 12 to 47 (n=9) with a mean of 30 (n=9);
outside of the East Waterway, maximum EAR for these compounds ranged from
0.5 to 14 (n=9), with a mean of 3.9 (n=9).
Chlorinated phenols/guaiacols tended to have similar distribution
patterns within the East Waterway, but several important distinctions were
apparent. Di-, tri-, and tetrachlorophenol distributions corresponded well
in the East Waterway (and in the overall study, r>0.8 for all correlations
between 2,4-dichlorophenol, 2,4,5- and 2,4,6-trichlorophenol, and 2,3,4,6-
tetrachlorophenol). Distributions of 2,4-dichlorophenol and 2,4,6-trichloro-
phenol (Figure 27) are representative of this group of compounds. As is
apparent in Figure 27, correlations between 2,4-dichlorophenol and 2,4,6-
trichlorophenol were particularly strong (r>0.99, n=19, PO.05). For di-
through tetrachlorophenols, maximum concentrations were observed at the head
133
-------
30-
20 -
10 -
THRESHOLD**"
FTKi
EW-11 EW-09 EW-06 EW-03
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THRESHOLD **J
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30-
20-1
THRESHOLD
U U
^C±.
EW-15 EW-14 EW-13 EW-12 EW-10 EW-07 EW-04 EW-01
STATIONS
2,4-Dichlorophenol
2,4,6-Trichlorophenol
Undetected at detection limit shown
*THRESHOLD - equivalent to
the highest concentration in
Pugel Sound reference areas.
Reference: U6.8 (ig/kg DW (2,4-dichloro- and 2,4,6-lrichlorophenol).
Figure 27. EAR of 2,4-dichlorophenol and 2,4,6-trichlorophenol
at individual stations in the East Waterway.
134
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of the East Waterway (i.e., at Stations EW-01 and EW-02; see Figure 27 and
Table 17). Concentrations of these compounds decreased sharply toward the
mouth of the waterway (e.g., Figure 27}, although the decrease in concentra-
tion from Station EW-01 to EW-04 was not as great for 2,4,5-trichlorophenol
and 2,3,4,6-tetrachlorophenol as it was for the compounds shown in Figure 27.
High detection limits were reported for chlorinated phenols at Station EW-12
(Figure 27). Full-scan analyses, which were less sensitive than the
dedicated chlorinated phenol analyses, were performed at Stations EW-12 and
EW-10.
Chlorinated guaiacol distributions in the East Waterway were similar to
those of di- through tetrachlorophenols in that strong concentration maxima
occurred at Station EW-01 for all guaiacols analyzed (e.g., Figure 28).
However, unlike the chlorinated phenols discussed above, all chlorinated
guaiacols were undetected at Station EW-02. 3,4,5-Trichloroguaiacol was the
most commonly detected of the chloroguaiacols (see Table 17).
Distributions of PCP and 2-chlorophenol in the. East Waterway were
somewhat different than those of the other chlorinated phenols and chlori-
nated guaiacols; both PCP and 2-chlorophenol had strong concentration maxima
at Station EW-04 (see Table 17), whereas concentrations at Station EW-01 were
considerably lower (Figure 29). However, as was observed for the other
chlorinated phenols, concentrations decreased sharply toward the mouth of
the waterway.
Outside of the East Waterway, chlorinated phenols and guaiacols were
seldom detected at concentrations exceeding the maximum detection limits
reported in Puget Sound reference areas (see Table 18) (in fact, most detec-
ted values were <10 ug/kg DW). Among the chlorinated phenols, 2-chlorophenol
occurred at the highest concentration outside of the East Waterway (36 ug/kg
DW at Station SD-02; EAR=10). Dichloro-, trichloro-, and pentachlorophenols
were detected at most OG stations, but typically at <5 ug/kg DW. Similar
chlorinated phenol results were observed at Station SS-03 in Steamboat
Slough. Chlorinated guaiacols were detected a total of seven times outside
of the East Waterway (at Stations OG-07, SD-02, SS-02, SS-03, SS-04, and
SS-06). The highest concentration occurred at Station SS-04 [43 ug/kg DW for
135
-------
20 -
15
10 -
5 ~
THRESHOLD* »(
0
EW-11 EW-09 EW-06 EW-03
O
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tr
UJ
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THRESHOLD*-
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35 -
30-
25-
20-
15-
10-
THRESHOLD
u u
u u
NA NA
u u
EW-15 EW-14 EW-13 EW-12 EW-10 EW-07 EW-04 EW-01
STATIONS
3,4,5-Trichloroguaiacol
Tetrachloroguaiacol
U Undetected at detection limit shown
NA Not analyzed
* THRESHOLD - equivalent to
the highest concentration in
Puget Sound reference areas.
Reference: U3 ng/kg DW (3,4,5-lrichloro- and tetrachloroguaiacol).
Figure 28. EAR of 3,4,5-trichloroguaiacol and tetrachloroguaiacol
at individual stations in the East Waterway.
136
-------
01
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THRESHOLD
Y,
EW-11 EW-09 EW-06 EW-03
**.
n -
II
u
EW-08 EW-05 EW-02
EW-15 EW-14 EW-13 EW-12 EW-10 EW-07 EW-04 EW-01
STATIONS
U Undetected at detection
limit shown
THRESHOLD - equivalent to
the highest concentration in
Puget Sound reference areas.
Reference: L33 (ig/kg DW.
Figure 29. EAR of pentachlorophenol at individual stations in the
East Waterway.
137
-------
4,5,6-trichloroguaiacol (EAR=14)]. All other chlorinated guaiacol concentra-
tions outside of the East Waterway were near detection limits (from 1 to 9
ug/kg DW).
Chlorinated Benzenes--Qn1v one reported chlorinated benzene concentra-
tion exceeded reference conditions in this study: 1,2-dichlorobenzene was
detected at 96 ug/kg DW at Station EW-04 in the East Waterway. Detection
limits for 1,2-dichlorobenzene were relatively high in the East Waterway
(e.g., 100 ug/kg DW at adjacent Station EW-07) and impeded data analysis
somewhat in this area. However, the detection limit at nearby Station EW-01
(10 ug/kg DW) indicated that contamination from Station EW-04 was not
prevalent at the head of the waterway.
Phthalate EstersTwo phthalate esters were of concern in this study
[butyl benzyl phthalate and bis(2-ethylhexyl)phthalate]. Bis(2-ethyl-
hexyl)phthalate was detected frequently (detection frequency = 39/54) but
was also observed as a laboratory contaminant in most method blanks.
However, concentrations in blanks were relatively low (e.g., equivalent to
roughly 50 ug/kg DW). The highest concentrations were observed in the East
Waterway (Station EW-14, 930 ug/kg DW, EAR=55). Concentrations at other
stations along the east shore of the East Waterway ranged from 110 ug/kg DW
(Station EW-15) to 650 ug/kg DW (Station EW-04); the samples with the
highest concentrations in the East Waterway were not associated with
contaminated method blanks. All other stations in the study had bis(2-
ethylhexyl)phthalate concentrations less than 5 times the maximum observed
blank concentration (i.e., roughly 250 ug/kg DW).
Butyl benzyl phthalate was detected infrequently (detection frequency =
6/54) and occurred above Puget Sound reference conditions at only three
stations: Station EW-01 in the East Waterway (70 ug/kg DW), Station SR-05
(44 ug/kg DW), and Station NG-14 (36 ug/kg DW). Detection limits for butyl
benzyl phthalate were 20 ug/kg DW or less throughout the study.
PesticidesPesticides were seldom detected in the study, although
detection limits in certain samples were relatively high as a result of
sample dilution during chemical analysis. Samples with relatively high
138
-------
detection limits included Stations EW-01, EW-04, EW-14, EW-15, and NG-09,
which typically had detection limits of 50 to-200 ug/kg DW for individual
pesticides. Two of these samples, EW-04 and NG-09, had high PCB concentra-
tions that were likely responsible for GC/ECD interferences. Data analysis
for pesticides was not greatly impeded by high detection limits at these
five stations because lower detection limits were reported at other stations
in these areas. The sole pesticide detection above reference conditions was
p,p'-ODT at Station SD-03 (23 ug/kg DW; EAR=2.3). Detection limits for
p,p'-DDT at nearby stations ranged from 1 to 10 ug/kg DW.
N-Nitrosodiphenvlamine--N-nitrosodipheny1amine was detected seven times
over a relatively narrow concentration range. The highest concentration
(57 ug/kg DW) was observed at Station EW-01. N-nitrosodiphenylamine was
detected at Stations OG-03 through OG-07 at concentrations of 15-38 ug/kg
DW. This compound was also detected at 48 ug/kg DW at Station SS-01 and at
28 ug/kg DW at Station SS-06. Other samples with reported concentrations
between 10 and 30 ug/kg DW included Stations ES-02, ES-03, NG-06, and SD-01.
Detection.limits for N-nitrosodiphenylamine were 10 ug/kg DW.
Miscellaneous Extractables and TIP CompoundsCompounds assigned to
this class include benzyl alcohol, benzoic acid, dibenzofuran, 2-methylnaph-
thalene, 1-methylpyrene, retene, a cymene isomer, dibenzothiophene, 1,2,4-
trithiolane, a diterpenoid hydrocarbon (possibly dehydroabietane), a
diterpenoid alcohol (possibly totarol), hexadecanoic acid, hexadecanoic acid
methyl ester, hexadecenoic acid methyl ester, cholesterol, campesterol, an
unidentified alkanol, and two isomers with mass spectral base peaks at
m/z 181. With the exception of the first four compounds, the chemicals
listed above are TIO compounds. TIO compounds are tentatively identified
organic compounds found during mass spectral searches of sample extracts;
they represent some of the most prevalent peaks in sample chromatograms that
were not among the original target compounds. Some, possibly most, of the
TIO compounds found in this study are related to target compounds in terms of
chemical structure, probable sources, or both. Relationships between target
compounds and TIO compounds will be addressed in this section, when appli-
cable.
139
-------
Several of the miscellaneous extractable organic compounds are closely
related to PAH (i.e., 2-methylnaphthalene, 1-methylpyrene, dibenzofuran, and
dibenzothiophene). Because these compounds correlated relatively well with
PAH, their distribution will not be described here. Correlation coefficients
between these compounds and related PAH are as follows: 2-methylnaphthalene
vs. naphthalene (r=0.96, n=35, P<0.05); 1-methylpyrene vs. pyrene (r=0.77,
n=25, PO.05); dibenzofuran vs. HPAH (r=0.95, n=44, P<0.05); and dibenzo-
thiophene vs. HPAH (r=0.96, n=19, P<0.05).
Benzoic acid was detected in roughly half of the samples in which it
was analyzed and occurred at the highest concentrations in Areas EW and NG
(Figure 30). The maximum benzoic acid concentration was reported at Station
EW-14 in the East Waterway (5,900 ug/kg DW, EAR=41) but benzoic acid was
undetected at nearby stations at detection limits of 200 ug/kg DW or less.
Benzoic acid was otherwise undetected throughout the East Waterway, although
detection limits were relatively high in most samples (up to 800 ug/kg DW).
In Area NG, benzoic acid concentrations were elevated at Stations NG-05,
NG-07, and NG-08 (1,300-2,100 ug/kg DW), whereas concentrations were.
typically at least 5 times lower at other NG stations. Benzoic acid concen-
trations also exceeded Puget Sound reference conditions at Stations SR-05
(1,000 ug/kg DW), SD-03 (770 ug/kg DW), and ES-03 (760 ug/kg DW; blank-
corrected). Of the samples discussed above, only the latter sample was
associated with the method blank contaminated at roughly 160 ug/kg DW (see
Sediment Chemistry, Quality Assurance/Quality Control Results in Methods
section).
Benzyl alcohol was detected above Puget Sound reference conditions in
four samples. The highest concentration was observed at Station EW-04 in
the East Waterway (810 ug/kg DW; EAR=81). Detection limits at nearby
stations ranged from 20 ug/kg DW to 100 ug/kg DW. Near the mouth of the
East Waterway, benzyl alcohol was detected at 58 ug/kg DW (Station EW-11)
and at 99 ug/kg DW (Station SD-03). Benzyl alcohol was detected at 42 ug/kg
DW at Station SR-05.
Most (14/15) TIO compounds had maximum concentrations in the East Water-
way, and 11/15 had maximum concentrations at Station EW-04 (see Table 17).
140
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15
UJ
O
z
UJ
cc
UJ
u.
UJ
DC-
UJ TO
§1
ffl *
z
o
10
5 -
THRESHOLD
UJ
_J
UJ
i
PS
\ZZA
LEGEND
P S Port Susan
N G Nearshore Port Gardner
O G Offshore Port Gardner
EW East Waterway
S D Snohomish Delta
SR Snohomish River
S S Steamboat Slough
E S Ebey Slough
* THRESHOLD - equivalent to the
highest concentration in Puget
Sound reference areas.
NG
OG
EW SO SR SS
ES
AREAS
Reference: L150 ng/kg DW.
Figure 30. Mean EAR of benzoic acid in sediments from all study areas.
-------
However, some TIO compounds were outstanding in their extreme elevations in
the East Waterway relative to other areas. The mean EAR of the following
four TIO compounds were over 15 times higher in the East Waterway than in
any other study area: retene; a diterpenoid hydrocarbon (possibly dehyro-
abietane); a diterpenoid alcohol (possibly totarol); and 1,2,4-trithiolane
(a sulfur-containing heterocycle). The mean EAR of retene in the East
Waterway (39) was 23 times the next highest mean EAR (in Area OG). Within
the East Waterway, retene distributions followed a bimodal pattern with
concentration maxima at Stations EW-04 and EW-13 (3,100 and 2,900 ug/kg DW,
respectively; EAR>100). This distribution pattern was similar to that
observed for DMA (Figure 19). The correspondence between DMA and retene
(r=0.99, n=20, P<0.05) is not unexpected, as the diagenetic transformation of
abietic-type resin acids to retene has been proposed by several researchers
(e.g., Simoneit 1986 and references therein; Wakeham et al. 1980; Barnes and
Barnes 1983). The structural relationship between retene and OHA is
apparent from Figure 15. Retene has previously been detected in marine
sediments near pulft mill discharges (Yamaoka 1979; Tetra Tech 1985 a.).
Related sources of retene exist (e.g., brown coal, which can contain fossil
resins; Thomas 1970), but are improbable in the East Waterway.
The diterpenoid hydrocarbon TIO compound was highly elevated in the
East Waterway (mean EAR=160 in the East Waterway vs. a mean EAR of 5 in Area
OG, the next most contaminated area). Within the East Waterway, this-
compound was predominant at Station EW-04 (23,000 ug/kg DW). The concentra-
tion at Station EW-04 was over 10 times the concentration at any other EW
station and at least 100 times the concentrations at stations in other study
areas. The mass spectrum of this hydrocarbon was similar to that of
dehydroabietane (e.g., see spectrum in Kitadani et al. 1970), although other
structures are possible. The structural relationship between dehydro-
abietane and DMA is apparent from Figure 15. In addition, dehydroabietane
has been reported in sulfite pulp effluent (Leuenberger et al. 1985) and has
been found in sediments near pulp mill discharges (Yamaoka 1979).
The concentration of the diterpenoid alcohol TIO compound also maximized
in the East Waterway, but its distribution was different than that of most
TIO compounds. The maximum concentration occurred at Station EW-11
142
-------
(8,600 ug/kg DW), with lower concentrations reported along the east shore of
the waterway (e.g., 1,100 to 1,300 ug/kg DW at Stations EW-01, EW-10, and
EW-14). Diterpenoid alcohols are structurally related to resin acids (see
Figure 15) and have been reported in pulp mill effluents (e.g., Leuenberger
et al. 1985; Leach and Thakore 1977). However, the distribution of the
diterpenoid alcohol TIO in the East Waterway did not closely correspond to
resin acid distributions. Also, the compound was detected at a relatively
high concentration away from pulp mill discharges (Station NG-11,
1,100 ug/kg DW). The mass spectrum was similar to that of totarol (a
podocarpa-8,ll,13-triene derivative).
1,2,4-Trithiolane, a sulfur-containing heterocycle (02^3), was most
concentrated at Station EW-04 (5,800 ug/kg DW), with lower concentrations at
other stations along the east shore of the East Waterway (1,400 to 1,600
ug/kg DW at Stations EW-10 and EW-01). Outside of the East Waterway,
detected concentrations were less than 200 ug/kg DW, and typically less than
100 ug/kg DW.
Concentrations of a cymene isomer were highest in the East Waterway at
Stations EW-04 (2,900 ug/kg DW) and EW-13 (1,000 ug/kg DW), and were thus
consistent with certain resin acid distributions. Concentrations outside
the East Waterway were highest in Area OG and were relatively consistent in
that area (240 + 77 ug/kg DW, n=7). Para-cymene has been reported in
sulfite pulp mill effluents and is thought to derive from alpha-pinene, a
cyclic monoterpene (Leuenberger et al. 1985), although other sources also
exist. The isomer (i.e., ortho-, meta-, or para-) observed in this study
could not be determined in the absence of standards.
Hexadecanoic acid occurred at the highest concentration in the East
Waterway at Stations EW-10 (2,300 ug/kg DW), EW-07 (1,400 ug/kg DW), and
EW-11 (1,000 ug/kg DW). Hexadecanoic acid methyl ester and hexadecenoic acid
methyl ester both occurred at the highest concentration at Station EW-04,
but the concentrations did not exceed an EAR of 10. These fatty acid methyl
esters were widespread and occurred over a relatively narrow concentration
range throughout the study area. Clg and C18 fatty acids occur commonly in
many organisms and are routinely reported in recent estuarine sediments
143
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(along with fatty acid methyl esters). Fatty acids, especially unsaturated
Cis and C^g fatty acids, have been reported as components of pulp mill
effluents (e.g., Leach and Thakore 1977) but did not appear to be highly
elevated in the East Waterway.
Two sterols were reported as TIO compounds: cholesterol and campes-
terol. Both compounds had maximum concentrations at Station EW-04 in the
East Waterway (cholesterol = 630 ug/kg DW; campesterol = 1,100 ug/kg DW),
although concentrations were generally not highly elevated.
Three TIO compounds reported in this study will not be discussed in
detail because their identities are not well characterized. The compounds
reported as base peak m/z (mass/charge) 181 (isomers 1 and 2) had simple
spectra with relatively strong ion intensities at m/z 165, 181, and 210 (the
latter was presumably the molecular ion). These compounds, which eluted
near one another during GC/MS analysis, both occurred at maximum concentra-
tions at Station EW-04 and had similar distributions overall (r>0.99, n=43,
PO.05). A compound tentatively identified as an alkanol also'maximized at
Station EW-04, but was widely distributed throughout the study area. This
compound had a mass spectrum with a characteristic alkane fragmentation
pattern and with no discernible molecular ion. However, the compound was
apparently of relatively high molecular weight, as it eluted near d^-
benz(a)anthracene (molecular weight = 240) during GC/MS analysis.
Volatile Organic CompoundsAcetone and total xylenes were infrequently
detected and occurred only in the East Waterway. Acetone was detected at
Stations EW-05 (230 ug/kg DW), EW-06 (140 ug/kg DW), EW-09 (120 ug/kg DW),
and EW-07 (83 ug/kg DW). Acetone was undetected at the remaining 15
stations tested with detection limits of 45 ug/kg DW or less. Total xylenes
were detected in the East Waterway along a transect of three stations
[Stations EW-09 (33 ug/kg DW), EW-08 (39 ug/kg DW), EW-07 (16 ug/kg DW)],
and at Station EW-01 (6 ug/kg DW). Detection limits at the other stations
tested were less than 25 ug/kg DW.
144
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Comparison with Recent Historical Data
Data from recent studies (1982 to 1987) of Everett Harbor were compiled
for comparison to contaminant distributions found in this study and for a
more comprehensive assessment of contamination. Data from the following
historical studies were compiled:
Storer and Arsenault (1987) - data from a sediment sampling
program conducted as part of the City of Everett CSO control
plan development.
Anderson and Crecelius (1985), Crecelius et al. (1984), and
U.S. Army Corps of Engineers (COE) (1985) - data from a
series of studies evaluating sediment quality relative to
development of the East Waterway port for the Navy
Battelle Northwest (1986) - a report presenting results of a
2-yr, multiagency study of eight locations in Puget Sound,
including Everett Harbor
U.S. EPA (1982) - unpublished results of sediment chemical
surveys of Everett Harbor performed in 1982
Mai ins et al. (1982, 1985) - data from three stations located
in and near the East Waterway (1982) and from two stations
located near Mukilteo (1985)
Chapman et al. (1984) - data from a survey of biological
effects in Everett Harbor, Samish Bay, and Bellingham Bay
conducted for the National Oceanic and Atmospheric Administra-
tion (only conventional sediment chemistry variables were
tested).
Sampling stations from these studies are plotted in Figures 31 and 32.
Historical data tended to confirm the distributions reported in the present
study in terms of overall trends. However, a number of chemicals that were
145
-------
LEGEND
» CHAPMAN ETAL. (1964)
0 CRECELIUS ET AJ_ (1964)
7 BATTELLE11966)
T US EPA (1982)
u UALINS ET AL (1982)
MALINSCTAL (19691
O ANDERSON ANOCRECELIUS(1965)
STORERANOARSENAUUri19e7)
O US APMVCORPSOFENOINEERS(196S]
mis STUDY
Figure 31. Locations of sampling stations from historical studies
of sediment chemistry in Everett Harbor.
146
-------
LEGEND
» CHAPMAN ETAL. (1984)
0 CRECELIUS ET AL. (1984)
-------
most concentrated in the present study (e.g., 4-methy1 phenol, dehydroabietic
acid) were not measured in historical studies. The chemicals detected at
high frequencies in historical studies were PAH, PCBs, and metals. Organic
EPA priority pollutants were measured by U.S. EPA (1982) but were typically
undetected at relatively high detection limits (typically 200 ug/kg DW for
A/B/N compounds). In the sections below, historical findings are discussed
for metals, PAH, PCBs, and several other chemicals. Phthalate ester and
methylene chloride data are not discussed because historical data were not
corrected for potential laboratory contamination.
Conventional Variables--
Sulfide and TOC measurements were made during only two of the nine
historical surveys. The highest historical concentrations of sulfide and
TOC were found in the East Waterway. The.maximum historical concentration
of sulfides (1,400 mg/kg DW) was measured at Station EDS-3 (U.S. Army COE
1985) along the southeastern shore of the East Waterway. Outside of the
.East Waterway, sulfide concentrations never exceeded the'210 mg/kg DW value
measured at Station EDS-1 in the Snohomish River. The maximum historical
concentrations of TOC (25 to 31 percent) were measured at Stations EDS-4
(U.S. Army COE 1985) and A4 (Anderson and Crecelius 1985) in the East
Waterway, near Station EW-13 of the present study (23 percent TOC). Outside
of the East Waterway, TOC concentrations never exceeded the 4.4 percent
value measured at Station EDS-2, located in the Snohomish River.
Metals--
Historical metals data generally supported the results of the present
study. The highest metals concentrations were generally measured in the
East Waterway. In no case did concentrations of metals of concern exceed
the maximum concentration measured in the present study (i.e., at Station
EW-14). Historical antimony and mercury data were limited by elevated
analytical detection limits. Antimony was undetected at all stations at
which it was measured at a maximum detection limit of 4.0 mg/kg DW. Mercury
detection limits were 0.4 mg/kg DW for many of the historical samples.
Three samples in the East Waterway had mercury concentrations exceeding the
148
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maximum reference area concentration; the highest mercury concentration
(0.406 mg/kg DW) was observed at Station E-06 (Battelle Northwest 1986).
Stations distributed across a relatively broad area exceeded the
maximum reference area concentrations for arsenic. Most of these stations
were within the East Waterway. However, the highest historical arsenic
concentration (46 mg/kg DW) was measured at Station e-11 (U.S. EPA 1982),
outside the East Waterway.
The highest historical concentrations of copper and lead (115 and 195
mg/kg DW, respectively) were measured at Station PS05 (Storer and Arsenault
1987), immediately adjacent to Station EW-07 of the present study (copper
and lead = 71 and 88 mg/kg DW, respectively). Historical copper concentra-
tions only exceeded the maximum reference area concentration in the East
Waterway or in the immediate vicinity of the East Waterway. Historical lead
and zinc concentrations exceeded maximum reference area concentrations over
the greatest area of metals measured in historical studies. Most of the
stations with high concentrations of these me'tals were located in the East
Waterway. However, sediment concentrations of both of these metals exceeded
their maximum reference area concentrations throughout the study area. The
highest historical concentrations of zinc (1,070-1,210 mg/kg DW) were
measured at Stations E-29 (U.S. EPA 1982) and E-04 (Battelle 1986), both
near Station EW-04 of the present study (235 mg/kg DW of zinc).
Concentrations of cadmium in historical data sets exceeded the maximum
reference area concentration only in the East Waterway. The highest
historical concentration of cadmium (4.63 mg/kg DW) was measured at Station
BPS-30 (Crecelius et al. 1984).
LPAH--
Historical LPAH data generally supported the results of the present
study, but comparisons revealed some spatial heterogeneity of concentrations,
especially in the East Waterway (Figure 33). Within the East Waterway,
highly contaminated Stations EW-04 and EW-07 (23,000 to 25,000 ug/kg DW)
were flanked by historical stations with high concentrations [Station E-04
149
-------
LEGEND
CHAPMAN ETAL. (1984)
0 CRECELIUS ETAL (1984)
v BATTELLE(1986)
* U.S. EPA (1982)
A MALINS ETAL (1982)
.4 MALINS ETAL. (1985)
D ANDERSON AND CRECELIUS (1985)
STORER AND ARSENAULTf 1987)
O U.S. ARMY CORPS OF ENGINEERS (1985)
THIS STUDY
LPAH
Designation
Number
1
2
3
4
ng/kg
(dry weight)
> 15,000
> 5,000- 15,000
>500 - 5,000
undetected - 500
Figure 33. Contours of LPAH concentrations in East Waterway
sediments.
150
-------
(17,000 ug/kg DW; Battelle Northwest 1986) and Station PS05 (100,000 ug/kg
DW; Storer and Arsenault 1987)]. Concentrations of most PAH were extremely
elevated at historical Station PS05, even when compared to adjacent Station
EW-07, which had EAR >1,000 for several PAH. However, results from the
present study and Storer and Arsenault (1987) agreed relatively well in
another area (Stations EW-10 and PS06 had LPAH concentrations between 5,200
and 8,100 ug/kg DW).
Historical LPAH concentrations outside the East Waterway were typically
<1,500 ug/kg DW, although a concentration of 11,000 ug/kg DW was observed at
Station MUK-B in Area NG (Malins et al. 1985). The concentration at Station
MUK-B was considerably, higher than that at adjacent Stations MUK-A and NG-10
(both 1,200 ug/kg DW).
HPAH--
Spatial heterogeneity in the East Waterway was more apparent for HPAH
than LPAH'(Figure 34). HPAH concentrations at three historical stations in
the East -Waterway (Stations PS05, EDS-4, and BPS-30) exceeded the maximum
HPAH concentration observed in the present study. The extremely high HPAH
concentration at Station PS05 (>200,000 ug/kg DW; Storer and Arsenault 1987)
exceeded the concentration at adjacent Station EW-07 by over 40 times.
Station EDS-4 (46,000 ug/kg DW; U.S. Army COE 1985) had a far higher
concentration than adjacent Station EDS-3 of the same study (8,400 ug/kg
DW). The HPAH concentration at Station BPS-30 (27,000 ug/kg DW; Crecelius
et al. 1984), was over 30 times higher than the concentration at the nearest
stations (E-02 and E-03; Battelle Northwest 1986).
Historical HPAH concentrations were typically far lower outside the
East Waterway (e.g., <5,000 ug/kg DW), although Stations MUK-B and MUK-A in
Area NG had concentrations of 15,000 and 5,700 ug/kg DW, respectively.
PCBs
PCBs were detected in roughly half of the 67 historical stations at
which they were measured. The highest historical PCB concentration occurred
151
-------
LEGEND
CHAPMAN ET AL. (1984)
0 CRECELIUSETAL. (1984)
<7 BATTELLE(1986)
T U.S. EPA (1982)
A MALINSETAL. (1982)
A MALINSETAL (1985)
Q ANDERSON AND CRECELIUS (1985)
STORER AND ARSENAULT (1987)
O U.S. ARMY CORPS OF ENGINEERS (1985)
THIS STUDY
Designation
Number
1
2
3
4
HP AH
ng/kg
(dry weight)
> 15,000
> 5,000- 15,000
>500 - 5,000
undetected - 500
Figure 34. Contours of HPAH concentrations in East Waterway
sediments.
152
-------
within the East Waterway (up to 1,000 ug/kg DW). Within the East Waterway,
PCB distributions appeared patchy (Figure 35), although stations on the east
shore and toward the head of the waterway were the mast contaminated. Three
historical stations near Station EW-04 (the station with the highest
concentration in the present study; 9,600 ug/kg DW) had concentrations
between 500 and 1,000 ug/kg DW (Stations E-29, E-03, and E-04) (U.S. EPA
1982; Battelle Northwest 1986). A PCB concentration of 1,000 ug/kg DW was
reported at Station BPS-30, north of that area. PCB concentrations from
100 to 650 ug/kg DW were reported at a number of other historical stations in
the East Waterway. However, PCBs were also undetected at low detection
limits (e.g., 20 ug/kg DW) throughout the East Waterway, including areas
with relatively high detected values (e.g., adjacent to Station BPS-30).
Other Organic Compounds
Phenol was detected only four times in historical studies (detection
limits for most historical stations were 200 ug/kg DW) (U.S. EPA 1982), but
detected concentrations generally supported the findings of the present
study. Along the east shore of the East "Waterway, the phenol concentration
at Station E-04 (1,400 ug/kg DW; Battelle Northwest 1986) was similar to
that at nearby Station EW-04 (2,100 ug/kg DW), and the concentration at
Station PS05 (660 ug/kg DW; Storer and Arsenault 1987) was similar to that
at nearby Station EW-07 (1,000 ug/kg DW). However, the phenol concentration
at Station E-01 was considerably lower than the blank-corrected value at
Station EW-01 (250 vs. 1,600 ug/kg DW).
Two historical stations in the East Waterway were analyzed for retene
(Maiins et al. 1982). The maximum level reported was similar to that
observed in the present study (roughly 3,000 ug/kg DW), although the highest
concentration observed by Mai ins et al. (1982; 2,900 ug/kg DW at Station M01)
was considerably higher than at nearby Station EW-11 of the present study
(62 ug/kg DW).
Total xylenes were detected once in historical studies (Station PS05 in
the East Waterway, 140 ug/kg DW; Storer and Arsenault 1987). Total xylenes
were detected in the same area during the present study in a cross-waterway
153
-------
LEGEND
CHAPMAN ETAL. (1984)
0 C REG ELIUS ET AL. (1984)
V BATTELLE(1986)
T U.S. EPA (1982)
A MALINS ETAL. (1982)
A MALINS ETAL (1985)
O ANDERSON AND CRECELIUS (1985)
STORER AND ARSENAULT (1987)
3 U.S. ARMY CORPS OF ENGINEERS (1985)
THIS STUDY
PCBs
Designation
Number
(dry weight)
> 1,000
> 500 - 1,000
>100-500
undetected - 100
Figure 35. Contours of PCS concentrations in East Waterway
sediments.
154
-------
transect composed of Stations EW-07, EW-08, and EW-09 (16 to 39 ug/kg DW).
Other volatile organic compounds were detected at the two stations from
Storer and Arsenault (1987) (e.g., trichloroethene at 400 ug/kg DW and
60 ug/kg DW at Stations PS05 and PS06, respectively; acetone, at 2,800 and
910 ug/kg DW at Stations PS05 and PS06, respectively). Blank contamination
by acetone, a common laboratory contaminant, is not documented in Storer and
Arsenault (1987).
Summary
The East Waterway was clearly the most contaminated of all
study areas. The highest concentrations of virtually all
chemicals measured in the study occurred at stations in the
East Waterway (e.g., Stations EW-01, EW-04, EW-07, EW-13, and
EW-14, all along the east shore). The predominance of East
Waterway contamination relative to other areas is apparent
from the summary information in Table 21, in which stations
are characterized by 90th percentile exceedances for a
diverse range of chemicals. . More moderate contamination in
terms of concentrations and complexity of contaminant
assemblages was observed in offshore and nearshore Port
Gardner study areas (i.e., Areas OG and NG) and at other
relatively isolated stations (e.g., Station SR-05 in the
Snohomish River).
Organic compounds were much more widely distributed at
elevated concentrations than metals. Among the organic
compounds with the highest detection frequencies and reported
at the highest concentrations were 4-methylphenol (maximum
concentration = 98,000 ug/kg DW; EAR=7,500), dehydroabietic
acid (maximum concentration = 83,000 ug/kg DW; EAR=1,300),
abietic acid (maximum concentration = 98,000 ug/kg DW;
EAR=650), PAH (naphthalene in particular; maximum concentra-
tion = 17,000 ug/kg DW; EAR=3,000), and several tentatively
identified organic compounds (most notably, a diterpenoid
hydrocarbon thought to be dehydroabietane; maximum concentra-
155
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ES-01
SD-03
TABLE 21. NUMBER OF CHEMICALS OF CONCERN EXCEEDING
90TH PERCENTILE CONCENTRATIONS*
Station
Miscellaneous
Resin Phenols/ PCBs/ Extractables/
Metals PAH" Acids Guaiacols Pesticides TIO Compounds
Nitrogen-
Containing
Phthalates Compounds
Volatile
Organic
Compounds
EW-01
EW-02
EW-03
EW-04
EW-05
EW-07
EW-08
EW-10
EW-11
EW-12
EW-13
EW-14
EW-15
N6-01
NG-03
NG-04
NG-05
NG-07
NG-08
KG-09
NG-11
NG-14
NG-15
OG-03
OG-06
3 1
4 16 6
592
4 2
1
4 16 3
6 17
2
9
10
1
8
4
1
8
1
3
2
2
1
1
4
1 14
1 6
6
6
1
7
6
2
1
1
1
1
1
1
1 2
1
1
1
1
1 1
1
1
1
1
1
1
1
1
SR-05
SR-07
SS-01
a Stations not shown did not have any chemicals exceeding 90th percentile concentrations. Chemicals exceeding 90th
percentile concentrations but not exceeding Puget Sound reference area concentrations were not included. Chemicals included
in each group are listed in Tables 14 and 17.
Includes LPAH and HPAH as groups as well as individual PAH.
156
-------
tion = 23,000; EAR>1,000). Other organic compounds occurred
at high concentrations at relatively isolated stations [e.g.,
PCBs (maximum concentration) = 9,600 ug/kg DW (EAR=1,600)].
All of the compounds mentioned above occurred at maximum
concentrations along the east shore of the East Waterway.
Metals concentrations were highly elevated at a single
station in the study (Station EW-14 in the East Waterway),
particularly for zinc (5,910 mg/kg DW; EAR=310), copper
(1,010 mg/kg DW; EAR=160), and arsenic (685 mg/kg DW;
EAR=200). Outside the East Waterway, 4-methylphenol was most
elevated over the widest area of any measured chemical.
Historical sediment chemistry data generally supported the
findings of the present study, although considerable spatial
heterogeneity was apparent for HPAH and PCBs in the East
Waterway. Notably, available historical studies did not
provide data for the organic compounds found at the highest
concentrations in the present study (.especially 4-methyl-
phenol, -dehydroabietic acid, and abietic acid) or for
distinctive geochemical tracers of the pulp industry observed
in the present study (especially chlorinated derivatives of
compounds occurring in coniferous woods, such as chlorinated
resin acids and chlorinated guaiacols).
BIOACCUMULATION
Bioaccumulation studies were conducted -to determine if selected
contaminants were accumulated in the tissues of indigenous organisms in the
Everett Harbor study area. The contaminants selected for analysis (PCBs,
mercury, and 12 chlorinated pesticides) have a high potential for accumula-
tion in higher organisms such as fishes and crabs. Previous studies in
Everett Harbor have also indicated that PCBs may be bioaccumulated at
concentrations exceeding reference levels. The objective of the present
study was to describe the geographic trends in bioaccumulation and to
determine whether tissue contaminants in the Everett Harbor study area were
elevated above concentrations observed at the Port Susan reference area.
157
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Mercury In Dunoeness Crabs
Mercury concentrations in edible muscle tissue of Dungeness crabs
(Cancer macn'ster) are presented in Figure 36. In general, mercury concentra-
tions were relatively homogeneous and low throughout the study area, ranging
from 0.042 to 0.130 mg/kg wet weight. Although tissue concentrations in
crabs from the East Waterway and Port Gardner shoreline were slightly higher
than at the Port Susan reference area, the maximum elevation above reference
was only 2.0 at Station EW-92. Crabs from the lower Snohomish River and
Snohomish River Delta areas had slightly lower mercury levels than crabs
from the reference area. Because sampling was not replicated at each
station, tests of the statistical significance of the observed differences
were not performed.
PCBs and Pesticides in Dunqeness Crabs
All 12 pesticides measured were undetected in the crab samples from the
Everett Harbor study area;. Detection limits for these substances ranged
from 0.1 to 0.8 ug/kg wet weight.
PCB concentrations in Dungeness crabs from the Everett Harbor study
area are presented in Figure 36. PCBs were detected in crab muscle samples
from all stations except SD-91. Because of low analytical recoveries (see
Bioaccumulation, Quality Assurance/Quality Control Results in Methods
section), all PCB data are considered potential underestimates of actual PCB
levels. In addition, the crab tissue data were not replicated at any
station except EW-91. Because of these limitations, no statistical analyses
were conducted to determine among-station differences. Instead, the data
are used only for relative comparisons of PCB levels among sampling sites.
The highest average PCB level measured in crabs (24 ug/kg wet weight)
was 4.7 times higher than the reference level and was measured at Station
NG-92 near Mukilteo. Lower PCB concentrations (i.e., 0.7 to 2.4 times the
reference level) were measured along the south Port Gardner shoreline and in
the lower Snohomish River. Crabs collected from the three Snohomish River
delta sites had PCB concentrations equal to or less than the reference level.
158
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STATIONS
LEGEND
P S Port Susan
NG Nearshore Port Gardner
EW East Waterway
S 0 Snohomish River Delta
S R Snohomish River
Figure 36. Concentrations of RGBs and mercury in Dungeness
crab muscle tissue samples from Everett Harbor and
Port Susan.
159
-------
As discussed in the Methods section, the PCB tissue data did not meet
the minimum 50 percent surrogate recovery levels specified by PSEP (Tetra
Tech 1986g). Recovery of a surrogate compound (DBOFB) can be used, however,
to calculate an estimated PCB concentration that may be more representative
of actual PCB levels than the low-recovery measurements for this study.
Although a single surrogate compound cannot accurately represent recovery of
all 209 possible PCB congeners, previous performance tests performed by
Battene (PTI and Tetra Tech 1988) indicated that DBOFB recoveries were
similar to overall recoveries of spiked PCB mixtures. For Station NG-92,
the DBOFB recovery was 36 percent, resulting in a theoretical maximum PCB
concentration in crabs of 67 ug/kg wet weight (i.e., 2.78 X 24 ug/kg). The
corresponding reference level in crabs corrected for DBOFB recovery was 18
ug/kg wet weight. Similar applications of surrogate recovery corrections
for the other sampling stations did not result in any calculated average PCB
levels exceeding 61 ug/kg wet weight. Therefore, using this approach, the
maximum calculated EAR for PCBs in crab tissue is 3.7 at Station NG-92.
Mercury, in English So^le
Mercury concentrations in English sole (Parophrvs vetulus) edible
muscle tissue from Everett Harbor are presented in Figure 37. In general,
mercury concentrations were relatively homogeneous throughout the study
area. The highest average mercury levels (0.067 mg/kg wet weight) were
measured at the Port Susan reference area. Mean concentrations of mercury
in English sole samples from Everett Harbor ranged from 0.010 to 0.062 mg/kg
wet weight, with no evidence of mercury bioaccumulation above reference
levels.
The relationship between mercury concentrations and muscle lipid
content was examined to determine if differences in lipid content were
influencing the bioaccumulation results. These analyses showed a statis-
tically significant negative correlation between total extractable organic
matter (a measure of lipid content) and mercury concentration (r=-0.34,
n=54, P<0.01). Thus, fish with higher lipid contents tended to have lower
mercury levels. The lipid content of English sole from the reference area
(8.6 mg/kg wet weight) was intermediate in the range of values for the
Everett Harbor area (6.7 to 15 mg/kg wet weight). Based on the relatively
160
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LEGEND
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Port Susan
Nearshore Port Gardner
East Waterway
Snohomish River Delta
Snohomish River
Figure 37. Concentrations of PCBs and mercury in English
sole muscle tissue samples from Everett Harbor and
Port Susan.
161
-------
low correlation of these variables, the relatively constant mercury concen-
trations, and the intermediate lipid levels at the reference site, it does
not appear that major differences in mercury concentrations among sampling
stations are due to differences in lipid content.
PCBs and Pesticides in English Sole
None of the 12 pesticides measured were detected in any of the English
sole tissue samples. The detection limits ranged from 0.1 to 0.8 ug/kg wet
weight for these analyses.
PCB concentrations in English sole muscle tissue samples are presented
in Figure 37. The mean PCB concentrations (as averages for five individual
fish) ranged from a minimum of 8.3 ug/kg wet weight at the reference site to
a maximum of 43 ug/kg wet weight at Station NG-92 near Mukilteo. The EAR
for measured concentrations ranged from 1.3 on the Snohomish Delta to 5.1 at
Mukilteo. Overall, the maximum value for an individual fish (99 ug/kg wet
weight) was measured in the lower Snohomish River. PCBs were detected in
all but two of the individual samples analyzed (detection limit of 3.5 ug/kg
wet weight).
The PCB data for English sole were characterized by the same low
surrogate recoveries as the crab data. The data should therefore be
considered as potential underestimates of actual PCB levels. The surrogate
recoveries were relatively consistent among sampling sites (most were 25 to
36 percent). Therefore, the data are probably accurate representations of
the relative magnitudes of PCB tissue concentrations among sampling sites.
For Station SR-92, the average DBOFB recovery was 26 percent, resulting in a
theoretical maximum PCB concentration in fish tissue at this sampling
station of 130 ug/kg wet weight (i.e., 3.85 x 34 ug/kg). The corresponding
reference level in sole corrected for DBOFB recovery was 35 ug/kg wet
weight. Similar applications of surrogate recovery corrections for the
other sampling stations did not result in any calculated average PCB levels
exceeding 120 ug/kg wet weight. Therefore, using this corrective approach,
the maximum calculated EAR for PCBs in fish muscle tissue was 3.7 at Station
SR-92.
162
-------
There was no statistically significant correlation between the muscle
lipid content of English sole and tissue concentration of PCBs (r=0.21,
n=54, P>0.05). The concentrations of total extractable organic matter were
also similar between the reference site (8.6 mg/g wet weight) and Station
SR-92 (9.6 mg/g wet weight). Therefore, it does not appear that any
differences in lipid content were influencing apparent differences in PCS
levels among sampling sites.
Comparison with Recent Historical Data
Historical data on bioaccumulation in fishes and crabs from the Everett
Harbor study area are very limited. The only available data on bioaccumula-
tion in English sole muscle tissue are in Cunningham (10 November 1982,
personal communication). In this study, PCB levels in English sole muscle
tissue ranged from 49 to 190 ug/kg wet weight in samples from the East
Waterway, Snohomish River, and Gedney Island. The maximum concentration was
measured in a sample from the Snohomish River. The PCB data are similar to
the PCB levels measured in the present study, especially when the latter
data are corrected for low surrogate recoveries. The maximum PCB level
measured was slightly higher than the maximum theoretical level calculated
for this study (130 ug/kg wet weight) (Cunningham, D., 10 November 1982,
personal communication).
Summary
For both Dungeness crabs and English sole, none of the 12
measured pesticides were detected in edible muscle tissue
from the Everett Harbor study area.
Mercury concentrations in edible muscle tissue from Dungeness
crabs and English sole from the Everett Harbor study area
were similar to, or less than, mercury levels in organisms
from the Port Susan reference area.
Interpretation of PCB data was limited by low analytical
recoveries. Measured PCB levels were generally higher in
163
-------
Dungeness crabs and English sole from the Mukilteo area, the
Snohomish River, and the East Waterway than in the Port Susan
reference area. However, the maximum theoretical concentra-
tions of PCBs (after adjustment for surrogate recoveries) in
crab and fish samples were not elevated substantially above
the reference area levels (i.e., maximum EAR of 3.7) and were
low when compared to other urban embayments in Puget Sound.
PCB levels measured in. crabs and fish in this study were
similar to levels measured in a previous study in Everett
Harbor.
SEDIMENT BIOASSAYS
The results of sediment toxicity tests using the amphipod Rhepoxvnius
abronius are presented in this section (see Appendix D for data listing).
First, amphipod bioassay results for Port Susan are compared with results
from other reference areas used during previous studies. The amphipod
mortality values for each station in the Everett Harbor system 'are then
presented and compared statistically with the Port Susan values. Finally,
results of the present study are compared with those of previous studies on
the toxicity of Everett Harbor sediments to R. abronius.
Evaluation of the Reference Area
Mean values of amphipod survival and their 95 percent confidence limits
are shown in Figure 38 for individual stations in Port Susan and other
reference areas of Puget Sound. Data for the 1985 survey of Port Susan,
which were collected as part of the Elliott Bay Toxics Action Program, are
also shown in the figure. Mean amphipod survival for several of the Port
Susan observations was low (<80 percent) relative to data for most other
reference areas. Mean survival was also low (<75 percent) at one station in
Carr Inlet, where a single replicate was an extreme outlier, and at one
station in Sequim Bay. The relatively low survival at some Port Susan
stations cannot be explained by a response of the amphipods to fine-grained
sediments. The product-moment correlation between mean amphipod survival
164
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CARR BLAKELY
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1986
PORT
SUSAN
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Figure 38. Amphipod bioassay data from Puget Sound reference areas.
-------
and percent fine-grained material at Port Susan stations was not significant
(r=0.38, n=7, P>0.05). The range of percent fine-grained material in
samples collected during 1985-1986 in Port Susan was 7.4-88 percent. Only a
single sample contained more than 24 percent fine-grained material.
Moreover, mean amphipod survival for that sample (Station PS-01, 1985) was
relatively high (87 percent).
The 1986 data for amphipod response to Port Susan sediments include one
station (PS-02) where mean survival (71 percent) indicated that the sediment
was toxic based on a toxicity threshold value (i.e., survival <76.4 percent)
derived in an extensive interlaboratory comparison by Mearns et al. (1986).
Consequently, the 1986 data from this station were unacceptable for use as
reference data and were excluded from further analyses. The 1986 data for
amphipod response to Port Susan sediments at Stations PS-03 and PS-04 are
considered marginally adequate for use as reference data. The mean survival
of amphipods exposed to sediments collected from these two stations during
1986 was 78 percent. " Nevertheless, Everett Harbor sites were compared
statistically with Port Susan rather than the West Beach (Whidbey Island)
control site because the latter is the natural habitat of the amphipods used
in this study. Use of a separate reference area (Port Susan) minimizes the
possible bias due simply to removal of amphipods from their native habitat
and placement in a non-native sediment. Moreover, Port Susan appears to be
an adequate reference area based on data for other indicators (see results
for sediment chemistry, bioaccumulation, benthic infauna, and fish pathol-
ogy). Contaminant concentrations in sediments at Stations PS-03 and PS-04
were typically within the range of those observed at other reference areas in
Puget Sound and were low relative to Puget Sound AET (see above, Sediment
Chemistry). Therefore, the 1986 bioassay data from Stations PS-03 and PS-04
were used for statistical comparisons with data from sites in the Everett
Harbor system.
General Patterns of Amohipod Mortality
The mean amphipod mortality and the range of station-specific means for
each study area within the Everett Harbor system and the reference area
(1986) are shown in Figure 39. The highest overall mortalities were found
166
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39. Mean and range of amphipod
bioassay responses within study areas.
-------
in the East Waterway (mean mortality = 63 percent). Total mortality
(100 percent) was observed at Stations EW-01 and NG-04. The range of mean
mortality at stations within the East Waterway and Nearshore Port Gardner
study areas (the most intensively sampled areas) was large, indicating
considerable spatial heterogeneity. Some stations within each area exhibited
mean mortality values less than or equal to the values for Stations PS-03 and
PS-04 in Port Susan.
Comparison of the Everett Harbor System with Port Susan
Results of the amphipod bioassay tests for all stations sampled during
the Everett Harbor investigation are summarized in Table 22. Statistical
comparisons between Everett Harbor sites and the reference area (Port Susan
1986, Stations PS-03 and PS-04 pooled) indicated that mean mortalities for
four test sediments were significantly different from the Port.Susan samples
(P<0.001). Three of these toxic sediments were from the East Waterway; one
was from Nearshore Port Gardner near the defense fuel storage depot at
Mukilteo (Figure 40).
At three of the seven stations that exhibited a mean amphipod mortality
>40 percent, mean mortality was not statistically different from the mean
reference value at PO.001. However, these stations (EW-10, NG-06, and
OG-03) did exhibit a significant difference from the reference area at
PO.05. The lack of significance at PO.001 for mean mortality values over
40 percent at some stations can be explained by low statistical power, partly
due to the relatively high mean mortality in the reference area. Also, the
variance of the bioassay test is typically higher at intermediate mortality
values (35-65 percent) compared with the extremes of the mortality range.
The variance of the mean was very high [standard deviation >28, corresponding
to a standard error >12] at three stations: Stations EW-10, OG-03, and
SR-07. The relative influence of reference mortality vs. variability on the
statistical power of the amphipod bioassay is being investigated in a
separate EPA project on refinement of sediment quality values.
168
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TABLE 22. SUMMARY OF AMPHIPOD BIOASSAY RESULTS
Station
ES-01
ES-02
ES-03
EW-01
EW-04
EW-07
EW-10
EW-12
EW-14
NG-01
N6-02
NG-03
NG-04
NG-06
NG-10
NG-12
NG-13
NG-14
NG-15
Range of
Mortality
(percent)
0-20
5-25
0-25
100B
95-100
60-100
10-100
10-20
15-55
0-10
0-15
5-15
100B
25-55
0-10
0-10
0-10
0-10
0-5
Mean
Mortality3
(percent)
10(4.2)
12(3.7)
15(4.2)
100(0)*
99(1.0)*
75(8.4)*
55(19)
13(2.0)
37(7.2)
5(1-6)
6(2.4)
13(2.0)
100(0)*
43(5.6)
5(1.6)
2(2.0)
6(1.9)
5(2.2)
1(1.0)
OG-03
15-90
58(12)
PS-02
PS-03
PS-04
SD-01
S'D-02
SR-01
SR-02
SR-04
SR-07
SR-08
SS-01
SS-03
Control0 A
Control B
Control C
Control 0
20-40
15-40
5-35
5-20 .
15-50
0-35
0-10
15-30
0-80
0-30
0-10
0-10
0-10
0-25
5-15
0-10
29(4.0)
24(4.6)
20(6.3)
15(3.2)
29(7.0)
12(6.0)
4(1.9)
21(2.9)
33(13)
15(5.7)
5(2.2)
6(2.4)
5(2.2)
10(4.2)
9(1.9)
4(1.9)
a Mean mortality is based on five replicate samples per station. Standard error
of each mean is given in parentheses.
° A mortality level of 100 percent was observed for each of the five replicates.
c Clean control sediments from the amphipod collection site at West Beach, Whidbey
Island.
*
Asterisk denotes that mean mortality differed significantly (P<0.001) from the
mean mortality of pooled replicates from two Port Susan stations (PS-03 and PS-
04).
169
-------
E W EAST WATERWAY
N G NEARSHORE PORT GARDNER
Figure 40. Significant (P < 0.001) amphipod bioassay mortalities
compared to the Port Susan reference area.
170
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Comparison with Recent Historical Data
There are no R. abronius sediment bioassay test data for Everett Harbor
in the Puget Sound Environmental Atlas (Evans-Hamilton and D. R. Systems
1987). Amphipod bioassay data from previous tests of Everett Harbor
sediments-were summarized by Long (unpublished). However, these data were
obtained from tests that deviated substantially from PSEP protocols (Tetra
Tech and E.V.S. Consultants 1986). Either the sediments were stored frozen
before being tested or, in one case (i.e., Battelle Northwest 1986), tested
without replication.
The results of unreplicated amphipod bioassays must be interpreted
cautiously. However, it should be noted that the Battelle Northwest (1986)
data support the results of the present study. The highest toxicity was
recorded in the East Waterway near a station where significant toxicity was
found in the present study. No historical data are available for the
Mukilteo area, where significant toxicity was found in the present study
(i.e., Station NG-04).
The U.S. Army COE (1985) tested composite samples from the East
Waterway and found relatively high toxicity in these sediments. Because the
sediments were composited, the magnitude of toxicity at specific stations is
unknown.
Summary
Sediments from 4 of the 29 Everett Harbor stations tested
displayed significant toxicities (P<0.001) in the amphipod
bioassay when compared with the Port Susan reference area
(Figure 40) (Table 22)
Although previous data are limited, there was good agreement
between the present study and results of previous amphipod
bioassays in Everett Harbor
171
-------
The most toxic area in Everett Harbor was the East Waterway.
Significant toxicity was also found at one station near
Mukilteo (Station NG-04).
BENTHIC MACROINVERTEBRATES
The purposes of this section are to describe the general characteristics
of benthic communities in Everett Harbor and the Port Susan reference area,
and to identify areas where benthic communities may be impacted. Charac-
terization of the benthic communities within Everett Harbor is based on the
abundance and distribution of individual taxa and the major infaunal
taxonomic groups (i.e., polychaetes, pelecypods, gastropods and crustaceans).
Identification of potentially impacted areas is based on comparisons of
benthic community indices among Port Susan and Everett Harbor stations
including major taxa abundance, species richness, abundance of dominant
taxa, pollution-tolerant or opportunistic taxa, and similarity of species
distributions.
The following discussion is organized into several major topics.
First, the adequacy of the reference area (Port Susan) is evaluated.
Second, the general characteristics of infaunal communities within Everett
Harbor and in Port Susan are described, and abundances of major taxonomic
groups are compared statistically to identify areas of impact. Third,
species level data are used to characterize each station and refine the
identification of the type of stress that may be impacting the benthic
community. Individual stations or areas within Everett Harbor that appear
to be degraded and the degree of the apparent degradation are then discussed.
Finally, comparisons are made with historical data.
Evaluation of the Reference Area
The ideal reference area for any investigation of anthropogenic effects
would be identical to the potentially impacted area, but would lack all
anthropogenic influences. This condition is not achievable because no two
areas are exactly alike naturally, and because most areas exhibit some
evidence of human activities. Nevertheless, a reference area should possess
172
-------
as many characteristics in common with the study area as possible, with the
exception of anthropogenic impacts, to allow unbiased comparisons between
areas. In this investigation, Port Susan was selected as the reference area
for benthic communities in Everett Harbor based the following characteris-
tics:
It has a major riverine input (i.e. Stillaguamish River)
similar to that of the Snohomish River in Everett Harbor
It does not have any major sources of contamination other
than possible slight organic enrichment from the Stillaguamish
River
It exhibits a range of sediment grain sizes similar to most
stations sampled in Everett Harbor
It is adjacent to the Everett Harbor study area and is likely
to share similar benthic fauna and physical influences (e.g.
currents, weather patterns). .
Port Susan is an extremely productive estuary, indicating that ample
sources of nutrients are- available to support the biota. The Stillaguamish
River may potentially be a source of nutrient enrichment in Port Susan, as
much of the river's watershed is agricultural. However, the sediment data
collected during both the 1985 Elliott Bay investigation (where Port Susan
was used as the reference area) and this survey do not show evidence of
organic enrichment in Port Susan.
Grain-size characteristics of the sediments at stations in Port Susan
appear to have been affected slightly by their distance from the mouth of
the Stillaguamish River. Station PS-04 (furthest from the river mouth)
consisted of coarse sandy sediments, whereas Station PS-02 (closest to the
river mouth) consisted of fine sandy sediments (see Appendix E). Other
conventional sediment variables (i.e., nitrogen, total organic carbon, total
solids) also exhibited slight gradients in relation to the distance from the
river (see Appendix E).
173
-------
Sediments at stations sampled in other selected reference areas in
Puget Sound are also predominantly sandy (Table 23). Mean concentrations of
total organic carbon, sulfides, and total solids at the Port Susan stations
were similar to those documented in the other reference areas listed in
Table 23, and appear to be typical of unimpacted areas.
Abundances of the major benthic taxonomic groups at the Port Susan
stations were also similar to those in other reference areas within Puget
Sound. Mean total abundances and mean abundances of polychaetes, molluscs,
and crustaceans were generally similar to mean abundances observed in Carr
Inlet, Blakely Harbor, Central Puget Sound (15-22 m depths), and at Port
Susan stations sampled in 1985 (Figure 41).
Comparisons of mean total abundances and mean abundances of the major
benthic macroinvertebrate taxa groups in Port Susan between 1985 and 1986
revealed differences between years (Figure 41). Mean total abundances were
significantly (P<0.05) lower in samples collected tn 1986 than in 1985.
Mean abundances among the major taxonomic groups were lower in 1986,
reflecting the decrease in total abundance, but the differences between
years were not statistically significant (P>0.05) for any major taxonomic
group.
Examination of the five most abundant taxa at each station in Port
Susan indicated that species composition was fairly similar both within and
between years (Table 24). Two to four species at each station were also
among the abundant taxa at the other stations in Port Susan. This high
degree of similarity documents that structurally similar assemblages of
benthic macroinvertebrates were sampled at all three stations in Port Susan
in 1986, and suggests that those assemblages were temporally stable.
Comparisons of the five most abundant species at the 1985 and 1986 Port
Susan stations with those at the Carr Inlet stations reveals little similar-
ity between these two areas (Table 24). This is not unexpected, however,
because Port Susan and Carr Inlet are located in different regions of Puget
Sound and exhibit different habitat characteristics (e.g., exposure,
freshwater input).
174
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TABLE 23. SURFACE SEDIMENT CHARACTERISTICS AT BENTHIC
INFAUNA STATIONS IN PORT SUSAN COMPARED WITH
OTHER REFERENCE AREAS IN PUGET SOUND
Reference Area
Port Susan (1985)b
Port Susan (1986,
this study)
Carr Inletd
Blakely Harbor6
Central Puget^
Sound (Seahurst)
Samish Bay9
Case Inlet9
Sequim Bay9
Sediment
Type3
sand-
clayey silts
sand
sand
sand
sand
silty sand/
clayey silt
" sandy silt
sandy silt
Mean TOC
0.78
0.34
0.41
1.65
1.51
1.65
2.2
2.35
Mean Sulfide
(mg/kg)
22.8
Uc
2.3
-15
--
--
--
--
Mean Total Depth
Solids (%) Range (
66.4 10-12
77.4 11-12
70.4 2-26
67.8 10-18
15-22
10-30
21-41
19-26
a Sediment type designations after Shephard (1954).
b Data from PTI and Tetra Tech (1988).
c Undetected at a detection limit of 6 mg/kg dry weight.
d Data from Tetra Tech (1985a).
e Data from Tetra Tech (1986d).
f Data from Word et al. (1984).
9 Data from Battelle (1986).
175
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INLET
(4 Stations)
LEGEND
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SEAHURST
(58 Stations)
(3 Stations)
Figure
41
. Mean total
abundances (no./m2) and
groups of benthic
invertebrates
mean
abundances of major taxonomic
in Puget Sound
reference areas.
-------
TABLE 24. NUMERICALLY DOMINANT TAXA AT PORT SUSAN
STATIONS SAMPLED IN 1985 AND 1986, AND AT
CARR INLET STATIONS SAMPLED IN 1984
Port Susan 1985 Port Susan 1986 Carr Inlet 1984
PS1 PS2 PS3 PS4 PS2 PS3 PS4 CR11 CR12 CR13 CR1<
Protomedia prudens
Psephidia lordi
Terebellldes stroemi
Euphilomedes producta
Lumbrineris spp.
Axlnopsida sern'cata
Lumbrineris luti »
Euphilomedes carcharodonta »
Ampharete acutifrons
Clinocardium nuttali
Leitoscoloplos pugetensis
Pectinaria qranulata
Macoma baltica
Pista spp.
Leptochelia dubia
Phvllochaetopterus prolifica
Prionospio steenstrupi
Qdostomia spp.
Platynereis bicanaliculata
Amphioda urtica
Scalibreqoma inflatum
Mitre11 a gauldi
Macoma nasuta
Caprellidae
Caprella mendax
Spiophanes berkelvorum
177
-------
Opportunistic and pollution-tolerant taxa (as defined by Pearson and
Rosenberg 1978) constituted an average 28.2 percent of the fauna at the
stations in Port Susan (Table 25). In Carr Inlet 21.8 percent of the fauna
was represented by those same taxa. Prionospio steenstruoi. Macoma nasuta
and Euphilomedes carcharodonta constituted most of the opportunistic and
pollution-tolerant organisms in Carr Inlet, accounting for 14.7 percent of
the total population. .Euphilomedes carcharodonta and E. producta were
abundant at stations in Port Susan, and accounted for nearly all of the
opportunistic and pollution-tolerant taxa at those stations. Euphilomedes
spp. are known to increase in abundance in areas where slight to moderate
organic enrichment has occurred (Word et al. 1977). Because Euphilomedes
spp. are common in areas of only moderate enrichment, these taxa may not be
a strong indicator of benthic community stress. Therefore if abundances of
Euphilomedes spp. are not considered in the foregoing calculations, oppor-
tunistic and pollution-tolerant organisms would have constituted <12.0
percent of the benthic macroinvertebrates at all stations in Port Susan, and
19.3 percent of the benthic macroinvertebrates in Carr Inlet. Thus,
abundances of opportunistic and pollution-tolerant taxa in Port Susan were
low, and appeared to be comparable to Carr. Inlet.
Overall, the foregoing comparisons of conditions in Port Susan in 1986
with conditions in other reference areas in Puget Sound, and with Port Susan
in 1985, affirm the adequacy of Port Susan as a reference area for benthic
macroinvertebrate communities in Everett Harbor. Sediment grain-size
characteristics, the values of other conventional sediment variables, and
abundances of the major taxonomic groups of benthic invertebrates at the
three Port Susan stations were similar to those in other reference areas.
The similarity between the numerically dominant taxa collected at the three
Port Susan stations sampled in both 1985 and 1986 further indicates that the
structure of the benthic assemblages in Port Susan may be temporally stable.
Finally, abundances of opportunistic and pollution-tolerant taxa were found
to be low, and comparable to the Carr Inlet reference area.
178
-------
TABLE 25. RELATIVE ABUNDANCES (PERCENT TOTAL FAUNA) OF
OPPORTUNISTIC AND POLLUTION-TOLERANT TAXAJ* AT STATIONS IN
PORT SUSAN AND CARR INLETb
Stations
Taxon
Euphilomedes carcharodonta (Os)^
Euphilomedes producta (Os)
Glvcinde picta (Po)
Gon.iada brunnea/maculata (Po)
Leitoscoloplos puqettensis (Po)
Macoma balthlca (Pe)
Macoma nasuta (Pe)
Mediomastus spp. (Po)
Nephtvs cornuta franclscana (Po)
Paraprionospio pinnata (Po)
Pn'onosplo steenstrupi (Po)
Scololplos armiger (Po)
Others
(No. of taxa)
Total
PS-02
8.3
1.3
0.0
0.3
5.3
1.6
0.0
0.5
0.0
0.0
0.3
0.5
0.7
(6)
18.8
PS-03
17.6
6.0
0.2
0.6
3.4
6.0
0.0
<0.1
0.0
0.0
0.5
0.1
0.3
(3)
34.7
PS-04
16.7
10.5
0.0
0.7
0.9
0.0
1.0
<0.1
0.0
0.0
0.7
O.I
0.9
(7)
31.4
Carr Inletc
2.9
0.1
0.5
0.1
1.6
0.2
3.2
1.6
0.7
0.7
8.6
0.0
1.9
(6).
21.8
a As defined by Word et al. (1977), Pearson and Rosenberg (1978), and Word (1980).
b Data from Tetra Tech (1985a).
c Mean value of four stations.
d Os=0stracoda, Po=Polychaeta, Pe=Pelecypoda.
179
-------
Justification of Use of Pooled Port Susan Data
In this study, impacts to the benthos were inferred using statistical
criteria to identify changes in the abundances of the major taxonomic groups
of benthic invertebrates. When comparing benthic communities in potentially
impacted areas with those in reference areas, it is often advisable to
stratify between-station comparisons by habitat characteristics. Because
sediment grain size is an important determinant of benthic community
structure (Sanders 1960; Johnson 1971; Gray 1974; Fresi et al. 1983), it can
be used to define the strata.
Sediments in Everett Harbor exhibited a wide variety of textural
characteristics, that ranged from clayey silts to coarse sands (Figure 42).
In many areas of Everett Harbor, the sediments showed evidence of anthro-
pogenic inputs, and can no longer be considered representative of "natural"
conditions. Typically, these sediments smelled of hydrogen sulfide or
petroleum, or both. Wood chips were common in the grab samples, as was
scrap metal, oil droplets, and other debris. Field notes indicate that over
*
half the stations sampled in E.verett Harbor exhibited evidence of sediment
modification (e.g., hydrogen sulfide, petroleum, foreign objects). Largely
because of these anthropogenic modifications, the entire spectrum of
sediment characteristics in Everett Harbor is not present in Port Susan.
The previous evaluation of Port Susan as a reference area and an a
priori examination of the sediment characteristics and benthic community
structure in Everett Harbor indicated that:
Total abundances and abundances of the major taxonomic groups
of benthic invertebrates in Port Susan were comparable to
abundances in other reference areas in Puget Sound, despite
differences in species composition
Species composition among Port Susan stations was temporally
stable between 1985 and 1986
180
-------
CLAY
SAND
SILT
Figure 42. Sediment grain size characteristics at benthic infauna
stations in Everett Harbor and Port Susan (1986).
181
-------
Species composition of dominant taxa among Port Susan
stations was very similar
Sediment characteristics among the three Port Susan stations
were very similar
The sediments in Everett Harbor are highly modified in many-
cases, and many sediment characteristics cannot be "matched"
in Port Susan.
For these reasons, data on abundances of the major taxonomic groups at the
three stations in Port Susan were not stratified by habitat characteristics
prior to statistical testing. Stratification of between-station comparisons
by sediment grain size would be inconsistent because grain-size characteris-
tics cannot be matched in many of the paired comparisons. Instead, the data
were pooled, such that mean values of variables at each station in Everett
Harbor were compared with mean values of variables across all three stations
in Port Susan. Pooling the Port Susan data increased the.number of replicate
reference values used in each statistical test from 5 to 15.
Comparisons of Benthic Communities in Everett Harbor and Port Susan
. Nineteen benthic stations were sampled as part of the Everett Harbor
study. Three stations were located in the Port Susan reference area, six
stations were located along the South Port Gardner shoreline, six stations
were located within the East Waterway, and two stations each were located in
the Snohomish River and delta areas. Species-level identifications were
available for all stations.
Infaunal Abundance--
A total of 62,419 individuals were collected among the 19 stations
sampled in 1986. Abundances varied among the different areas, but tended to
be higher in the East Waterway and in South Port Gardner. Total abundances
at the station in Port Susan were very similar to each other and ranged from
3,950 to 4,418/m2 (x=4,249/m2) (Figure 43). In contrast, total abundances
182
-------
25,000 -r-
C»
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10,000 --
5,000 --
-PREFERENCES
AREA
0
\
/
PS-02 PS-04 NG-02 NG-04 NG 10 EW-04 EW-10 EW-14 SD-02 SR-08
PS-03 NG-01 NG-03 NG-06 EW-01 EW-07 EW-12 SD-01 SR-07
STATIONS
Note: Numbers at lop of bars indicate numbers of significant depressions delected
in major laxa abundances relative to the Port Susan reference area.
Figure 43. Mean number of individuals/m2 at each benthic station in Everett Harbor and
Port Susan.
-------
at stations in Everett Harbor ranged from 300 to 20,676/m2 (x=7,005/m2).
Hence, total infaunal abundances at the stations in Everett Harbor were more
variable than total abundances at the stations in Port Susan.
Abundances of the major taxonomic groups were also highly variable in
Everett Harbor, compared with those in Port Susan (see Appendix F).
Polychaete abundances ranged from 1,002 to 2,152/m2 among the Port Susan
stations, and from 10 to 14,462/m2 among the Everett Harbor stations. Total
crustacean abundances ranged from 650 to 1,344/m2 among the Port Susan
stations, and from 16 to 10,644/m2 among the Everett Harbor stations.
Abundances of other major taxonomic groups (i.e. gastropods, pelecypods,
amphipods, other crustaceans, echinoderms and miscellaneous taxa) also
-showed similar high degrees of variability in Everett Harbor. Polychaetes
followed by pelecypods, total crustaceans, and crustaceans other than
amphipods were the most abundant major taxonomic groups in Port Susan,
whereas total crustaceans followed by polychaetes, other crustaceans, and
pelecypods were the most abundant major taxonomic groups among the Everett
Harbor stations (see Appendix F).' Gastropods and echinoderms were very minor
contributors (i.e., <5.0 percent) to species richness and abundance at most
stations.
Statistical analyses of infaunal abundances were conducted during this
study to determine whether any of the differences in abundances (i.e.,
enhancements or depressions) between the Port Susan reference stations and
stations in Everett Harbor were significant. Results of the t-tests are
summarized in Table 26. The relative degree of impact at each test station
was estimated by ranking stations according to the number of significant
depressions in the abundances of the following major taxonomic groups:
polychaetes, total crustaceans, pelecypods and gastropods. (For a discussion
of the statistical rationale, see Indices for Decision Criteria below).
Among the 64 paired comparisons that were performed (i.e., 16 stations times
4 major taxonomic groups), 28 comparisons were not statistically significant,
18 comparisons indicated enhanced abundances, and 18 indicated depressed
abundances (Table 26). In comparisons with the reference area, polychaetes
and pelecypods in Everett Harbor most frequently exhibited depressed
abundances, whereas total Crustacea in Everett Harbor most often exhibited
184
-------
TABLE 26. RESULTS OF PAIRWISE COMPARISON FOR
ABUNDANCE OF MAJOR TAXA BETWEEN THE PORT SUSAN
AND EVERETT HARBOR STATIONS*
Station
NG-01
NG-02
NG-03
NG-04
NG-06
NG-10
EW-01
EW-04
EW-07
EW-10
EW-12
EW-14
SD-01 '
SD-02
SR-07
SR-08
Total
Abundance
NSf
_d
+e
NS
+
NS
NS
+
_
NS
NS
NS
NS
_
NS
Polychaetesb
NS
-
-
-
NS
+
_
+
_
+
NS
NS
_
NS
_
NS
Pelecypods^
NS
NS
+
+
+
+
_
-
-
-
NS
-
_
NS
_
-
Gastropods
NS
NS
+
+
+
+
NS
-
NS
+
NS
NS
NS
NS
NS
Total
Crustaceans'*
NS
NS
+
+
+
+
NS
NS
NS
NS
+
NS
NS
+
_
NS
a Significance level for a single comparison of either depressions or enhancements
P<0.001.
b Used as index for decision criteria.
c NS = Not significant at P<0.001.
d - = Abundance significantly depressed.
e + = Abundance significantly enhanced.
185
-------
elevated abundances. Two stations in the East Waterway (i.e., EW-01 and
EW-07), Station SD-01 near the mouth of Ebey Slough, and Station SR-07 in the
Snohomish River exhibited the greatest number of depressions (two or three
out of four) in abundances of the major taxonomic groups. Four stations in
South Port Gardner exhibited significant (P<0.001) elevations in the
abundances of three or four major taxonomic groups (i.e., Stations NG-03,
NG-04, NG-06, and NG-10).
Numbers of Taxa--
A total of 403 taxa were collected among the 19 stations sampled in
Everett Harbor and Port Susan. Mean numbers of taxa per 0.1-m^ grab sample
varied considerably among those stations (Figure 44). At stations in Port
Susan, mean numbers of species per grab varied from 47 to 63, and averaged
55.6. In Everett Harbor, mean numbers of species per station varied from 4
to 96. The highest mean numbers of species occurred in South Port Gardner
at Stations NG-06 and NG-10 (96 and 81, respectively). The lowest mean
numbers of species occurred in the East Waterway at Stations EW-01, EW-04
and EW-07 (4, 16 and 16, respectively), at Station SD-01 in the Snohomish
River Delta (9) and in the Snohomish River at SR-07 (16). Two or three
significant depressions of major taxa abundance occurred at each of the
stations that exhibited low numbers of species, with the exception of
Station EW-04 where only the abundance of pelecypods was depressed. The
remaining nine stations in Everett Harbor (i.e., Stations NG-01, NG-02,
NG-03, NG-04, EW-10, EW-12, EW-14, SD-02, and SR-08) exhibited mean numbers
of species that were similar to those observed in Port Susan: 31-60 species
per grab sample (Figure 44). One or no significant depressions in major
taxa abundances occurred at each of these stations.
Numerically Abundant Taxa--
Relative and absolute abundances of the five numerically dominant taxa
at each station are summarized in Appendix G. Among the Port Susan stations,
abundances and relative abundances of the dominant taxa were fairly consis-
tent. They ranged from 2,130 to 3,002/m2 and from 53.9 to 67.9 percent of
the fauna, respectively. Species composition of the dominant taxa among
186
-------
00
X
U_Z
00
«.H
DOC
2S!
Z
<
LJJ
100
90
80
70
60
50
40
30
20
10
0
REFERENCED
AREA
PS-02 PS-04 HG-Q2 NQ-04 NQ-10 EW-04 EW-10 EW-14 SD-02 SR-08
PS-03 NG-01 NQ-03 NG-06 EW-01 EW-07 EW-12 SD-01 SR-07
STATIONS
Nole: Numbers at top of bars indicate numbers of significant depressions delected
in major laxa abundances relative to the Port Susan reference area.
Figure 44. Mean numbers of benthic taxa (no./0.1 m2,) at stations in Everett Harbor and
Port Susan (1996).
-------
these stations was also similar. Each station had at least two, and as many
as four taxa in common with each of the other stations. Moreover, at no
station did a single taxon dominate the community, to the exclusion or near
exclusion of other taxa.
Among the Everett Harbor stations, relative abundances of the dominant
taxa ranged from 44 to 99 percent of total infaunal abundances. At 8 of the
16 stations (i.e., Stations NG-01, NG-02, NG-03, EW-01, EW-04, EW-10, EW-12,
and SD-01) the five numerically dominant taxa represented over 70 percent of
the total abundance at each station (Figure 45). High relative abundances
of dominant taxa often indicate stressed conditions. As less tolerant
species are eliminated from the habitat, opportunistic species fill the
vacant niches, often achieving high abundances (Pearson and Rosenberg 1978;
Gray 1982).
Numerically dominant taxa averaged 2,567 individuals/m^ among the Port
Susan stations. Abundances of the numerically dominant taxa at most Everett
Harbor stations were greater"than this average, and abundances at Stations
NG-03, NG-06,-. NG-10, EW-04-, EW-10, and .EW-12 greatly exceeded this value
(Figure 45). These stations also exhibited significant enhancements for
total infaunal abundance and several major taxonomic groups including
pelecypods, gastropods, and total crustaceans. Abundances of amphipods (as
a subgroup of crustaceans) were also enhanced significantly.
Abundances of the numerically dominant taxa were greatly depressed
below the corresponding Port Susan value at Stations EW-01, EW-07, SD-01 and
SR-07. Total abundance per station ranged from 300 to 1,162 individuals/m2-
Greatly depressed abundances often indicate excessively enriched sediments
or the presence of toxic contaminants or both (see Pearson and Rosenberg
1978; Carriker et al. 1982; Wolfe et al. 1982; Dillon 1984; Bilyard 1987).
These four stations exhibited the highest number of significant depressions
among the Everett Harbor stations, with three or four depressions occurring
at each station.
Swartz's Dominance Index (SDI) can be used as one indicator of stressed
conditions due to organic enrichment. The index is defined as the number of
188
-------
CO
Ui
<
z
<
HI
o
oc
HI
D.
100
90
80
70
60
50
40
30
20
10
0
REFERENCE*-1
AREA I 1
1%
//
1 0
7
/,
0
y/
PS-02 ' PS-04 NG-02 NG-04 NG-10 ' EW 04 EW-10 EW-14 SD-02
PS-03 NG-01 NG-03 NG-06 EW-01 EW-07 EW-12 SD-01
STATIONS
Note: Numbers al lop at bars indicate numbers ol significant depressions delected
in major taxa abundances relative to the Port Susan reference area.
SR-08
Figure 45. Relative abundances of the five numerically dominant taxa (as percent of total
fauna) at stations in Everett Harbor and Port Susan (1986).
-------
dominant taxa that account for 75 percent of the total abundance. A low
index value results when a few taxa contribute most of the individuals in
the assemblage. A high index value results from a highly diverse population
wherein a limited number of taxa do not dominate the assemblage. SDI
appears to be less indicative of contamination by toxic substances or
physically stressed conditions in the benthic environment. Under those
conditions, abundances are often depressed, but the diversity of the
community is less disrupted. Under conditions of physical stress or
contamination of the sediments by toxic substances, both common and rare
species often exhibit reduced abundances, a condition that tends to maintain
the species distribution to a greater degree than under conditions of
organic enrichment (see Bilyard 1987). Under these conditions, a higher
index value may be calculated, even though the community is stressed.
Values of SDI ranged from 7.4 to 11.8 among the Port Susan stations
(x=10.1). In Everett Harbor, index values suggested that moderate stress
may be occurring at Stations NG-01, NG-02, NG-03, EW-12, and SD-01 (SDI=5.5,
4.2, 3.0, 5.9, and 4.4, respective-ly). Values of SDI indicated that
Stations EW-01, EW-04; and EW-10 were highly stressed (SDI=1.5, 1.3,' and 2.1
respectively). However, index values did not reflect the greatly depressed
abundances that occurred at Stations EW-07, SD-01, and SR-07, and that may
be indicative of toxic contamination or great physical stress. The SDI
values for all Everett Harbor and Port Susan stations are summarized in
Figure 46.
An analysis of species composition at each of the Everett Harbor
stations provided further information regarding impacted areas. Taxonomic
composition of the dominant species differed considerably within Everett
Harbor (see Appendix G). For example, nematodes, Capitella capitata. and
the crustacean Nebalia spp. were among the dominant taxa at the stations in
East Waterway. No other station in Everett Harbor or Port Susan exhibited a
similar group of numerically dominant taxa. Sub-surface deposit-feeding
nematodes and capitellid polychaetes are known to reach very high abundances
in organically enriched sediments, often to the exclusion of other taxa
(Nichols 1977; Pearson and Rosenberg 1978; Van Es et al. 1980). Nebalia spp.
are not considered classic indicators of organic pollution, yet they are
190
-------
<
X
<
DC
LU
ffi
18
16
14
12
10
8
6
4
2 4-
: REFERENCE*-
AREA
-------
found at high abundances at many East Waterway stations. Field observations
made during other benthic surveys in central Puget Sound found that Nebalia
spp. only achieves high abundances where wood chips or fibers contribute to
composition of the sediment (Word, J.Q., 8 April 1988, personal communica-
tion). Field observations made during this study confirmed the association
of Nebalia spp. with wood chips. Station SR-07 was dominated by Tharvx spp.
and several species of capitellid polychaetes (Heteromastus filibranchus and
Barantolla americana). Tharvx spp. is a surface deposit-feeding polychaete
(Fauchald and Jumars 1979) that was numerically dominant in many of the
benthic communities in contaminated areas of Elliott Bay and Commencement
Bay, and may be indicative of stressed conditions (Tetra Tech 1985a). In
summary, the identities of the dominant taxa and the low total abundances
observed at Stations EW-01, EW-07, and SR-07 suggest that the sediments at
these stations are highly organically enriched, contaminated with toxins, or
both.
Total abundance was also depressed at Station SD-01, but two crustaceans
contributed greatly to the total abundance (i.e., Archaeomvsis grebnitzkii
and Grandifoxus qrandis). It is reasonable to assume that these two species
of crustaceans are pollution-sensitive. Species closely related to each,
are either known to be pollution-sensitive, or are used as test organisms in
water and sediment toxicity bioassays tests. Thus, species composition of
the numerically dominant taxa indicates that some effect other than organic
enrichment or toxic contamination contributed to the low total abundance
recorded at this station. Field observations suggest that swift currents
may cause great physical stress at this station.
Relative abundances of opportunistic and pollution-tolerant taxa (as
defined by Word et al. 1977; Pearson and Rosenberg 1978; Word 1980) at the
16 Everett Harbor stations and the three Port Susan stations further support
the conclusion that benthic infaunal communities at many East Waterway and
some other Everett Harbor stations are stressed. Among the Port Susan
stations, relative abundances of opportunistic and pollution-tolerant taxa
averaged 28.2 percent of the total fauna. The ostracods Euphilomedes
carcharodonta and E. producta constituted the largest proportions of the
opportunistic and pollution-tolerant taxa at these stations. Euphilomedes
192
-------
spp: are known to increase in abundance in areas where only slight to
moderate organic enrichment of the ecosystem is occurring (Word et al.
1977). Within Everett Harbor, 9 of the 16 stations exhibited relative
abundances of opportunistic and pollution-tolerant taxa that were higher
than those at any of the Port Susan stations (Figure 47, see also Appen-
dix H). Relative abundances of those taxa within Everett Harbor ranged from
40.8 to 98.2 percent of the total fauna. Stations EW-01, EW-04, and EW-10
exhibited the highest relative abundances of opportunistic and pollution-
tolerant taxa, ranging from 88.9 to 98.2 percent. Two of these stations
(i.e., Stations EW-01 and EW-07) also exhibited the greatest number of sig-
nificant depressions in the abundances of the major taxonomic groups.
Moreover, Capitella capitata contributed the largest proportion of oppor-
tunistic and pollution-tolerant taxa at all three stations. C. capitata is
a known indicator of organically enriched conditions, and is often the only
species found in highly stressed, organically enriched areas.
Relative abundances of opportunistic and pollution-tolerant species at
Stations NG-03, NG-04, NG-06, NG-10 in South Port Gardner, EW-12 in the East
Waterway, SD-01 and SR-08 in the Snohomish Delta and River ranged from 9.4
to 33.0 percent, and did not exceed the relative abundances of those taxa
observed at the Port Susan stations. The most common opportunistic or
pollution-tolerant species at these stations was Euphilomedes carcharodonta.
which was also relatively abundant at the Port Susan stations.
Classification Analyses
Similarities between station pairs and groups of stations based on the
Bray-Curtis Similarity Index and normal classification analysis are shown in
Figure 48. Station groups were determined by selecting a 35 percent
similarity value. This level of similarity separated the stations into
three interpretable groups with two outliers.
Group 1 included all three Port Susan stations, five South Port Gardner
stations (i.e., Stations NG-01, NG-02, NG-03, NG-04 and NG-06), and one
Snohomish River Delta station, Station SD-02. Results of the normal
classification analysis indicated a high degree of similarity among the
193
-------
UD
UL
UL
O
UJ
o
-------
z
100
r~
PS-03
PS-04
PS-02
NG-01
SD-02
NG-06
NG-03
NG-04
NG-02
EW-12
SR-08
EW-14
NG-10
SR-07
EW-04
EW-10
EW-07
EW-01
SD-01
-I
- O
-El
- O
90
T
80
70
SIMILARITY (Percent)
60 50 40
30
nr
20
r~
10
NOTE: Station groups delineated by a similarity level of 35 percent are enumerated. Outliers are designated as "O"
Figure 48. Results of a Q-mode classification analysis (Bray-Curtis similarity index, group
average clustering strategy) using log-transformed [log(x+1)] abundances of
the benthic infauna at stations in Everett Harbor and Port Susan (1986).
-------
three Port Susan stations (56 percent). All other members of this group
clustered at least 50 percent similarity. Stations PS-03 and PS-04 were
very similar to one another, probably due to the similar abundances of
Euphilomedes carcharodonta. Pseohidia lordi. E. oroducta. and Pectinaria
oranulata that occurred at each station. These taxa were also among the five
most abundant species at Port Susan stations. Euphilomedes carcharodonta and
£. lordi were common to all nine stations in Group 1, and Axinoosida
serricata. E. producta. and £. oranulata were common to seven, four, and
three of the stations, respectively. Sediments at the Port Susan stations in
Group I ranged from coarse to fine sands. The five South Port Gardner
stations in Group I and Station SD-02 exhibited a similar range of grain
sizes as observed at the Port Susan stations. TOC content of the sediments
was low. among the Port Susan stations, ranging from 0.26 to 0.40 percent.
Sediments at the remaining stations in this group exhibited TOC contents
similar to those at the Port Susan stations (i.e., 0.18-0.54 percent).
Among the Everett Harbor stations in this group, all exhibited either no
significant depressions of major taxa abundance, or only one significant
depression in the abundance of polychaetes (see Table 26).-
Group 2 included Station NG-10 from South Port Gardner, Stations EW-12
EW-14 from the East Waterway, and Station SR-08. Between-station similari-
ties ranged from 41 to 45 percent (based on the similarity coefficient).
Fewer dominant taxa than Group 1 were common among the four stations.
Alvania spp. and Platvnereis bicanaliculata were both common at three
stations, and Leptochelia dubla was common at two stations. The sediments
at Stations EW-12 and SR-08 consisted primarily of medium to fine sands.
Stations NG-10 and EW-14 also exhibited sandy substrate but sediments at
those stations included 12 and 38 percent gravel or gravel sized particles
(i.e., woodchips), respectively. Total organic carbon content of the
sediments at the stations in Group 2 ranged from 0.71 to 4.66 percent. One
or no depressions in the abundances of the major taxonomic groups were
recorded at each station in this cluster. Both of the two recorded depres-
sions were for pelecypods.
Group 3 consisted of Stations EW-01, EW-04, EW-07 and EW-10. All four
stations were numerically dominated by Capitella capitata. nematodes and
196
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Nebalia spp. C. capitata and nematodes were the most abundant at Stations
EW-04 and EW-10. These stations clustered together with a fairly high
similarity coefficient (57 percent). Results of the t-tests documented
significant enhancements in abundances of polychaetes at both stations.
These same taxa were also dominant at Stations EW-01 and EW-07, but abun-
dances there were very low. Abundances of polychaetes, pelecypods and
gastropods were significantly depressed at Stations EW-01 and EW-07.
Sediment characteristics were similar among all four stations. Percent
fines (silt and clay) ranged from 56 to 79 percent. Most importantly, TOC
content of the sediments was elevated at all four stations, and ranged from
8.7 to 29.4 percent. The highest TOC value occurred at Station EW-04, which
also exhibited the highest total abundance (i.e., 20,676/m2) among the
Everett Harbor and Port Susan stations sampled in 1986.
Stations SD-01 and SR-07 were both outliers in the classification
analysis. Low total abundances were recorded at both stations, and both
exhibited significant depressions in the abundances of polychaetes and
pelecypods1. Total crustacean abundances were also depressed at Station
SR-07. Archaeomvsis qrebnitzkii and Grandifoxus orandis were the most
common species at Station SD-01. Species composition at this station was the
least similar of all the Everett Harbor stations. The hydrographic regime at
this station (i.e., high currents) probably contributed to this unique
species composition. Station SR-07 was numerically dominated by Tharvx spp.,
Macoma nasuta. M. carlottensis. and Heteromastus filibranchus. These species
are opportunistic or pollution-tolerant, and are often numerically dominant
in areas where sediments are organically enriched, or where other stresses
favor opportunistic species. The sediments at Station SD-01 were coarse
sand with some gravel. Sediment TOC content was low (i.e., 0.24 percent)
and comparable to that in Port Susan and at other Everett Harbor stations.
The sediments at Station SR-07 were primarily clayey silts (percent fines =
95.4 percent). This sediment type was found at no other station in Everett
Harbor. Sediment TOC content was 3.2 percent, a value slightly higher than
most sediments throughout Puget Sound.
197
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Comparison of .Species and Ma.ior Taxa Level Analyses
Species-level data provided detailed information about benthic com-
munities at each test station in Everett Harbor. In most cases, the species
data identified the same problem areas as did the statistical comparisons
using abundances of major taxonomic groups. Pairwise statistical comparisons
of the abundances of major taxonomic groups identified Stations EW-01,
EW-07, SD-01 and SR-07 as potential problem areas. Each of these stations
exhibited three or four depressions in total abundances or the abundances of
the four major taxonomic groups (see Table 26). However, examination of the
species composition at Station SD-01 suggested that this station exhibited
depressed abundances due to effects other than organic enrichment or
contamination of the sediments by toxic substances. Although total abundance
at Station SD-01 was the lowest observed in Everett Harbor, this station was
dominated by two crustaceans that belong to families that are known to be
highly sensitive to pollutants (i.e., phoxocephalid amphipods and mysids).
Other members of these two families are used as experimental animals in
water and sediment toxicity bioassays. Field observations suggested that
this station experiences swift currents that cause extreme physical stress
on the benthic.community.
Further examination of benthic community indices that use species-level
data indicated that in addition to Stations EW-01 and EW-07, Stations EW-04
and EW-10 in the East Waterway were also experiencing stress due to organic
enrichment. The species composition at these two stations were very similar
to those at Stations EW-01 and EW-07. All four of these stations were
dominated by opportunistic or pollution-tolerant taxa (i.e., nematodes,
Capitella caoitata. and Nebalia spp.) The sediments at Stations EW-04 and
EW-10 contained the highest concentrations of sulfides and total organic
carbon measured at any Everett Harbor station. The benthic communities at
these stations exhibit the classic response to high organic enrichment [as
defined by Pearson and Rosenberg (1978)] wherein opportunistic species become
very abundant and dominate the benthic community (Figure 49). Between
station statistical comparisons of the abundances of the major taxonomic
groups were unable to detect a potential problem at these stations because
abundances of the numerically dominant taxa were extremely elevated. Only
198
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-~ s
Increasing Organic Input
S = Species numbers
A = Total abundance
B = Total biomass
PO = Peak of opportunists
E = Ecotone point
TR = Transition zone
Reference: Pearson & Rosenberg (1978).
Figure 49. Generalized diagram of changes in species, abundance,
and biomass along a gradient of organic enrichment.
199
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pelecypods exhibited significant depressions in abundance at these stations
(see Table 26).
In general, crustaceans as a group did not display the sensitivity to
pollutant stress that has been observed in other Puget Sound embayments.
Examination of the species data suggested that this phenomena may have been
due (in part) to the abundance of a group of amphipods (Aoroides spp.) that
appear to be tolerant of, or enhanced by, organic enrichment. This group of
amphipods was present at 13 of the 19 stations sampled in Everett Harbor and
Port Susan and was among the dominant taxa at Stations EW-04, EW-07, EW-10
and EW-14. These four stations were characterized by fine-grained sediments
(percent fines ranged from 32.3 to 77.1 percent), elevated sediment sulfide
concentrations (700-7,610 ppm) and elevated sediment TOC content (4.7-29.4
percent). An additional dampening effect to the responsiveness of crusta-
ceans to environmental contamination was created by the presence Euphilomedes
spp. Euphilomedes carcharodonta was dominant at 11 of the 19 stations
sampled and was often the most abundant taxon.
Indices for Decision Criteria
Concentrations of toxic substances in the sediments may cause reductions
in the abundances of sensitive taxa (Wolfe et al. 1982; Rygg 1985, 1986) or
all taxa (Bilyard 1987). An extreme degree of organic enrichment may also
result in the loss of infaunal species (Pearson and Rosenberg 1978). In
this study, the locations and magnitudes of impacts were determined by the
results of the comparisons of major taxa abundance between Port Susan and
Everett Harbor stations discussed earlier (see Table 26). Species level data
were used to infer whether the presence of organic materials, toxic sub-
stances, or possibly other effects were causing the observed depressions in
taxonomic abundance.
The relative degree of impact at each test station was estimated by
ranking stations according to the number of statistically significant
depressions in the abundances of Polychaeta, Crustacea, Pelecypoda, and
Gastropoda. The major taxonomic groups comprise many different species with
varying degree of sensitivities to organic enrichment and toxic chemicals.
200
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In general, pelecypods and crustaceans appear to be fairly sensitive to
stressed conditions, and tend to exhibit reduced abundances. Because of
this sensitivity, they tend to be good indicators of stressed conditions at
the major taxonomic level. In contrast, polychaetes tend to have species
that are both sensitive and tolerant to these inputs. Because of this
variability, polychaetes often provide less useful information at the major
taxonomic level. Moreover, total infaunal abundance often mirrors polychaete
abundance because polychaetes are often the most abundant group, and may
account for greater than 50 percent of the total abundance.
The aforementioned pattern of sensitivity among the major taxonomic
groups has been observed in several Puget Sound urban embayments, including
Elliott Bay (PTI and Tetra Tech 1988) and Commencement Bay (Tetra Tech
1985a). However, in Everett Harbor the major taxonomic groups did not
always exhibit typical responses. Hence, analyses of the abundances of the
major taxonomic groups did not always provide complete indications of the
factors to which the benthic communities were responding.
Using the statistically-detected differences in the abundances of the
major taxonomic groups, Stations EW-01, EW-07, SD-01 and SR-07 appeared to
be the most impacted: two or three depressions were recorded at each of
these stations (Figure 50). Abundances of all major taxonomic groups at
these four stations were depressed 70 to 100 percent when compared with
abundances at Port Susan. East Waterway Stations EW-01 and EW-07 were
dominated by nematodes and Caoitella capitata. both of which are opportunis-
tic or pollution-tolerant taxa. These stations may be responding to extreme
organic enrichment, sediment contamination by toxic substances or both. It
is difficult to attribute causality to these effects because high levels of
organics in the sediments and toxic substances can cause large depressions
in infaunal abundances. However, examination of the benthic communities at
nearby Stations EW-04 and EW-10 showed extremely elevated populations of the
same species. Sediments at these four East Waterway stations were charac-
terized by fine grained sediments (percent fines ranged from 56.4 to 78.8),
elevated levels of total organic carbon (6.0 to 29.4 percent), and very high
concentrations of total sulfides (1,200 to 7,610 ppm). Based on these data
it appears that these four stations were responding to organic enrichment
201
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EW-041 I
EW-07
EW-10C~I
I IEW-12<
I IEW-U
NG-04f_J
« JJ&sf* 'v NG-06II
NG-101 I
I I 0 SIGNIFICANT DEPRESSIONS
I I 1 SIGNIFICANT DEPRESSION
2 SIGNIFICANT DEPRESSIONS
3 SIGNIFICANT DEPRESSIONS
4 SIGNIFICANT DEPRESSIONS
Figure 50. Summary of spatial patterns of significant (P < 0.001)
benthic depressions among the Everett Harbor stations
202
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[as described by Pearson and Rosenberg (1978)]. Stations EW-01 and EW-07 may
have been beyond the "peak of opportunists," and therefore exhibited highly
depressed abundances. At Stations EW-04 and EW-10, opportunistic species
are still dominant but may not have gone past the "peak of opportunists."
Exclusive use of the abundances of the major taxonomic groups was able to
detect only two of the four stations in the East Waterway where communities
were stressed.
Abundances of the major taxonomic groups also identified Station SR-07
as a potential problem site. Species composition at this station differed
greatly from that at most other Everett Harbor stations. Station SR-07 was
also characterized by the finest-grained sediments observed in Everett
Harbor (fines = 95.4 percent), elevated total sulfides in the sediments
(600 ppm), and a slightly elevated concentration of total organic carbon
(3.24 percent). Species data indicated that the community at this site was
dominated by two capitellid polychaetes (Heteromastus filibranchus and
Barantolla americana), two species of the bivalve Macoma (M. carlottensis and
M. nasuta) and the cirratu-lid polychaete Tharvx spp. Several of'these taxa
have been defined as pollution-tolerant or opportunistic (Word et -al..!977;
Pearson and Rosenberg 1978; Word 1980) which would support the interpreta-
tion that the benthic community at this station is experiencing some degree
of pollutant stress. However, data are insufficient (i.e., there are no
other nearby benthic stations) to interpret whether or not the observed
stresses are due to organic enrichment, toxic substances, or both.
Station SD-01 also exhibited a high number of depressions in the abun-
dances of the major taxonomic groups. The physical characteristics of this
station consisted of sandy sediments (with 12 percent gravel present), low
total organic carbon content, low sulfide, and swift currents. The species
composition at this station was the least similar to all other stations
sampled. It was dominated by the mysid Archaeomvsis qrebnitzkii and the
phoxocephalid amphipod Grandifoxus qrandis. A few pollution-tolerant or
opportunistic taxa were present (16.7 percent). These data contradict the
identification of this site as a potential problem area. As discussed
earlier this community may be stressed by physical factors.
203
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No other station in Everett Harbor was identified as a potential problem
area using depressed abundances of the major taxonomic groups as the decision
criteria. All other stations (i.e., Stations NG-01, NG-02, NG-03, NG-04,
NG-06, NG-10, EW-12, EW-14, SD-02 and SR-08) exhibited only one or no
depressions. Sediment characteristics (i.e., grain size, TOO, sulfides) at
the majority .of these remaining stations were very similar to Port Susan
sediments. Species composition at each of these stations was also very
similar to Port Susan, with Euphilomedes carcharodonta. Axinopsida serri-
cata. and Psephidia lordi being the dominant taxa at 50-80 percent of these
remaining stations.
Comparison with Recent Historical Data
Historical data collected during 1984 and 1985 during the Navy Homeport
Study (Parametrix 1985; U.S. Army COE 1985) were reviewed and compared with
the results of this study. In 1984, nine stations were sampled in the
nearshore areas of Everett Harbor, the East Waterway and the Snohomish
River. This study was conducted in the summer of 1984, and the majority of
the stations were located in East Waterway. The 1985 study occurred in the
winter and sampled seven stations located adjacent to the East Waterway, and
in the lower Snohomish River and delta. The laboratory processing methods
used in this later study were not comparable to standard benthic sample
processing techniques (e.g. use of 1.0-mm screen) and tended to underestimate
species richness and abundance of the benthic assemblages.
Historical data tended to identify problem areas similar to those found
in this study. Total abundances at the historical stations sampled in the
East Waterway ranged from 52 to 5,203 individuals per station and mean
number of taxa collected there ranged from 1.8 to 21.4. The benthic
community was dominated by Capitella capitata. nematodes, and Nebalia
puqettensis. In some areas within the East Waterway in 1984, these species
accounted for 100 percent of the organisms collected. SDI calculated for
these stations reflected these highly dominated assemblages: most values
were less than 1.0. Reference areas were not sampled as part of these
historical studies so no statistical comparisons of the abundances of the
major taxonomic groups could be made. However, examination of the data
204
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showed that molluscs, total Crustacea, and amphipods were either absent, or
occurred at very low abundances at many of these stations.
Additional historical stations adjacent to the mouth of East Waterway
were also sampled during the 1984 and 1985 studies. Mean numbers of taxa at
those stations ranged from 31.6 to 69 per station. Total abundance was also
higher at those stations than at stations in the East Waterway, and ranged
from 2,496 to 9,676 individuals/m2. SDI was less than 5.0 at all stations.
Communities were dominated by many of the same taxa as in East Waterway, but
included Euohilomedes carcharodonta.
Values of various.benthic community indices that were calculated using
historical data from the three stations in the -Snohomish River initially
suggested a potential problem in the lower river where the channelization of
the river mouth begins. Numbers of taxa and total abundances were low at
two stations (mean nos. of taxa were 7 and 7; total abundances were 265 and
556), and values of SDI were low (1.80 and 2.85). However, the numerically
.dominant taxa at these stations were not indicative of a high degree of
stress rel-ated to organic enrichment or the presence of toxic substances in
the sediments. Insufficient data are available to determine whether the
benthic community in this area was responding to some type of physical
stress.
Numbers of taxa and total abundances recorded at three historical
stations sampled within the river delta were slightly higher than in samples
from the river channel. Mean numbers of taxa ranged from 13.8 to 20 per
station, and total abundance ranged from 374 to 1,299 individuals/m2.
Values of SDI ranged from 3.44 to 4.17. In most cases, these values of the
SDI would suggest that the possibility of stresses to the benthic community
be explored.
Summary
Eighteen significant (P<0.001) depressions in abundances were
detected among 64 statistical comparisons of four major
taxonomic groups at 16 benthic stations in Everett Harbor.
205
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Significantly enhanced abundances were detected in 18 eases,
and no significant differences were found in 28 comparisons.
Five stations in Everett Harbor exhibited no depressions in
the abundances of the four major taxa selected for problem
identification (polychaetes, pelecypods, gastropods and total
crustaceans). Seven stations exhibited one depression, one
station exhibited two depressions, and three stations
exhib-ited three depressions.
The most impacted stations in Everett Harbor were Stations
EW-01, EW-07 (East Waterway), SD-01 (Snohomish River Delta),
and SR-07 (Snohomish River) based on depressions detected in
major taxonomic abundance. Species level data also identi-
fied East Waterway Stations EW-04 and EW-10 as being greatly
impacted.
The lowest number of taxa occurred at Stations EW-01, EW-04,
EW-07, SD-01, and SR-07, all of which exhibited three sig-
nificant (P<0.001) depressions in the abundances of the major
taxonomic groups, with the exception of Station SD-01, where
polychaetes and pelecypods were depressed, and Station EW-04,
where only pelecypods were depressed. Station EW-04 was also
characterized by the highest total abundance of benthic
infauna observed in Everett Harbor in 1986.
Species compositions of the benthic communities at the East
Waterway stations was very similar. Several dominant taxa
were common to those stations. This area had the greatest
number of stations that exhibited significant depressions in
abundances of the major taxonomic groups. Many of the
numerically dominant taxa present at the South Port Gardner
Stations SD-02 and SR-08 were also numerically dominant in
Port Susan. Only one group or no groups exhibited depressed
abundances at Stations SD-02, SR-08, or any of the stations
in South Port Gardner.
206
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Station groups that resulted from the classification analysis
tended to confirm the identification of potential problem
areas based on both the depressed abundances of the major
taxonomic groups and on species composition. Stations EW-01,
EW-04, EW-07, and EW-10 were included in one group, Stations
EW-12, EW-14, NG-10, and SR-08 were included in a second
group, Stations PS-02, PS-03, PS-04, NG-01, NG-02, NG-03, NG-
04, NG-06, and SD-02 'were included in a third group, and
Stations SR-07 and SD-01 were outliers.
FISH ECOLOGY
This section provides a description of the general characteristics of
the demersal fish assemblages and English sole populations sampled at the 10
*
transects in Everett Harbor and the single transect in Port Susan (see
Figure 6). Demersal fish assemblages are compared between Everett Harbor
and Port Susan with respect to species composition, total abundance, total
number of species, and diversity. English sole populations are compared
between the two areas with respect to abundance and relative abundance.
Demersal Fish Assemblages
Species Composition
A total of 6,373 fishes, representing 17 families and 38 species, was
sampled in this study (Table 27). Everett Harbor yielded 5,790 individuals
and 37 species, whereas 583 individuals and 21 species were captured at Port
Susan. Much of the observed difference in catches between the two study
areas likely resulted from the larger sampling effort expended in Everett
Harbor, but may also have been partly the result of increased habitat
complexity (e.g., pilings, rocks, debris) in Everett Harbor.
The most abundant family of fishes sampled in both Everett Harbor and
Port Susan was Pleuronectidae (62.6 and 48.3 percent, respectively). The
207
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TABLE 27. RELATIVE ABUNDANCES OF FISHES CAPTURED
IN EVERETT HARBOR AND PORT SUSAN
Fami 1 y
Squal idae
Chlmeridae
Clupeidae
Osmeridae
Batrachoididae
Gadidae
Zoarcidae
Gasterosteidae
Embiotocidae
Bathymasteridae
Stlchaeldae
Scorpaeni dae
Hexagramnidae
Cottldae
Agon idae
Both idae
Pleuronectidae
Relative Abundance (%)
Species
Saualus acanthi as
Hvdrolaaus colliei
Cluoea harengus oallasi
Hypomesus pretiosus
oretlosus
Porichthvs nota.tus
Gadus macrocephalus
Theraora chalcogramma
Microaadus proximus
Lvcodopsis pacifica
Aulorhvnchus flavidus
Cymatoqaster aqqreqata
Embiotoca lateral is
Rhacochi lus vacca
Ronauilus .iordani
Lumpenus saaitta
Sebastes caurinus
Hexaqrammos decaqraimus
Hexaqramnos stelleri
Oxvleblus oictus
Chitonotus puaetensis
Enophrvs bison
Leptocottus armatus
Mvoxocephalus
ool vacanthocephal us
Nautichthvs oculofasciatus
Rhamphocottus richardsoni
Scorpaeni chtnvs tnarmoratus
Aqonus acioenserinus
Citharichthvs sordidus
Citharichthvs stiqmaeus
Atheresthes stomias
Glvptocephalus zachirus
Hipppqlossoides elassodon
Lepidopsetta bi 1 i neata
Lvopsetta exi 1 is
Microstomus pacificus
Parophrvs vetulus
Platichthvs stellatus
Psettichthvs melanostictus
Common Name Everett Harbor Port Susan
spiny dogfish
ratfish
Pacific herring
surf smelt
plainfin midshipman
Pacific cod
walleye pollock
Pacific tomcod
blackball y eelpout
tube-snout
shiner perch
striped seaperch
pile perch
northern ronquil
snake prickleback
copper rockfish
kelp greenling"
whitespotted greenling
painted greenling
roughback sculpin
buffalo sculpin
Pacific staghorn sculpin
great sculpin
sailfin sculpin
grunt sculpin
cabezon
sturgeon poacher
Pacific sanddab
speckled sanddab
arrowtooth flounder
rex sole
flathead sole
rock sole
slender sole
Dover sole
English sole
starry flounder
sand sole
Total Catch
-------
most abundant pleuronectid in both areas was English sole (52.1 and 37.9
percent, respectively).
Assemblage Characteristics--
Demersal fish assemblages at individual transects in Everett Harbor
were compared qualitatively with the assemblage at Port Susan on the basis
of three major characteristics: total abundance, total number of species,
and diversity (Table 28). The latter variable was estimated using the
Shannon-Wiener index (H1) (Shannon and Weaver 1949).
Total abundance at 3 of the 10 Everett Harbor transects (i.e., EW-91,
SD-92, SD-94) exceeded the value at Port Susan (i.e., 16.2 individuals/100 m)
by a factor of 2 or greater. By contrast, total abundances at four Everett
Harbor transects (i.e., NG-91, NG-92, NG-93, NG-94) were lower than the
value at Port Susan by a factor of 2 or greater.
The total number of species at Everett Harbor transects (i.e./
range = 11-24) exceeded the value observed at Port Susan (i.e., 21) at one
transect (i.e., EW-92) and was lower than that value at the remaining nine
transects. The diversity at Everett Harbor transects (i.e., range = 1.06-2.12)
exceeded the value observ-ed at Port Susan (i.e., 1.98) at one transect
(i.e., EW-92) and was lower than that value at the remaining transects.
In summary, the total abundance of fish assemblages was substantially
reduced along most of the southern shoreline of Port Gardner relative to the
observed abundance in Port Susan. By contrast, total abundance of fish
assemblages was much higher in the East Waterway and throughout most of the
Snohomish Delta than the observed value in Port Susan. Throughout most of
the Everett Harbor study area, both the number of species and diversity of
fish assemblages were lower than the observed value in Port Susan. The only
exception to this pattern was found at the transect outside of the East
Waterway (i.e., EW-92). Although these comparisons are largely descriptive,
the general pattern of reduced numbers of species and diversity values
throughout most of the Everett Harbor study area suggest that fish assem-
blages may be negatively affected relative to the assemblage in Port Susan.
209
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TABLE 28. COMPARISONS OF MAJOR CHARACTERISTICS
OF FISH ASSEMBLAGES IN EVERETT HARBOR
AND PORT SUSAN
Transect
Port Susan
PS-91
Everett Harbor
NG-93
NG-92
NG-91
NG-94
EW-92
EW-91
SR-92
SD-91
SD-94
SD-92
Total
Abundance
(per 100 m)
16.2
6.3
5.6
5.4
2.0
15.5
34.0
12.6
20.2
39.8
67.9
Number
of Species
21
17
11
11
15
24
20
17
18
13
17
Diversity
(H1)
1.98
1.77
1.20
1.43
1.40
2.12
1.59
1.06
1.43
1.06
1.75
210
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However, the reasons for these potential negative effects are uncertain.
They could be related to chemical contamination or to other variables such
as low salinity, low habitat complexity, or reduced densities of prey
organisms.
English Sole Populations
The abundance of English sole at 3 of the 10 Everett Harbor transects
(i.e., EW-91, SD-91, SD-92) exceeded that at Port Susan (i.e., 6.1 indi-
viduals/100 m) "by a factor of 2 or greater (Table 29). By contrast, the
abundance of English sole at three transects (NG-91, NG-93, NG-94) was
lower than the value in Port Susan by a factor of 2 or greater. The
relative abundance of English sole at Everett Harbor transects (i.e.,
range = 25.8-63.5 percent) exceeded the value observed at Port Susan (i.e.,
37.9 percent) at all transects except Transect SD-94.
Summary
The most abundant fami.ly of fishes in both Everett Harbor and,
Port Susan was Pleuronectidae
The most abundant pleuronectid in both study areas was
English sole
The abundances of demersal fishes at four Everett Harbor
transects were substantially lower (i.e., <50 percent) than
the abundance at Port Susan
The total numbers of species and diversities of fish assem-
blages at most transects in Everett Harbor were lower than
the respective values at Port Susan.
FISH HISTOPATHOLOGY
This section presents the results of histopathological analyses
conducted on the livers of English sole collected at 10 trawl transects in
211
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TABLE 29. COMPARISONS OF ABUNDANCE AND RELATIVE
ABUNDANCE OF ENGLISH SOLE IN EVERETT HARBOR
AND PORT SUSAN
Transect
Port Susan
PS-91
Everett Harbor
NG-93
NG-92
NG-91
NG-94
EW-92
EW-91
SR-92
SD-91
SD-94
SD-92
Abundance
(per 100 m)
6.1
3.0
3.5
3.0
1.3
6.6
20.1
8.3
12.8
10.3
27.3
Relative
Abundance
(percent)
37.7
47.6
62.5
55.6
65.0
42.6
59.1
65.9
63.4
25.9
40.2
212
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Everett Harbor and at one transect in a reference area in Port Susan
(see Figure 6). Three major kinds of lesion were evaluated: neoplasms,
foci of cellular alteration, and megalocytic hepatosis (see Methods section).
Before the lesions are considered, the age and sex characteristics of the
English sole sample from each Everett Harbor transect are compared with the
respective characteristics of the sample from Port Susan. The overall
prevalences of the lesions in Everett Harbor and at Port Susan are then
presented, and the relationships between the prevalence of each lesion and
fish sex and .age are determined. Next, comparisons of lesion prevalences
between each Everett Harbor transect and Port Susan are made. Finally,
results of the present study are compared with historical information on the
prevalence of hepatic lesions in English sole from Everett Harbor.
Age and Sex Characteristics of Fish Populations
Ages of English sole at three transects in Everett Harbor differed
significantly (P<0.05) from ages of fish captured in Port Susan (Table 30).
In two cases (i.e., Transects NG-91 and NG-92), median fish age was greater
than that observed in Port Susan. At. Transect SR-92, median fish age was
less than that observed in Port Susan. Male proportion of English sole at
two transects in Everett Harbor (i.e., Transects NG-93 and EW-92) was
significantly (P<0.05) greater than the proportion in Port Susan (Table 30).
General Patterns of Lesion Prevalences
A total of 71 of the 594 (12.0 percent) English sole (age >3 yr)
sampled from Everett Harbor and Port Susan had one or more of the three
kinds of hepatic lesions considered in this study (Table 31). Of this
total, 56 (9.4 percent) had only a single kind of lesion, 13 (2.2 percent)
had two kinds of lesions, and 2 (0.3 percent) had all three kinds of lesions.
The prevalence of each kind of hepatic lesion evaluated in this study
was greater in Everett Harbor than in Port Susan (Table 31). In most cases,
the differences between these two areas were substantial. Foci of cellular
alteration was the lesion found most frequently in Everett Harbor and Port
213
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TABLE 30. COMPARISONS OF AGE AND MALE
PROPORTION BETWEEN ENGLISH SOLE FROM
EVERETT HARBOR AND PORT SUSAN
Transect
Port Susan
PS-91
Everett Harbor
NG-93
NG-92
NG-91
NG-94
EW-92
EW-91
SR-92
SD-91
SD-94
SD-92
Sample
Size3
56
56
60
58
57
55
49
41
58
51
53
Median
Age (yr)b
4.0
4.4 ns
5.6***
5^7***
4.6 ns
3.6 ns
3.3 ns
3.0*
3.8 ns
3.8 ns
3.1 ns
Male
Proportion0
0.18
0.45*
0.08 ns
0.10 ns
0.18 ns
0.47*
0.41 ns
0.44 ns
0.28 ns
0.20 ns
0.17 ns
a All fish were >3 years old.
b Comparisons were made using the Mann-Whitney U-test.
* = P<0.05; *** = P<0.001; ns = P>0.05.
c Comparisons were made using the G-test of independence.
* = P<0.05; ns = P>0.05.
214
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TABLE 31. PREVALENCES OF HEPATIC LESIONS
IN ENGLISH SOLE FROM EVERETT HARBOR
AND PORT SUSAN
Hepatic Lesion
Neoplasms
Liver cell adenoma
Hepatocellular carcinoma
One or more kinds of neoplasm^
Foci of celluar alteration
Eosinophilic foci
Basophilic foci
Clear cell foci
One or more kinds of foci of
cellular alteration"
Megalocytic hepatosis
One or more of the three major
kinds of hepatic lesion"
Everett Harbor
(n=538a)
1.9
0.7
2.4
7.6
3.0
2.2
10.8
2.4
12.5
Port Susan
(n=56a)
0
0
0
5.4
0
1.8
7.1
0
7.1
a All fish were >3 years old.
b Some fish had more than one kind of hepatic lesion.
215
-------
Susan (10.8 and 7.1 percent, respectively). Neoplasms and megalocytic
hepatosis were not found in Port Susan.
Within Everett Harbor, prevalences of neoplasms and foci of cellular
alteration were correlated positively (P<0.05) with increasing age of fish
(Figure 51). These patterns are consistent with the results of past studies
(Malins et al. 1982; McCain et al. 1982; Becker et al. 1987; Rhodes et al.
1987; PTI and Tetra Tech 1988). Prevalence of neoplasms increased from
0 percent in fish aged 2-5 yr old to 15.6 percent in fish aged >9 yr old.
Prevalence of foci of cellular alteration increased from 0 percent in 2-yr-
old fish to 40.6 percent in fish aged >9 yr old. Prevalence of megalocytic
hepatosis was not linearly correlated with fish age (PX1.05) (Figure 51),
which is consistent with results of past studies (Becker et al. 1987;. Rhodes
et al. 1987; PTI and Tetra Tech 1988). However, the prevalence of megalo-
cytic hepatosis peaked at an age of 6 yr, which corresponds to the trend
found by Tetra Tech (1985a) and PTI and Tetra Tech (1988).
The prevalence of megalocytic hepatosis exhibited a significant
difference (P<0.05) between sexes, whereas prevalences of neoplasms and foci
of cellular alteration did not differ significantly (P>0.05) between sexes
(Table 32). Past studies of English sole populations have reported the lack
of a difference in the prevalence of megalocytic hepatosis between sexes
(McCain et al. 1982; Malins et al. 1982; Krahn et al. 1986; Becker et al.
1987; Rhodes et al. 1987).
Comparisons of Lesion Prevalences Between Study Areas
Because prevalences of neoplasms and foci of cellular alteration in
Everett Harbor correlated with fish age (Figure 51), age distributions at
those transects that differed from Port Susan with respect to fish age
(i.e., NG-91, NG-92, and SR-92; Table 30) were adjusted before comparisons
with the reference area were made. Adjustments were made by sequentially
removing the youngest fish from Transect SR-92 and the oldest fish from
Transects NG-91 and NG-92 until each remaining age distribution did not
differ significantly (P>0.05) from the age distribution at Port Susan. In
making these adjustments, 4, 12, and 15 fish were removed from Transects
216
-------
Neoplasms
20 -]
15
10 -
5 -
rs=0.87**
(0) (0) (0) (0)
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FISH AGE (yr)
AGE
GROUP
2
3
4
5
6
7
8
>9
SAMPLE
SIZE
62
137
128
78
65
60
38
32
Figure 51. Comparisons of prevalences of hepatic lesions
with age of English sole from Everett Harbor using
Spearman's coefficient of rank correlation (rs).
**P<0.01, ns = P>0.05.
217
-------
TABLE 32. COMPARISONS OF LESION PREVALENCES BETWEEN MALE
AND FEMALE ENGLISH SOLE FROM EVERETT HARBOR
Percent having Each
Kind of Lesion3
Hepatic Lesion
Neoplasms
Foci of cellular alteration
Megalocytic hepatosis
Males
(n=145)
2.8
11.0
5.5
Females
(n=393)
2.3
10.7
1.3
Significance15
ns
ns
**
All fish were >3 years old.
Comparisons were made using the G-test of independence.
** = P<0.01; ns = P>0.05.
218
-------
SR-92, NG-91, and NG-92, respectively. A graphical comparison between the
age distribution at each Everett Harbor transect (including the three
adjusted distributions) and the age distribution at Port Susan is presented
in Figure 52.
Although prevalence of megalocytic hepatosis differed between sexes
(Table 32), the sex distributions at those transects that differed from Port
Susan with respect to male proportion were not adjusted before comparisons
with the reference area were made. Adjustments were not made primarily
because the relationship observed in this study is not consistent with
results of past studies of hepatic lesions in English sole (McCain et al.
1982; Mai ins et al. 1982; Becker et al. 1987; Rhodes et al. 1987). Thus,
the relationship observed in this study does not appear to be a general
pattern.
In most cases, prevalences of each kind of hepatic lesion at each
transect in Everett Harbor exceeded the corresponding value from Port Susan
(Table 33). Concordance among the prevalences of the three kinds of lesion
across all 11 transects was not significant (W=0.45, P>0.05).
Prevalence of neoplasms at the 10 Everett Harbor transects ranged from
0 to 8.8 percent, with the highest value observed at Transect NG-94. The
prevalence of neoplasms at each transect in Everett Harbor did not differ
significantly (P>0.001) from the prevalence of 0 percent observed at Port
Susan.
Prevalence of foci of cellular alteration at Everett Harbor transects
ranged from 0 to 21.1 percent, with the highest value observed at Transect
NG-94. The prevalence of this lesion at each transect in Everett Harbor did
not differ significantly (P>0.001) from the prevalence of 7.1 percent
observed at Port Susan.
Prevalence of megalocytic hepatosis at Everett Harbor transects ranged
from 0 to 14.3 percent, with the highest value observed at Transect EW-91.
The prevalence of megalocytic hepatosis at each transect in Everett Harbor
219
-------
50-
I
III
O
QC
UJ
o
z
UJ
3
O
UJ
DC
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40-
30-
20-
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30-
20-
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SO-i
40-
30-
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. 0
50-,
40-
30 -
20 -
10 -
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SO-i
40-
30-
20-
10-
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EW-91
n >49
EW-92
n.SS
NG-91
n.46
30-94
n-51
50-
40-
30-
20-
10-
0
50-
40-
30-
20-
10-
0
50-
40-
30-
20-
10-
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50-
40-
30-
20-
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0
50-
40-
30-
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NG-93
n-56
NG-94
n.57
30-91
n.SS
SR-92
n-37
34 56 7 8 >8
3 4 5 6 7 8 >8
FISH AGE (yr)
Figure 52. Comparisons of age distributions between Everett Harbor
(solid lines) and Port Susan (dashed lines) transects.
22.0
-------
TABLE 33. COMPARISONS OF PREVALENCES OF HEPATIC LESIONS
IN ENGLISH SOLE FROM EVERETT HARBOR AND PORT SUSAN
Prevalence (%)b
Transect
Port Susan
PS-91
Everett Harbor
NG-93
NG-92
NG-91
NG-94
EW-92
EW-91
SR-92
SD-91
SD-94
SD-92
Sample
Size3
56
56
45
46
57
55
49
37
58
51
53
Neoplasms
0
5.4 ns
0 ns
2.2 ns
8.8*
0 ns
2.0 ns
0 ns
1.7 ns
0 ns
1.9 ns
Foci of
Cellular
Alteration
7.1
17.9 ns
8.9 ns
10.9 ns
21.1*
0 ns
10.2 ns
8.1 ns
3.5 ns
13.7 ns
5.7 ns
Megalocytic
Hepatosis
0
5.4 ns
0 ns
0 ns
0 ns
1.8 ns
14.3**
2.7 ns
0 ns
0 ns
1.9 ns
One or
More
Lesions
7.1
21.4*
8.9 ns
13.0 ns
21.1*
1.8 ns
16.3 ns
8.1 ns
5.2 ns
13.7 ns
7.6 ns
a All fish were >3 years old, and the age distribution at each transect from
Everett Harbor does not differ significantly (P>0.05) from the age distribution
at Port Susan. Age distributions at Stations NG-91, NG-92, and SR-92 were adjusted
before statistical comparisons (see text).
Comparisons were made using the G-test of independence.
* = pn.ns.
221
-------
did not differ significantly (PXJ.001) from the prevalence of 0 percent
observed at Port Susan.
Prevalence of one or more of the three kinds of hepatic lesions at
Eyerett Harbor transects ranged from 1.8 to 21.4 percent, with the highest
value observed at Transect NG-93. The prevalence of one or more of the
three lesions at each transect in Everett Harbor did not differ significantly
(P>0.001) from the prevalence of 7.1 percent observed at Port Susan.
The spatial distributions of the three kinds of hepatic lesions are
presented in Figures 53-55. The highest prevalences of both neoplasms and
foci of cellular alteration were found off Pigeon Creek and the Mukilteo
Ferry Terminal. The highest prevalences of megalocytic hepatosis were found
in the East Waterway and off the Mukilteo Ferry Terminal. The spatial
distributions of the three kinds of hepatic lesion indicate that most
abnormalities were found near the Mukilteo Ferry Terminal and along the
shoreline in and near the East Waterway.
*
Comparison with Recent Historical Data-
Results of the present study were compared with those from surveys
conducted throughout Everett Harbor between 1979 and 1983 (Maiins, D.C.,
21 November 1984, personal communication; Mai ins et al. 1984, 1985,
unpublished). Comparisons were limited to descriptive evaluations because
different age distributions, of English sole were examined in the two studies
and because, in some cases, fish were collected at different locations and
during different seasons. In making these comparisons, prevalences were
averaged (if necessary) within five areas: the East Waterway (Transect
EW-91), the Everett Waterfront (Transects EW-92 and NG-94), the Mukilteo area
(Transect NG-93), the Snohomish River Delta (Transects SR-92 and SD-91), and
Port Susan (Transect PS-91).
In general, the relative spatial patterns of lesion prevalences in the
present study were similar to those found in earlier studies (Figure 56).
In most cases, the prevalences of all three kinds of hepatic lesion were
222
-------
LEGEND
I I 0%
1 - 5%
Figure 53. Spatial patterns of the prevalences of neoplasms in
Everett Harbor.
Z23
-------
Figure 54. Spatial patterns of the prevalences of foci of cellular
alterations in Everett Harbor.
224
-------
ZZ5
-------
PRESENTSTUDY
MALINSETAL (1984)
Neoplasms
8-
4-
QJ
P
Ort _,
O
PREVALENCE (PEF
t* tn »
o o o *». co ro
ii i i i i
30-
20-
10-
0-
R3
1 Hi n * (0) (o.
Foci of Cellular Alteration
Me
ga
I/////////
__
n
i 1 n B
i nt ni ,0,1
locytlc Hepatosis
1
EAST
WATERWAY
(86-49)
MUH
(6(
m n n (o (o,
EVERETT PORT
WATERFRONT SUSAN
(61-112) (33-56)
HLTEO SNOHOMISH
3-56) DELTA
(47-95)
LOCATION
NOTE: Sample sizes are shown in parentheses below location names.
Figure 56. Comparison of prevalences of hepatic lesions in English
sole sampled in the present study (stippled bars) and in
Malins et al. (1984) (open bars).
226
-------
higher along the shoreline between the East Waterway and Mukilteo than on
the Snohomish River Delta or in Port Susan.
The absolute prevalences of neoplasms and foci of cellular alteration
found in the present study were also similar to those found in earlier
studies. However, the absolute prevalences of megalocytic hepatosis
observed in the present study were considerably lower than the values found
by the earlier studies. Rhodes et al. (1987) found that prevalences of this
lesion exhibited significant interannual variation at eight sampling sites
throughout Puget Sound. By contrast, prevalences of neoplasms and foci of
cellular alteration did not exhibit significant interannual variation.
Rhodes et al. (1987) suggested that the increased temporal variability of
megalocytic hepatosis indicates that it may have different patterns of
pathogenesis and progression than neoplasms and foci of cellular alteration.
The similarity in the relative spatial patterns of lesion prevalences
between the present study and the studies conducted 3-7 yr earlier indicate
that these patterns are real (i.e., they are not artifacts of the design of
the various studies), and that they are relatively stable over time. The
temporal stability of these patterns suggests that the causes of the lesions
are localized primarily along the shoreline between the East Waterway and
Mukilteo, and that the causes have not been reduced substantially between
1979 and 1986.
Summary
Three kinds of hepatic lesion were considered in this study:
neoplasms, foci of cellular alteration, and megalocytic
hepatosis.
Prevalences of neoplasms and foci of cellular alteration were
correlated positively (P<0.05) with fish age.
Prevalence of megalocytic hepatosis was higher (P<0.05) in
males than in females.
227
-------
Prevalences of all three lesions at many of the 10 Everett
Harbor transects were substantially elevated above reference
values, but these differences were not statistically signifi-
cant at PO.001.
The spatial distributions of the three kinds of hepatic
lesions indicate that most abnormalities were confined to the
shoreline between the East Waterway and Mukilteo.
Results of the present study were compared with historical
data collected 3-7 yr earlier. The relative magnitudes of
lesion prevalences among areas were similar between studies.
The absolute magnitudes of lesion prevalences were similar
between studies for neoplasms and foci of cellular alteration.
However, prevalences of megalocytic hepatosis were consider-
ably lower in the present study than the values found in the
earlier studies.
228
-------
CONTAMINANT', TOXICITY, AND BIOLOGICAL EFFECTS RELATIONSHIPS
Quantitative relationships among the contaminant, toxicity, and
biological effects variables used in the Everett Harbor investigation are
examined in this section. The objectives of this section are to:
Determine potential correlations between sediment contamina-
tion and benthic infauna depressions or toxicity to amphipods
Compare amphipod bioassay mortality with effects on major
taxa of benthic infauna.
The Everett Harbor database, includes sediment chemistry and biological
information at sites displaying a wide range of sediment contaminant levels.
Therefore, the data were evaluated to detect correlations that may reflect
potentiaT cause-effect relationships. In this study, it was assumed that
contaminants whose distributions were associated with biological effects had
a higher potential for being causative agents than contaminants displaying
no discernible relationships. However, demonstration of actual cause-effect
relationships would require confirmation by laboratory toxicity experiments.
Such studies were beyond the present scope, but may prove useful to support
identification of toxic contamination problems in the future.
In a later section, the Puget Sound AET (Tetra Tech 1986c, 1987) are
used to identify problem stations based on sediment chemistry data from
previous studies where appropriate biological effects data were unavailable
(see Prioritization of Problem Areas and Contaminants). As part of an
ongoing EPA project, the contaminant-effects data from the Everett Harbor
investigation will be incorporated into the SEDQUAL database to derive
updated AET.
229
-------
RELATIONSHIPS AMONG CONTAMINANTS, TOXICITY, AND BENTHIC EFFECTS
This section examines the correspondence between the physical-chemical
characteristics of sediments and their toxicity to amphipods or observed
impacts on indigenous benthic infaunal taxa.
General Correlation of Indicators
Significant amphipod mortality relative to reference was found at four
of the 29 test sites in the Everett Harbor system (P<0.001; see Figure 40).
Significant benthic effects were observed at 11 of the 16 stations sampled
for benthic infauna (see Figure 50). In these analyses, benthic effects were
defined as a statistically significant (P<0.001) depression in at least one
of four major taxa (Polychaeta, Pelecypoda, Gastropoda, Crustacea) relative
to conditions at the Port Susan reference area.
Significant bioeffects were measured in at least one of the site-
specific biological tests at all four, stations where EAR exceeded 1,000 for
at least one problem chemical in sediments (Stations EW-04, EW-07, EW-10,
and EW-14 in Table 20). In other sediments where there were no significant
toxic responses and benthic effects (i.e., Stations NG-06, NG-10, and SD-02),
concentrations of organic compounds classified as problem chemicals were
generally low (EAR<30), but sometimes exceeded AET. For example, the
concentration of 4-methylphenol was 1,800 ug/kg DW (EAR=140), or 1.5 times
the HAET, at Station NG-10. EAR for problem metals at stations without
significant biological effects ranged up to only about three times reference
conditions (zinc at Station SD-02) and were always less than AET.
Examples of relations-hips between biological variables and physical/
chemical variables are shown in Figures 57-62. These figures were selected
from a complete set of scatterplots developed for the following variables:
Chemicals: LPAH, HPAH, naphthalene, phenol, 4-methylphenol,
pentachlorophenol, 2,4,6-trichlorophenol. 3,4,5-trichloro-
guaiacol, abietic acid, dehydroabietic acid, 12-chlorodehydro-
230
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of selected benthic taxa and sulfides concentration
(mg/kg dry weight) in sediments.
234
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Figure 61. Relationships between abundances (no./0.1 m2)
of selected benthic taxa and sediment grain size
(percent fine-grained material).
235
-------
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Figure 62. Relationships between amphipod bioassay response (percent mortality)
and LPAH (n.g/kg dry weight), 4-methyl phenol (^g/kg dry weight), retene
(p.g/kg dry weight), sulfides (mg/kg dry weight), and TOC (percent dry
weight) in sediments.
236
-------
abietic acid, benzoic acid, retene, a cymene isomer, and
sulfides
Benthic taxa: Capitella caoitata (Polychaeta), Euohilomedes
spp. (Crustacea), Psephidia lordi (Pelecypoda), Ax1 PODSida
serricata (Pelecypoda), Crustacea, Gastropoda, Pelecypoda,
and Polychaeta
Amphipod bioassay mortality.
The chemicals listed above were selected for this analysis mainly because of
their- high detection frequency, high concentration, potential toxicity,
potential value as tracers of pollutant sources, or some combination of
these attributes. Concentrations of most of the selected chemicals were
greatly elevated above corresponding reference values. Conventional
sediment variables "[sulfides, TOC, and grain size (percent fine-grained
material)] were also entered in the analysis. Relationships of biological
variables to metals in sediments were not examined because metals concentra-
tions were not substantially elevated in the study area. The benthic
species listed above were selected because they were widely distributed in
the project area and they represented the dominant species within their
respective major taxa at selected stations. C. capitata was also selected
because it is well known as a pollution-tolerant species. The examples shown
in Figures 57-62 were chosen because they illustrate some of the clearest
relationships between physical/chemical and biological variables. The
results for Polychaeta and Pelecypoda were selected because among major taxa
they exhibited the most depressions in abundance relative to Port Susan (see
Benthic Macroinvertebrates in Results section). Relationships of biological
variables to conventional variables (e.g., sulfides, percent fine-grained
material) are shown to provide perspective in interpreting relationships
between biological variables and toxic chemicals.
A common feature of the relationship between sediment chemistry and
biological variables is the wide scatter in the sediment toxicity and taxa
abundances at lower chemical concentrations (Figures 57-60 and 62). This
scatter is expected when relating a single chemical (or related group of
237
-------
chemicals) to a biological variable because at lower concentrations of the
chemical the biological variable could be more strongly influenced by an
unrelated chemical or other factors. For the selected chemical variables
(LPAH, 4-methylphenol, retene, and sulfides in Figures 57-60 and 62), the
primary trend observed was the consistent occurrence of high values of
sediment toxicity and low values of benthic taxa abundances at higher
concentrations of the chemicals evaluated. Aside from £. capitata and its
respective higher taxon (Polychaeta), all of the taxa analyzed were consis-
tently low in abundance at stations with higher concentrations of chemicals,
including some of the other chemicals analyzed but not shown here (e.g.,
HPAH, phenol). C. capitata was extremely abundant at Station EW-04 despite
high concentrations of many chemicals at that station. TOC content in
sediments at Station EW-04 was 29 percent, the highest value observed in the
study and among the highest values found in polluted areas of Puget Sound.
High abundance of C. capitata is typically an indicator of disturbed
conditions, especially organically-enriched habitats.
Most taxa exhibited consistently low abundances at higher concentrations
of sulfides, except C. capitata and Pol-ychaeta," which displayed an apparent
linear increase with sulfide concentration (Figure 60; r=0.98, n=19, PO.001
and r=0.94, n=19, PO.001, respectively). These apparently linear relation-
ships were each driven by two points (see Figure 60) and therefore should be
considered tentative. Nevertheless, a clear positive relationship between
the abundance of C. capitella and sulfide concentration in sediments was
found in a recent study of Elliott Bay (r=0.70, n=18, P<0.05) (PTI and Tetra
Tech 1988).
Sediment toxicity as measured by mortality in the amphipod bioassay was
generally high at higher concentrations of 4-methy1 phenol, retene, sulfides,
and TOC (see Figure 62). No clear relationship was found between amphipod
mortality and LPAH or HPAH. The amphipod bioassay has previously been shown
to be insensitive to a wide range of PAH concentrations in the environment
(e.g., Tetra Tech 1986d). The data for the other chemical variables used in
this analysis were too limited to evaluate their relationships to amphipod
mortality.
238
-------
Because fine-grained sediments were found mainly in the East Waterway
where chemical concentrations were also highly elevated (see Sediment
Chemistry in Results section), the cgvariance of chemical variables (includ-
ing sulfides) with sediment grain size probably explains the observed
relationships between several benthic taxa and percent fine-gained material
(see Figure 61). To minimize the importance of chemical factors relative to
physical structure of the sediments, the relationship of benthic infauna
abundance to grain size was examined using only reference area data. Based
on data from seven stations in Port Susan (1985 and 1986 data combined),
there was no apparent relationship between the abundances of Pelecypoda,
Axinopsida serricata. and Psephidia lordi and percent fine-grained material.
Although pelecypods were relatively less abundant at the station with the
largest fraction of fine-grained material (Station PS-01, 1985, 88 percent
fine-grained material), their relationship to sediment grain size was
clearly nonlinear, with maximum abundances achieved at stations with about
24 percent fine-grained material. At the Port Susan stations, Gastropoda
showed no clear relationship to grain size. The greatest abundance of
gastropods was found at Station PS-01 in 1985, with 88-percent fine-grained
material. Euphilomedes spp. showed a trend toward increased abundances'in
coarse-grained sediments based on the Port Susan stations, but the variation
with grain size (on the order of 2-4 times) cannot account for tire large
differences in abundance between some stations in Figure 61.
A positive linear correlation was found between amphipod mortality and
percent fine-grained material in sediments, although the relationship does
not explain much of the variance in amphipod response (r=0.57, n=32,
P<0.001). Only 33 percent of the variance is explained by a regression of
percent mortality against percent fine-grained material [Y=0.641X+13.4
(standard error of slope=±0.168; standard error of intercept = 5.68)]. The
relationship between amphipod mortality and fine-grained material in
Figure 62 is confounded by high chemical contamination at some stations with
very fine-grained sediments. Using only the data for seven sediment samples
from Port Susan (1985 and 1986 reference area data combined), no relationship
between the amphipod response and sediment grain size was found.
239
-------
DeWitt et al. (1988) developed a relationship between Rhepoxvnius
abronius mortality and percent fine-grained material in sediments from eight
reference areas of Puget Sound. Using the method of DeWitt et al. (1988)
to correct for the effects of sediment grain size, all samples with mean
mortality values identified as significantly different (P<0.05 or PO.001)
from reference in the present study would still be classified as toxic (see
Sediment Bioassays in Results section). The regression equation derived by
DeWitt et al. (1988) explained approximately 29 percent of the variance in
the relationship between amphipod mortality and percent fine-grained
material. Although DeWitt et al. (1988) were able to demonstrate experi-
mentally that very fine sediments in the silt-clay size range decreased
amphipod survival relative to survival in coarser sediments, they concluded
that particle size could not account for all of the background mortality in
reference area sediments. Moreover, they concluded that particle size is
probably just a variable that is strongly correlated with the actual cause
of mortality. In any case, the high amphipod mortalities found for several
stations in the present study cannot be explained by the effects of sediment
grain size alone.
Relationships Between Chemical and Biological Variables in the East Waterway
Because the most severe chemical contamination and associated biological
effects were found in the East Waterway, relationships between chemical and
biological variables were examined further for this area (Figure 63). Six
stations along a nearshore transect formed the main basis for this analysis:
Stations EW-01, EW-04, EW-07, EW-10, EW-12, and EW-14 in order from north to
south. Two additional stations (Stations NG-01 and NG-02) from the adjacent
area immediately south of the East Waterway were also included to provide
perspective based on relatively uncontaminated conditions. Chemicals
selected for this analysis included LPAH, 4-methy1 phenol, 2,4,6-trichloro-
phenol, dehydroabietic acid, and sulfides. All of these chemicals exhibited
elevated concentrations in the East Waterway and are representative of
important compound classes in that area. LPAH represents a group of six PAH
compounds, with naphthalene as a predominant component in East Waterway
sediments. Relationships between biological variables and HPAH were similar
to those shown for LPAH. 4-Methylphenol, an alkyl-substituted phenol, was a
240
-------
20
^800 -i
LEGEND
EW-01 |EW-07]EW-12| NG-01
EW-04 EW-10 EW-U NG-02
O
cc
UJ
01
Z
Z
PELECYPODA
GASTROPODA
TOTAL ABUNDANCE
NUMBER OF TAXA
SULFIDES
* 2.4 6-TRICHLOROPH6NOL
* - OEHYOROABIETIC ACID
4.M6THYLPHENOL
* LPAH
NORTH -
STATIONS
-SOUTH
Figure 63. Relationships between selected biological and chemical
variables in the East Waterway and adjacent areas.
241
-------
problem chemical that occurred at substantially elevated concentrations
throughout much of the study area, but especially in the East Waterway.
Dehydroabietic acid, a resin acid, occurred at very high concentrations in
the East Waterway and had the highest EAR values among resin acids. 2,4,6-
Trichloropheriol occurred at less elevated concentrations than the compounds
above, but was selected to represent the covarying class of chlorinated
phenolic compounds (chlorinated phenols and chlorinated guaiacols) often
reported in bleached pulp effluents. Sulfides were included in the analysis
because of their known association with pulp mill discharges and because of
their extreme concentrations in the East Waterway.
The data shown in Figure 63 indicate a maximum biological impact at
Station EW-01 and a gradient of generally decreasing effects toward Stations
NG-01 and NG-02. Station EW-14 exhibited slightly increased biological
effects relative to adjacent stations. Amphipod mortality was 100 percent
at Station EW-01 and generally decreased from north to south toward Stations
NG-01 and NG-02 (Figure 63). A moderate increase in mortality was observed
at Station EW-14 compared with adjacent stations. The 'total number of
benthic infaunal taxa and the abundances of Gastropoda arid Pelecypoda
increased from Station EW-01 to Station EW-12. The number of taxa remained
generally high along the remainder of the transect, decreasing slightly from
Station EW-14 to Station NG-02. Gastropoda abundance decreased consistently
and Pelecypoda abundance fluctuated from Station EW-12 to Station NG-02.
The abundance of total Mollusca generally increased from Station EW-01 to
Station NG-01, with a decrease at Station EW-14 relative to adjacent
stations. The total abundance of benthic infauna fluctuated greatly from
Station EW-01 to Station EW-10 and decreased thereafter toward Station
NG-02. The high abundances of the polychaete C. capitata. the crustacean
Nebalia spp., and nematode worms at Stations EW-04 and EW-10 account for the
peaks in total infauna abundance at these sites. The high abundances of
these opportunistic taxa and the relatively low number of total taxa indicate
severely disturbed conditions in the benthic assemblages at these sites. The
crustacean Leptochelia spp. accounted for the high abundance of total infauna
at Station EW-12. The presence of this taxon and the relative increase in
total number of taxa indicate less disturbed conditions compared with other
sites in the East Waterway.
242
-------
The general pattern of chemical contamination among these stations
corresponded to the biological effects pattern (see Figure 63). However, the
distribution of chemical concentrations among stations differed among
specific chemicals. The clearest gradient relationships between single
chemicals and biological variables were found for sulfides and 2,4,6-
trichlorophenol. Concentrations of sulfides and 2,4,6-trichlorophenol
generally decreased from the head of the East Waterway to Stations NG-01 and
NG-02. Other chemicals that displayed maximum concentrations at Station
EW-01 included sandaracopimaric acid, 2,4-dichlorophenol, 2,3,4,6-tetra-
chlorophenol, 3,4,5-trichloroguaiacol, 4,5,6-trichloroguaiacol, and tetra-
chloroguaiacol. In contrast to the distribution pattern shown by sulfides
and 2,4,6-trichlorophenol, the concentrations of LPAH, 4-methy1 phenol, and
dehydroabietic acid at Station EW-01 appeared relatively low compared to
Stations EW-04 and EW-07. Dehydroabietic acid concentrations maximized at
Station EW-04 and 4-methy1 phenol concentrations maximized at Station EW-07.
Finally, concentrations of LPAH, 4-methy1 phenol, and sulfides were higher at
Station EW-14 relative to those at Stations EW-12 and NG-01, corresponding
to'the increased biological effects at-that site. It should be emphasized-
that the general pattern of decreasing chemical contamination and decreasing
biological effects from north to south in the East Waterway (see Figure 63)
may not represent the actual fine-scale pattern of chemical and biological
conditions. Chemical concentrations at additional stations in the waterway
where biological variables were not measured suggest a complex pattern of
contamination at nearshore stations (see Sediment Chemistry in Results
section). Most notably, Station EW-13, which was not tested for site-
specific biological effects, had very elevated concentrations of certain
chemicals related to the pulp industry (e.g., the highest concentrations of
abietic acid, neoabietic acid, and isopimaric acid in the study).
Two potential patterns of chemical distribution and effects may be
invoked to explain the apparent decrease in biological effects from the head
of the East Waterway to stations along the southern shore of Port Gardner
(see Figure 63). First, a gradient in concentrations of a chemical or of a
group of chemicals may correspond to the observed trend in biological impacts
(e.g., sulfides, chlorinated phenols). Second, a pattern of transition from
243
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one dominant chemical to another in a complex mixture may account for the
gradient in observed biological effects (e.g., transition from maximum
sulfides at the head of the East Waterway to maximum dehydroabietic acid at
Station EW-04 to maximum 4-methylphenol at Station EW-07). Although the
specific chemical or suite of chemicals responsible for biological effects
probably varies among stations, the major biological impacts observed at
Stations EW-01, EW-04, and EW-07 are likely related to pulp mill discharges.
The contributions of variations in percent fine-grained material and TOC to
the observed pattern of biological effects is probably minor, as discussed
previously. The extreme depressions of benthic infauna and the high
bioassay mortalities observed at selected stations in the East Waterway
cannot be accounted for by variations in physical structure and organic
carbon content of the sediments.
Comparison of Contamination and Significant Biological Effects
Both sediment, toxicity and the number of significant benthic effects
were generally high at the most contaminated stations. Among the 23
priority (Tier II). problem stations identified in the next chapter (see
Prioritization of Problem Areas and Contaminants), HAET were exceeded for at
least one chemical at 21 stations. Of these 21 stations, sediment toxicity
to amphipods, benthic infauna abundances, or both were evaluated at 12
stations. Eight of these 12 stations (=67 percent) displayed significant
toxicity to amphipods, depressions in the abundances of major taxa of
benthic infauna, or both (PO.001). At the four problem stations without
significant biological effects (Stations ES-03, EW-12, NG-10, and NG-14),
concentrations of problem chemicals were not substantially higher than HAET
(1-3 times HAET, with a mean of 1.9 times HAET). Seven of the eight
stations with significant effects exhibited severe biological effects that
were sufficient for problem area definition (i.e., >40 percent amphipod
mortality or >80 percent depression of at least one major taxa of infauna).
Three stations that exhibited severe effects for both the amphipod bioassay
and indigenous benthic assemblages were among the highly contaminated sites
in the Everett Harbor system. These three stations are listed below:
244
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Station EW-01, located in the East Waterway, exhibited
exceedances of HAET for phenol and 4-methylphenol in sedi-
ments. Maximum concentrations in the study area were also
observed for sandaracopimaric acid, 2,4-dichlorophenol,
2,4,6-trichlorophenol, 2,3,4,6-tetrachlorophenol, 3,4,5-
trichloroguaiacol, 4,5,6-trichloroguaiacol, and tetrachloro-
guaiacol (AET are not available for these compounds).
Station EW-04, located in the East Waterway, displayed HAET
exceedances for LPAH, 4-methy1 phenol, phenol, 2-methy1 phenol,
2,4-dimethylphenol, benzyl alcohol, PCBs, 1,2-dichlorobenzene,
and TOC. The dehydroabietic acid concentration at this
station exceeded an EAR of 1,000 (no AET is available for
DMA). Many other compounds (e.g., all chlorinated resin
acids, PCP, 2-chlorophenol, and most TIO compounds) had
maximum concentrations at this station.
Station EW-07, located in the East Waterway, exhibited HAET
exceedances for LPAH, 4-methy1 phenol, 2-methy1 phenol, and
2,4-dimethylphenol.
Concordance between the biological and chemical results at these stations and
others that exhibited significant biological effects was generally reflected
in similar priority rankings based on chemical vs. biological variables (see
Prioritization of Problem Areas and Contaminants).
Although either severe sediment toxicity or effects on benthic infauna
were usually observed at highly contaminated sites, one exception to this
trend is notable. Significant, but not severe, biological effects were
found at Station EW-14 which had highly contaminated sediments exceeding
HAET for the following chemicals: LPAH, phenol, 4-methylphenol, dibenzo-
furan, benzoic acid, copper, and zinc. Among stations in the Tier II
problem areas with a full complement of biological indicators, Station EW-14
was the only station that exhibited a difference of at least 30 percent
between the separate priority scores based on chemistry and biology (see
below, Prioritization of Problem Areas and Contaminants). Nevertheless,
245
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increased biological effects were apparent at Station EW-14 relative to
adjacent sites (see Figure 63). Also, the abundance of pelecypods was
significantly reduced at Station EW-14 compared to Port Susan reference
conditions (PO.001).
Severe biological effects observed in this study were rarely associated
with low chemical contamination (i.e., concentrations below AET). Severe
biological effects were sufficient for definition of a problem area at only
one station (Station SD-01) where chemical contamination was relatively low
(i.e., where LAET were not exceeded for any chemical). Several benthic taxa
displayed >80 percent depression at Station SD-01. However, swift currents
within the delta channel where this station was located (as indicated by
bathymetry and coarseness of the sediments) may be responsible for disturb-
ance of the benthic community. The concentration of sulfides at Station
SR-07 was 600 mg/kg DW, which is in the range of amphipod and benthic AET
(540-630 ug/kg DW) currently being developed under a separate EPA project.
Severe depressions in abundances of gastropods, pelecypods, and polychaetes
were observed at Station SR-07. The low abundances of benthic infauna at
this site may be caused partly by the extreme sediment texture (95.5 percent
fine-grained material) or periodic hypoxia due to poor flushing within the
marina. Also, TBT was detected in a sediment sample from Station SR-07.
In conclusion, significant (P<0.001) biological -effects as measured by
the amphipod toxicity bioassay and reductions in abundances of benthic
infauna taxa were generally associated with high concentrations of contami-
nants in sediments. At the four problem stations without significant
biological effects (Stations ES-03, EW-12, NG-10, and NG-14), concentrations
of problem chemicals were not substantially higher than HAET.
COMPARISON OF BIOASSAY RESPONSES WITH BENTHIC INVERTEBRATE ASSEMBLAGES
This section examines the degree of consistency between bioassays and
benthic infauna as indicators of environmental contamination. The amphipod
bioassay represented the acute (10-day) response of an individual species
(Rhepoxvnius abronius) to sediment removed from its natural setting, whereas
benthic infauna represented the in situ, acute and chronic (weeks to months)
246
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responses of groups of organisms (i.e., major taxa). The objectives of the
following sections are to determine whether the two indicators were corre-
lated or displayed similar patterns of statistically significant differences
from reference conditions. Because the two indicators measure somewhat
independent biological responses, complete concordance between bioassay and
benthic infauna results is not expected. Comparisons of bioassay responses
with abundances of benthic infauna taxa were based on the 16 stations in the
Everett Harbor system and the three stations in Port Susan at which both
indicators were evaluated.
Correlation of Indicators
The abundances of Amphipoda and Gastropoda were each consistently low
at stations that exhibited a mean mortality greater than about 50 percent in
the amphipod bioassay (Figure 64). Thus, the relationship between percent
mortality in the bioassay and the abundance of amphipods was characterized by
a response region (i.e., area of consistently low mortality) rather than a
simple linear function (Figure 64). The abundances of Polychaeta and
Pelecypoda were not clearly related to amphipod mortality.
PTI and Tetra Tech (1988) found distinct response regions in the rela-
tionships between amphipod mortality and abundances of several infaunal
taxa. For example, the abundances of Euphilomedes. JP. lordi. and total
crustaceans were consistently low at mean amphipod mortalities above
50 percent. The amphipod mortality bioassay was a good predictor of the
response of these taxa at >50 percent amphipod mortality. Below 50 percent
mortality in the bioassay, the response of all benthic taxa evaluated was
variable.
Tetra Tech (1985a) reported a lack of linear relationships between the
amphipod bioassay response and the abundances of the following major taxa in
the Commencement Bay system: Polychaeta, Mollusca, Crustacea, Echinodermata,
and total taxa. Similarly, PTI and Tetra Tech (1988) did not find simple
linear relationships between amphipod mortality and the abundances of
Euphilomedes spp., Pseohidia lordi. Qdostomia spp., Pelecypoda, and Crus-
tacea. As noted in the latter report, the wide range of abundances of
247
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Figure 64. Relationships between abundances of selected benthic
taxa (no./0.1 m2) and amphipod bioassay response
(percent mortality).
248
-------
infaunal taxa at lower mortality levels in the amphipod bioassay (Figure 64)
may be explained by the potentially higher sensitivity of indigenous benthic
assemblages to toxic chemicals. This higher relative sensitivity of the
infaunal assemblages could result from chronic exposure (compared to short-
term exposure in the bioassay) or exposure of sensitive juvenile stages
(compared with exposure of adult organisms in the bioassay).
Comparison of Bioassav Responses with Benthic Groupings
Values of amphipod mortality were compared with the groupings of
stations determined by classification analysis of benthic invertebrate
assemblages (see above, Benthic Macroinvertebrates in Results section). The
results of this comparison show that the mean level of amphipod mortality
differed among groups of stations that differed in benthic infaunal charac-
teristics (Figure 65). The mean bioassay mortality among benthic infaunal
Group I stations displayed a large range (5-100 percent mortality) relative
to other benthic infaunal groups. Most stations in Group I displayed mean
amphipod mortalities of. less than 35 percent. Amphipod mortalities at
stations in benthic infaunal Group II ranged from 5 to 37 percent, with a
mean of 18 percent. The stations in Groups I and II each exhibited one or
no significant depressions (P<0.001) of the four major taxa used to define
problem areas (i.e., Polychaeta, Pelecypoda, Gastropoda, and Crustacea).
At Group I Station NG-04, only the abundance of polychaetes was significantly
lower than reference conditions (P
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k
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LEGEND
STATION MEAN
MEAN AMONG STATIONS
STATION GROUP
Figure 65. Amphipod bioassay responses in relation to station groupings based on
classification analysis of benthic assemblages.
-------
In co.nclusion, stations that exhibited the most severe benthic effects
also displayed the highest toxicity levels found in the study. These
stations were all located in the East Waterway. Mean amphipod mortality was
generally less than 50 percent at stations with little or no effects on
benthic infauna. A similar finding was reported by Tetra Tech (1985a) and
PTI and Tetra Tech (1988).
Comparison of Significant Responses
The relationship of significant mortality in the amphipod bioassay to
the occurrence of at least one significant depression of a major taxa of
benthic infauna is presented in Table 34. Overall, the concordance in the
responses of the bioassay and infauna was 56 percent (i.e., the percentage
of stations showing consistent responses was about 56 percent). Because of
the small sample size (n=16 stations), concordance for the study area as a
whole was not substantially better than that expected by chance alone (i.e.,
50 percent). Concordance between the bioassay and benthos was found at
highly contaminated sites, especially in the East Waterway (see above,
General Correlation of Indicators in Relationships among Contaminants,
Toxicity, and Benthic Effects section). The lack of study-wide concordance
between significant responses in the amphipod bioassay and in benthic
infauna despite strong concordance within geographically distinct problem
areas was also reported by Tetra Tech (1985a) and PTI and Tetra Tech (1988)-
for Commencement Bay and Elliott Bay, respectively.
SUMMARY
Biological effects as measured by the amphipod toxicity
bioassay and significant reductions in abundances of benthic
infauna taxa were generally associated with higher concentra-
tions of contaminants in sediments.
The relationship between sediment contamination and abund-
ances of several selected benthic taxa was characterized by a
response region where abundances were consistently low at
high concentrations of contaminants. An apparent threshold in
251
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TABLE 34. CORRESPONDENCE BETWEEN STATIONS HAVING
SIGNIFICANT (PO.001) BIOASSAY RESPONSES
AND STATIONS HAVING SIGNIFICANT (P<0.001)
BENTHIC DEPRESSIONS
Benthic Depression
Bioassay Response Yes No
Yes 25% 0%
No 44% 31%
NOTE: Total no. stations = 16.
252
-------
the biological response was found for AxiHODSida serricata.
Euohilomedes spp., Pseohidia lordi. Pelecypoda, and Gastropoda
in relation to specific concentrations of each of the
following chemicals: LPAH, HPAH, naphthalene, 4-methylphenol,
retene, phenol, and sulfides. For the other organic compounds
evaluated, the number of stations with detected values was
too small or the distribution of the data was too skewed to
show a strong association with biological variables.
The abundance of the pollution-tolerant polychaete Capitella
caoitata displayed a roughly linear increase with sulfide
concentration in sediments and no apparent relationship with
concentrations of other chemicals or grain size.
Amphipod mortality was generally high at higher concentrations
of 4-methylphenol, retene, TOC, chlorinated phenols, resin
acids, and sulfides, but was not clearly related to the other
chemical variables evaluated. The high amphipod mortalities
found at several stations were not fully explained by the
potential relationship between sediment toxicity and grain
size.
Biological effects generally decreased along a spatial
gradient from the head of the East Waterway (Station EW-01) to
stations southwest of the historical Weyerhaeuser kraft mill
site. The concentrations of sulfides and chlorinated phenols/
guaiacols followed a similar trend at selected stations where
biological variables were measured. Concentrations of some
resin acids, 4-methy1 phenol, and LPAH were relatively low at
the head of the East Waterway compared with the next station
to the south (Station EW-04), but otherwise corresponded
generally to the biological effects data. Although the
specific chemical or suite of chemicals responsible for
biological effects probably varies among stations, the major
biological impacts observed at Stations EW-01, EW-04, and
EW-07 are likely related to pulp mill discharges. The
253
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observed spatial gradient is probably not representative of
fine-scale spatial patterns, since chemical contamination is
more complex along a similar transect when data from chemistry
only stations are considered.
Both severe (>40 percent) amphipod mortality and severe
(>80 percent) depression of at least one major taxon of
infauna were observed at the following highly contaminated
sites: Stations EW-01, EW-04, and EW-07. Severe biological
effects were found at only one station (i.e., depressions of
three major taxa at Stations SD-01) where chemical contamina-
tion was relatively low (i.e., all concentrations were below
LAET). Sediment structure and physical disturbance due to
current scour probably accounts for benthic depressions at
Station SD-01.
The abundances of both indigenous amphipods and gastropods
were consistently low at stations with >50 percent amphipod
mortality in the toxicity bioassay. The abundances of. both
polychaetes and pelecypods were not clearly related to
amphipod mortality.
Concordance between statistically significant responses in the
toxicity bioassay and depressions of infaunal taxa was not
substantially greater than that expected by chance alone.
This is not surprising given the wide range and levels of
contaminants in the Everett Harbor system and the different
endpoints measured by these two indicators (i.e., acute
mortality of adults of a single species in the bioassay and
chronic effects on all life stages of an assemblage of species
in the benthic infaunal indices). Moreover, concordance
between the bioassay and benthos was found at highly contami-
nated sites, especially in the East Waterway.
254
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PRIORITIZATION OF PROBLEM AREAS AND CONTAMINANTS
In this section, the selected data for indicators of sediment contami-
nation, toxicity, and biological effects are integrated to evaluate toxic
contamination problems in the Everett Harbor system. The approach for the
ranking of problem areas was described earlier (see Decision-Making Framework
in Methods section) and is summarized in Figure 3. Based on the significance
and magnitude of EAR compiled in the Action Assessment Matrix format,
analysis of problem areas and their priority ranking was performed in the
following phases:
Tier I Problem DefinitionIdentification of broad areas that
exceeded action-level guidelines (see Table 3) for combined
significant elevations of sediment chemistry, fish pathology
and bioaccumulation
Tier II Problem DefinitionIdentification of problem
stations that triggered action-level guidelines based on
significant EAR and exceedance of a) the 90th percentile
concentration or HAET of chemicals in sediments, b) 80
percent depression of any one of four major benthic taxa
(Polychaeta, Crustacea, Pelecypoda, or Gastropoda), c) 40
percent mortality in the amphipod bioassay, or d) any
combination of the preceding.
Grouping of problem stations into multi-station problem areas was based on
chemical distributions (including data from recent historical studies), the
nature and proximity of potential sources, and geographic and hydrographic
boundaries.
Ranking of Problem SitesScoring of problem stations
following the criteria in Table 4, and ranking of each multi-
station problem area based on the average of the scores for
individual stations within the area.
255
-------
A characterization of each Tier II problem area based on the distributions
of potential problem chemicals that exceeded AET is also provided in this
section.
IDENTIFICATION OF PROBLEM AREAS
Broad areas of the nearshore Everett Harbor system displayed concentra-
tions of chemical contaminants in sediments above the maximum values for
Puget Sound reference areas. Nevertheless, chemical "elevations at most
stations outside the East Waterway were not highly elevated above reference
values. Because neither bioaccumulation nor pathological variables were
significantly elevated in the study area (P>0.001), Tier I problem evaluation
did not result in definition of large-scale problem areas. Areas of
potential concern were defined based on exceedance of LAET for at least one
chemical in sediments. As shown below, these areas of potential concern are
largely contiguous with the problem areas defined in the Tier II analysis.
Information on the significance of EAR for all indicators, at each
station was compiled in an Action Assessment Matrix. Stations identified as
Tier II problem sites (Figure 66) were considered for further priority
ranking. A matrix of priority scores for Tier II problem areas and the
indicators that exceeded action levels for severe contamination and effects
is presented in Appendix I.
The following problem areas containing multiple stations were identified
(Figure 66):
EW (the East Waterway)
NG (near the Mukilteo sewage discharge, ferry terminal and
defense fuel storage depot).
In addition, the following single stations were identified as localized
problem areas: ES-03, 06-01, SD-01, SD-03, SR-05, SR-07 (Figure 66).
256
-------
NG-09
NG-10
NG-11
O
LABELED STATIONS WITHIN
SOLID LINES EXCEEDED HAET
OH TIER II BIOLOGICAL CRITERIA
LABELED STATIONS WITHIN
DASHED LINES EXCEEDED LAET
OR 90TH PERCENTILE CONCEN-
TRATIONS FOR CHLORINATED
PHENOLSOUAIACOLS AND/OR
RESIN ACIDS
SMI Titles 07. 38 and Appendix J
lot infoimalion on which cftgmicaM
eicaeded AET al (he stations shown
aoove and a hotoncal alalions.
Figure 66. Everett Harbor problem areas.
257
-------
RANKING OF PROBLEM AREAS
Ranking of problem areas within the Everett Harbor system was performed
using the Action Assessment Matrix. Arithmetic mean EAR values compiled for
each data type and each multi-station problem area (Tier II) are shown in
Table 35. Reference values are shown on the right-hand side of the table.
For each indicator, mean- reference values across all stations within the
reference area are shown for comparison. The original value for an indicator
can be obtained by multiplying the EAR reported in the table by the appro-
priate reference value. Only the original data for the prevalences of liver
neoplasms and megalocytic hepatosis are shown because the reference area
prevalences were zero, resulting in infinite elevations.at the study sites.
Note that benthic infauna EAR are calculated as the inverse of the ratio
used for other indicators (i.e., as the ratio of the reference value to the
study site value) because a toxic effect is expected to produce a depression
in abundance. Refer to Appendix I for information on each station in the
multi-station problem areas.
For perspective in interpreting. Table 35, each of the following
represent a severe effect that is sufficient for definition of a problem
area:
>40 percent amphipod mortality, which corresponds to an EAR
of >1.8
>80 percent depression in abundance of one or more benthic
taxa, which corresponds to an EAR of >5
Exceedance of the HAET or the 90th percentile (for selected
chemicals without AET) for sediment chemistry
Significant elevation of any three indicators.
At least one of the four primary conditions just listed are met by each area
shown in Table 35. Significant EAR for sediment chemistry and exceedances
of HAET were found in all o.f the Tier II problem areas except Station SD-01,
258
-------
TABLE 35. ACTION ASSESSMENT MATRIX OF SEDIMENT CONTAMINATION,
TOXICITY, AND BIOLOGICAL EFFECT INDICES
FOR EVERETT HARBOR PROBLEM AREAS
Problem Area Elevations3
Variable
Sediment Chemistry
LPAH
HPAH
4-methyl phenol
Phenol
2-methyl phenol
2, 4-di methyl phenol
Benzoic acid
Dehydroabietic acid
Benzyl alcohol
PCBs
p.p -DDT
1 , 2-di chl orobenzene
Copper
Zinc
East
Waterway
310
89
1,900
40
40
14
14
430
17
180
20
26
43
Area
NG
31
36
200
24
LJLU
1 120 1
11
2.8
3.0
ES-03
4.4
3.6
110
36
E3T]
3.8
3.6
OG-01
21
8.4
98
14
5.4
4.4
SD-01 SD-03
1.1 9.8
0.70 3.6
0.20 57
3.9
0.50
3.2
f 273"]
2.9 8.2
2.7 4.8
SR-05
21
22
150
3.6
6.9
56
4.2
9.0
5.5
SR-07
12
17
17
ITX
1.4
15
8.1
Reference
Val ueb
<41 ppb
<79 ppb
<13 ppb
<33 ppb
U 7 ppb
U 7 ppb
<150 ppb
<63 ppb
U 10 ppb
<6 ppb
U 10 ppb
U 3.5 ppb
6.37 ppb
19 ppb
Sediment Taxicity
Amphipod mortality
Infauna"
Polychaetes
Gastropods
Pelecypods
Crustaceans
Fish Pathology
Neoplasms'"
Foci
Megalocyt'ic hepatosisc
Bioacc mutation
0.68
0.68
1.5
PCBs
PCBs
English sole
Dungeness crab
3.5
1
0.71
3.2
2.1
2.7
1.9
2.7
3.8
2.8
1.7
0.49
0
2.8
0.70
22%
1,570/mi:
50/n£
i.seo/m^
1,000/m2
7.1%
0%
8.3 ppb
5.0 ppb
a Boxed numbers represent elevations of chemical concentrations that exceed all Puget Sound reference area
values, and statistically significant (P<0.001) toxicity and biological effects at one or more stations
compared with reference conditions in Port Susan. Significance tests were not performed on the bioaccumulation
data (see Results). Chemicals shown in the table had concentrations exceeding HAET or ^EAR >1,000. The "U"
qualifier indicates the chemical was undetected and the detection limit is shown. The "<" qualifier indicates
the chemical was undetected at one or more stations. The detection limit is used in the calculations.
Infauna EAR are based on the elevation in biological effects represented by reductions in infaunal abundances
relative to reference conditions. EAR for all other variables reflect an increase in the value of the variable
at Everett Harbor compared with reference conditions. Blank spaces in sediment chemistry columns indicate
that the chemical was undetected throughout the problem area.
b EAR values shown for each area are based on Carr Inlet reference values for sediment chemistry and on Port
Susan (1986) reference values for biological variables.
c Prevalences of neoplasms and megalocytic hepatosis at each problem area are shown in table instead of EAR
because the reference values were 0%.
259
-------
which exhibited severe depressions in .the abundances of major taxa of
benthic infauna, but not significant (P<0.001) amphipod mortality. Chemicals
that exceeded AET at each station are discussed in the next section (see
Chemical Characterization of Problem Areas).
Total scores for sediment chemistry and biological effects were
determined separately for each station. The ranking criteria presented in
Table 4 were applied to the Action Assessment Matrix for single stations
(Appendix I). The score for each multi-station area was calculated as the
average of the scores for individual stations within the area (for details,
see Decision-Making Framework in Methods section). Normalized scores for
the Tier II problem areas and single stations are presented in Figure 67.
Of the two multi-station problem areas, the East Waterway ranked
highest, with average scores of 58 percent for chemistry and 21 percent for
biology. The multi-station problem area near Mukilteo received average
scores of 34 percent for chemistry and 20 percent for biology. Biological
scores varied greatly- among stations within both of these areas. Sediment
chemistry scores were heterogeneous within the East Waterway, but not within
the NG problem area near Mukilteo.
Ten stations scored >50 percent based on either sediment chemistry or
biological effects (Figures 67 and 68). Of the 10 highest priority stations,
three scored >50 percent for both sediment chemistry and biological effects:
Station EW-01
Station EW-04
Station EW-07.
Stations EW-10, EW-13, and EW-14 scored >50 percent based on chemical
variables alone. Stations NG-09, NG-11, SD-01, and SR-07 scored >50 percent
based on biological variables alone. Station SD-01 received a high score
for biology because benthic infauna were apparently impacted. However,
swift currents within the delta channel where this station was located (as
260
-------
EW-14
EW-04
-13
EW-01
EW-07
-10
NG-04 NG-10 ES-03 EW-11
-05 -11 SR-05 -12
-09 -U -15
NG-07 SR-07 OG-01
-08 SD-03
SD-01
100^
80-
60-
40-
20-
0-"
EW-01 NG-09 SD-01
-04 -11 SR-07
-07
EW-10 NG-04
NG-10
EW-14
EW-11 ES-03 NG-05 SD-03
-12
-13
-15
-07
-08
-14
CHEMISTRY BIOLOGY
AVERAGE RANK SCORE
LEGEND
NG Nearshore Port Gardner
OG Offshore Port Gardner
EW East Waterway
S 0 Snohomish River Delta
S R Snohomish River
E S Ebey Slough
NOTE: Limited biological data were available for most stations (see Appendix I).
Figure 67. Ranking of single stations classified as problem sites.
261
-------
EW-04 (C,8)
EW-07 (C.B)
EW-10(C)
EW-13(C)
EW-14(C)
NG-09(8)
NG-11 (B)
NOTE: Problem Stations - HAET or Tier II biological criteria exceeded
Problem Areas Contain several problem stations. Lines
delineating problem areas are estimated boundaries based on
available data (including Historical data Irom stations shown
in Figures 3 1 -32) and are not highly precise. Stations not
exceeding the criteria may exist within problem areas. See
Tables 37. 38, and Apoendix J lor information on AET
exceedances at each station.
Problem area EW and the single stations wim labels sxmb.ted
scores 2 50% for chemistry (C), biology (8), or both (C. 8).
Identification of station SD-01 as a problem site is tentative
(see text).
26Z
-------
indicated by bathymetry and coarseness of the sediments) may be responsible
for disturbance of the benthic community. Because bioassay mortality was
low (15 percent) at Station SD-01, and because species composition of
benthic infauna indicated an absence of impacts attributable to toxic
chemicals, the designation of Station SD-01 as a problem area should be
considered tentative. Sediment texture, hypoxia, or high sulfides concentra-
tions at Station SR-07 may have contributed to the severe depressions in the
abundances of infaunal taxa at that site. Station EW-14 received the
maximum possible score of 100 percent for chemistry, but scored very low (6
percent) for biology. Despite the lack of statistical significance in some
EAR for biological variables, increased toxicity of sediments to amphipods
and effects on benthic infauna at Station EW-14 were apparent based on.
comparisons with adjacent stations (see Figure 63).
CHEMICAL CHARACTERIZATION OF PROBLEM AREAS
In this section, the Tier II multiple-station and single-station
problem areas listed above are characterized with regard to the distributions
of selected problem chemicals (Table 36) and other chemicals of-concern. To
facilitate analysis by the Everett Harbor Work Group, a description is
provided of the chemicals at notable stations within each problem area.
Detailed tables of AET exceedances (including the factor by which AET were
exceeded) are included in Appendix J, and more detailed descriptions of
chemical distributions are presented in the Results section. The following
points should be considered regarding the application of AET to chemical
data in this study:
AET values have not been established for all chemicals
measured in the present study (most notably, resin acids and
chlorinated phenols/guaiacols). For this reason, another
criterion (EAR >1,000) was used in addition to AET to
establish problem chemicals. Also, 90th percentile concentra-
tions of chlorinated phenols/guaiacols and resin acids were
used to designate lower priority problem stations.
263
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TABLE 36. EVERETT HARBOR PROBLEM CHEMICALS
LPAHa HPAHc'd
2-methylnaphthalene butyl benzyl phthalated
dibenzofuran N-nitrosodiphenylamined
dibenzothiophene arsenicd
4-methylphenol cadmiunr
phenol lead"
2-methylphenol mercuryd
2,4-dimethylphenol
benzoic acid
dehydroabietic acid"
benzyl alcohol
PCBs
p.p'-ODT
1,2-dichlorobenzene
copper
zinc
a The term LPAH represents the following chemicals: naphthalene,
acenaphthylene,-acenaphthene, fluorene, phenanthrene, and anthracene.
b Established as a problem chemical based upon -EAR>1,000. No AET
is available for dehydroabietic acid.
c The term HPAH represents the following chemicals: fluoranthene,
pyrene, benzo(a)anthracene, chrysene, total benzofluoranthenes,
benzo(a)pyrene, indeno(l,2,3-c,d)pyrene, dibenzo(a,h)anthracene,
and benzo(g,h,i)perylene.
d This chemical exceeded the LAET but not the HAET. Other chemicals
in this table exceeded the HAET at least one time (except dehydro-
abietic acid, footnote b).
264
-------
AET for antimony, chromium, nickel, beryllium, and thallium
were not used to determine problem stations in this study.
The AET for antimony and chromium were not used because of
the likelihood that analytical methods used to generate AET
for these chemicals are not directly comparable to the
methods used in the present study (see Chemistry, Quality
Assurance/Quality Control Results in Methods section). The
AET for nickel was not used because the range of nickel
concentrations in the database used to generate existing
Puget Sound AET is relatively limited. Beryllium and
thallium were excluded for similar reasons; the exclusion of
these two chemicals applies only to historical data, as they
were not measured in the present study.
East Waterway Problem Area
Sediment contamination in this depositional area is extreme and
complex., and appears strongly related to pulp industry discharges. Addi-
tional sources (e.g., CSOs and storm drains) may be important for some
chemicals. The East Waterway problem area contained the highest sediment
concentration of virtually every chemical measured in this study, including
phenolic compounds (e.g., alkyl-substituted phenols, chlorinated phenols,
chlorinated guaiacols), resin acids (both chlorinated and unchlorinated),
PAH, PCBs, and most metals. The most severe contamination was observed
along the east shore of the waterway (near potential sources), although the
area near the west shore of the waterway was less well characterized for
certain organic compounds.
Although many chemicals exceeded HAET in the East Waterway problem
area, 4-methylphenol and LPAH concentrations exceeded HAET most frequently
(Table 37) and were important in defining problem area boundaries. 4-Methyl-
phenol concentrations maximized at Station EW-07 (98,000 ug/kg DW;
EAR=7,500). Concentrations decreased along the east shore moving away from
Station EW-07, but nonetheless exceeded an EAR of 1,000 at Stations EW-04,
EW-10, EW-13, and EW-14 (concentrations ranged between 15,000 and
35,000 ug/kg DW at these stations). LPAH concentrations in the East
265
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TABLE 37. EAST WATERWAY PROBLEM AREA3
Station
EW-01
BPS30e
E-04f
EW-04
EW-07
PS059
BPS296
PS069
EW-10
EW-11
EW-12
BPS28e
EDS-4h
A41
EW-13
EW-14
EW-15
HAET Exceedances _
LPAH HPAH 4MEPHNL PHNL 2MEPHNL 2,4-MEPHNL BNZACID BNZOH PCBS 1,201 CLBNZ
X X
X X
X X
X XXX X XXX
XX XX
X X
X
X
X X
X
X
X
X
X X
XXX X
X X
CU ZN TOC DHAC TOTXYLENE LAET Exceedancesd
BUTBNZPH, NNP [24CLPHNL, 245CLPHNL,
246CLPHNL, 2346CLPHNL, 345TCG,
456TCG, TETCG, SANDARACO]
PCBS, ZN
HPAH, PCBS, ZN
X X HPAH [2CLPHNL, 24CLPHNL, 2346CLPHNL
PCP, ABIET1C, ISOPIMARIC. SANDARACO
12CLDHA, 14CLDHA]
PHNL [ISOPIMARIC, 12CLDHA]
X ZN
HPAH, PCBS
HPAH
LPAH, HPAH, HG
BNZOH, PHNL
HPAH, PCBS
X PCBS
X
X X PHNL, ZN, HPAH [24CLPHNL. ABIETIC,
ISOPIMARIC]
X X HPAH, AS, CD, PB, HG
a Chemical codes used in this table:
LPAH - Signifies AET exceedances for the sum of naphthalene, acenaphthylene, acenaphthene, fluorene, phenanthrene, and anthracene, or any of these compounds individually.
To simplify the presentation of AET exceedances in this table, exceedances of AET for 2-methylnaphthalene, dibenzofuran, and dibenzothiophene are included under
LPAH. These compounds covaried with LPAH but are not included in LPAH sums.
HPAH - Signifies AET exceedances for the sum of fluoranthene, pyrene, benzo(a)anthracene, chrysene, total benzofluoranthenes, benzo(a)pyrene, indeno(l,2,3-cd)pyrene,
dibenzo(a,h)anthracene, and benzo(g,h,iJperylene, or of any of these compounds individually.
4MERHNL - 4-methyl phenol
PHNL - phenol
2MEPHNL - 2-methyl phenol
2,4-MEPHNL - 2,4-dimethyl phenol
BNZACID - benzoic acid
BNZOH - benzyl alcohol
PCBS - polychlorinated biphenyls
2CLPHNL - 2-chlorophenol
24CLPHNL - 2.4-dichlorophenol
245CLPHNL - 2,4,5-trichlorophenol
246CLPHNL - 2,4,6-trichlorophenol
2346CLPHNL - 2,3,4.6-tetrachlorophenol
PCP - pentachlorophenol
345TCG - 3,4,5-trichlo_roguaiacol
-------
"FABLE 37. (Continued)
1.2DICLBNZ - 1.2-dichlorobenzene 4561CG - 4.5,6-trichloroguaiacol
CD - copper TETC6 - tetrachlorogua-iacol
ZN - zinc ABIETIC - abietic acid
TOC - total organic carbon 1SOP1MAR1C - isopimaric acid
DHA - dehydroabietic acid SANDARACO - sandaracopimaric acid
TOTXYLENE - total xylene 12CLDHA - 12-chlorodehydroabietic acid
14CLDHA - 14-chlorodehydroabietic acid
BUTBNZPH - butyl benzyl phthalate
NNP - N-nitrosodiphenylamine
H6 - mercury
AS - arsenic
CO - cadmium
PB - lead
Chemicals exceeding HAET for Puget Sound. More detailed information on exceedances is presented in Appendix J.
c DHA has no established AET, but was considered a problem chemical because concentrations exceeded EAR of 1,000. Stations with EAR >1,000 are noted in this table.
Chemicals exceeding LAET for Puget Sound. More detailed information on exceedances is presented in Appendix J. Chemicals shown in brackets exceeded 90th-percentile concentra-
tions for chlorinated phenols/guaiacols and/or resin acids.
e Crecelius et al. (1984).
f Battelle (1986).
9 Storer and Arsenault (1987).
h U.S. Army COE (1985).
1 Anderson and Crecelius (1985).
-------
Waterway problem area were somewhat patchy overall, but the highest concen-
trations occurred near Stations EW-04 and EW-07 (LPAH concentrations in this
area ranged from 17,000 to 100,000 ug/kg DW, including historical stations)
and at Stations EW-13 and EW-14. Naphthalene was typically the predominant
PAH in the East Waterway and, like 4-methylphenol, occurred at its maximum
concentration at Station EW-07 (17,000 ug/kg DW; EAR=3,000).
Many compounds strongly related to the pulp industry were observed at
elevated concentrations in the East Waterway problem area, especially at
Station EW-01 (at the head of the waterway), Station EW-04, and Station
EW-13. Relationships between certain observed chemicals and pulp industry
activities are discussed in the Results section. Stations EW-04 and EW-13
had the highest observed concentrations of DMA and abietic acid, the most
prevalent resin acids in the study (the highest concentrations of both resin
acids were between 80,000 and 100,000 ug/kg DW). Distribution patterns of
resin acids suggested that contamination at Stations EW-04 and EW-13 derived
from distinct sources of a similar nature; however, chlorinated compounds
were more prevalent at Station EW-04 than" at Station EW-13. Chlorinated
resin acid concentrations maximized at Station EW-04, as did 2-chlorophenol,
pentachlorophenol, 2-methylphenol, 2,4-dimethylphenol, most TIO compounds
(including compounds potentially related to resin acids, such as retene and
a diterpenoid hydrocarbon), and a number of other compounds (see Table 17).
Chlorinated phenols (dichloro- through tetrachloro-) and chlorinated
guaiacols had pronounced concentration maxima at the head of the waterway,
at Stations EW-01 and EW-02. Stations EW-02 and EW-03 (at the head of the
waterway) and EW-05 are not strictly included in the problem area (see
Figure 66), but are lower priority problem stations based upon the exceed-
ances of 90th percentile concentrations for various chlorinated phenols.
The contaminant assemblage at Station EW-14 was unique in the problem
area, as HAET were exceeded for copper (1,010 mg/kg DW), zinc (5,910 mg/kg
DW), and benzoic acid (5,900 ug/kg DW), as well as other problem chemicals
that were relatively widespread in the problem area (e.g., LPAH and 4-methyl-
phenol). Copper and zinc concentrations were over an order of magnitude
lower at other East Waterway stations.
268
-------
Distributions of conventional sediment variables were consistent with
distributions- of organic compounds that are likely related to pulp mill
activities. For example, TOC content was elevated in the East Waterway
overall, but particularly at Stations EW-04 and EW-13 (from 20 to 30 percent
TOC). Sulfides were highly concentrated (>7,000 mg/kg DW) at the head of
the waterway and at Station EW-04.
Problem Area NG
Problem Area NG was most extensively contaminated with polar organic
compounds (i.e., 4-methy1 phenol, benzoic acid, and to a lesser extent,
phenol), although relatively high concentrations of PAH and PCBs were
observed in localized areas (Table 38). Overall, distributions of different
contaminants were not consistent in this problem area. Of the problem
chemicals in this area, 4-methylphenol most often exceeded HAET [Table 38;
Stations NG-04, NG-05, NG-09, NG-10, NG-11, and NG-14 (intertidal)].
Station NG-05 had the highest 4-methylphenol concentration in this area
(9,700 ug/kg DW), with concentrations between 1,600 and 2,400 ug/kg DW at'
the other stations mentioned above. Concentration gradients of 4-methyl-
phenol were not apparent and the stations with the highest concentrations
were not all contiguous. For example, Stations NG-05 and NG-09 (2,400 to
9,700 ug/kg DW) were separated by a transect of four stations all with
concentrations <1,000 ug/kg DW. However, 4-methylphenol distributions
between the East Waterway and this problem area suggest a local source (or
sources) rather than transport from the more highly contaminated East
Waterway.
An area near the Mukilteo wastewater treatment plant and west of the
Mukilteo fuel depot had relatively high concentrations of several contami-
nants in addition to 4-methylphenol (particularly Station NG-09 and histori-
cal Station MUK-B). PAH concentrations were particularly elevated at
historical Station MUK-B (LPAH=11,000 ug/kg DW; HPAH=15,000 ug/kg DW). PAH
concentrations at Station NG-09 and NG-11 were within a factor of 2-3 of
these values, whereas PAH concentrations at NG stations east of NG-09 were
over 30 times lower. The PCS concentration at Station NG-09 (5,500 ug/kg DW)
269
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TABLE 38. NEARSHORE PORT GARDNER (NG) PROBLEM AREA3
Station
NG-14
NG-04
NG-05
NG-07
NG-08
NG-09
MUK-Bd
NG-10
NG-11
HAET Exceedances^
LPAH HPAH 4MEPHNL PHNL BNZACID
X
X
X X
X
X
X X
X
X
X
PCBS LAET Exceedances
PHNL
4MEPHNL
X LPAH
HPAH, PCBS
PHNL
PHNL, LPAH
a Chemical codes used in this table:
LPAH - Signifies AET exceedances for the sum of naphthalene, acenaphthylene, acenaph-
thene, fluorene, phenanthrene, and anthracene, or any of these compounds
individually. To simplify the presentation of AET exceedances in this table,
exceedances of AET for 2-methylnaphthalene are included under LPAH. This
compound covaried with LPAH but is not included in LPAH sums.
HPAH - Signifies AET exceedances for the sum of fluoranthene, pyrene, benzo(a)an-
thracene, chrysene, total benzofluoranthenes, benzo(a)pyrene, indeno(l,2,3-
cd)pyrene, dibenzo(a,h)anthracene, and benzo(g,h,i)perylene, or of any of
these compounds individually.
4MEPHNL - 4-methylphenol.
PHNL - Phenol.
BNZACID - Benzoic acid.
PCBS - Polychorinated biphenyls.
b Chemicals exceeding HAET for Puget Sound. More detailed information on exceedances is
presented in Appendix J.
c Chemicals exceeding LAET for Puget Sound. More detailed information on exceedances is
presented in Appendix J.
d Mai ins et al. (1985).
270
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exceeded the HAET, although nearby stations had concentrations (or detection
limits) that were over 25 times lower. The HAET for phenol was also
exceeded at Station NG-09 (2,100 ug/kg DW). Station NG-09 was also
somewhat enriched in TOC relative to other NG stations (3.8 percent TOC vs.
<0.8 percent at other NG stations).
Benzoic acid concentrations exceeded HAET at three stations offshore
from the Mukilteo fuel depot (Station NG-05, NG-07, and NG-08; 1,300 to
.2,100 ug/kg DW). A transect of stations was sampled in this area [moving
away from shore: Station NG-15 (intertidal), Station NG-06, Station NG-07,
and Station NG-08]. Notably, benzoic acid concentrations nearer shore (10
to 80 ug/kg DW) were considerably lower than at Stations NG-07 and NG-08
farther offshore.
Problem Area QG-Q1
The sole problem chemical at Station OG-01 was 4-methylphenol
(1,300 ug/kg DW)» Most other OG stations had similar 4-methylphenol
concentrations that were slightly below the HAET but above the LAET
(Stations OG-02 to OG-06; 720 to 1,200 ug/kg DW). Overall, this area was
characterized by very consistent concentrations of a number of chemicals,
including 4-methy1 phenol, PAH (dominated by naphthalene, as in the East
Waterway), resin acids (unchlorinated and chlorinated), and a cymene isomer.
These chemicals have varying degrees of association with the pulp industry
(e.g., of this group, resin acids are most strongly associated with this
industry). Although such chemicals could have been transported from the
East Waterway, several lines of evidence suggest that contamination derives
from the OG area itself (e.g., from the pulp industry discharge near
Station OG-03): (1) concentrations are consistent in the OG area, and do not
clearly decrease with distance from the East Waterway; (2) examination of
chemical contamination along a transect from Station EW-15 (at the mouth of
the East Waterway) to Station NG-01 (near Station EW-15) to Station OG-01
(further from Station EW-15) reveals that concentrations of several
diagnostic compounds (4-methylphenol, naphthalene, a cymene isomer, the
diterpenoid hydrocarbon TIO) decrease from Station EW-15 to NG-01 and then
increase at Station OG-01 (note that resin acids were not tested at
271
-------
Stations NG-01 and OG-01); and (3) contamination patterns, within the East
Waterway (i.e., prominent concentration maxima for certain chemicals) do not
suggest the presence of strong advection processes.
Problem Area SR-05
Station SR-05 was located on the Snohomish River near a kraft mill
facility. Benzoic acid and 4-methylphenol exceeded HAET at this station
(1,000 and 2,000 ug/kg DW, respectively). The 4-methylphenol concentration
at adjacent Station SR-04 exceeded the LAET (980 ug/kg DW). A number of
resin acids were detected at Station SR-05, including DHA and abietic acid
(3,500 and 2,300 ug/kg DW). Concentrations of these resin acids decreased
moving upriver from Station SR-05 to SR-03, and were roughly five times
lower at Station SR-04 than at Station SR-05 (although these two stations
had similar sediment texture). A chlorinated resin acid (12-chlorodehydro-
abietic acid) was detected below nominal detection limits at Station SR-04
(63 ug/kg DW).
Problem Area SO-03
Station SD-03, located on the Snohomish River delta near the East Water-
way, had concentrations of three chemicals exceeding HAET: benzoic acid
(770 ug/kg DW), benzyl alcohol (99 ug/kg DW), and p,p'-DDT (23 ug/kg DW).
The 4-methylphenol concentration at this station exceeded LAET (760 ug/kg DW).
Problem Area ES-Q3
Benzoic acid and 4-methylphenol exceeded HAET at this Ebey Slough
station (760 and 1,400 ug/kg DW, respectively). The LAET for phenol was
also exceeded at Station ES-03 (1,200 ug/kg DW, blank-corrected). Concen-
trations of benzoic acid and 4-methylphenol at Station ES-02 (upriver) were
at least 30 times lower than at Station ES-03.
272
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Problem flr.ea SD-01
Station SD-01 on the Snohomish River delta did not have any chemicals
exceeding AET; it was designated as a problem station based upon benthic
effects that exceeded action-level guidelines. EAR for Everett Harbor
problem chemicals did not exceed four at this station. Sediment at this
station was predominantly coarse-grained (<5 percent fine-grained material).
Problem Area SR-07
Station SR-07, located near the Everett marina on the Snohomish River,
was also designated as a problem station based upon benthic effects that
exceeded action-level guidelines; no AET were exceeded at this station.
However, TBT was reported at 0.093 mg/kg DW at this station, and the
sediment was very fine-grained (96 percent fine-grained material) and had a
high sulfide concentration (600 mg/kg DW) .
SUMMARY
Identification of Problem Areas
Broad areas of nearshore Everett Harbor and the lower
Snohomish River displayed low elevations of chemical concen-
trations in sediments relative to Puget Sound reference
areas. Because the area-wide indicators related to bioaccumu-
lation and pathology were not significantly elevated
(P>0.001), large-scale problem areas were not identified
throughout most of the study area.
Specific prpblem areas were defined on a finer spatial scale
(Tier II). Twenty-three stations were designated as problems.
Seventeen of these stations were grouped into the following
multi-station problem areas: East Waterway, and the nearshore
area from Elliott Point in Mukilteo east to Powder-mill Gulch.
273
-------
Ranking of Problem Areas
Ranking of Tier II problem areas showed that the East
Waterway was a higher priority than the Nearshore Port
Gardner problem area.
Ten stations were identified as the highest priority sites.
Of these, Stations EW-01, EW-04, and EW-07 scored >50 percent
for both chemical and biological variables.
Characterization of Problem Areas
East Waterway Problem Area--
Sediment contamination in this depositional area is extreme
and complex, and appears strongly related to pulp industry
discharges, although additional sources may be important for
some chemicals. The East Waterway problem area contained the
maximum sediment concentration of virtually every chemical
measured in this study, although maximum concentrations of
different chemicals occurred at different stations: Station
EW-01 (chlorinated guaiacols and dichloro- through tetra-
chlorophenols); Station EW-04 (certain chlorinated and
unchlorinated resin acids, some alkyl-substituted and
chlorinated phenols, most TIO compounds, and PCBs; this
station had the largest number of exceedances of HAET and
90th percentile concentrations in the study); Station EW-07
(4-methylphenol and naphthalene); Station EW-13 (certain
unchlorinated resin acids); and Station EW-14 (most PAH,
benzoic acid, zinc, copper, arsenic, and other metals).
The relationship between pulp industry activities and
sediment contamination was suggested by several lines of
chemical evidence, including distributions of distinctive
geochemical tracers (e.g., chlorinated resin acids and
chlorinated guaiacols) and related compounds (e.g., unchlor-
274
-------
inated resin acids, chlorinated phenols, retene, diterpenoid
hydrocarbons), as well as distributions of other compounds
potentially related to the pulp industry [e.g., 4-methylphenol
and naphthalene; refer to Tetra Tech (1985a) for a discussion
of the problem area at the mouth of St. Paul Waterway in
Commencement Bay, WA, where these chemicals were also
associated with a pulp mill discharge] and -TOC and sulfides
distributions.
Significant depressions in the abundances of benthic infaunal
taxa were found at all six stations sampled in the East
Waterway (P<0.001). Abundances of three of the four major
taxa analyzed were significantly reduced at Stations EW-01
and EW-07. Significant sediment toxicity to amphipods was
found at three of the six stations sampled in the East
Waterway (Stations EW-01, EW-04, and EW-07; P<0.001). The
mean amphipod mortality for all six stations was 2.9 times
the mean mortality at the Port.Susan stations.
Nearshore Port Gardner Problem Area--
The Nearshore Port Gardner problem area was primarily
contaminated with polar organic compounds (i.e., 4-methyl-
phenol, benzoic acid, and to a lesser extent, phenol),
although relatively high concentrations of PAH and PCBs were
observed in localized areas. Overall, distributions of
different problem chemicals were not consistent in this area.
Of the problem chemicals in this area, 4-methylphenol most
often exceeded HAET. Based upon observed distributions,
4-methylphenol contamination in this area probably derived
from undetermined local sources rather than transport from the
East Waterway.
In the Nearshore Port Gardner problem area, a significant
depression in the abundance of benthic taxa was found only at
Station NG-04 (Polychaeta; P<0.001). Mean mortality in the
275
-------
amphipod bioassay was 100 percent at Station NG-04 (P<0.001).
For Problem Area NG as a whole, the mean amphipod mortality
was approximately 1.7 times the reference value.
276
-------
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