Metal Concentrations (As, Cd, Cr, Pb, Hg and Se) in Dolly

METAL CONCENTRATIONS (AS, CD, CR, PB, HG AND SE) IN DOLLY

VARDEN (SALVELINUS MALMA) FROM THE ALEUTIAN ISLANDS, ALASKA

CHRISTIAN JEITNER

A thesis submitted to the

Graduate School-New Brunswick

Rutgers, The State University of New Jersey

in partial fulfillment of the requirements

for the degree of

Master of Science

Graduate Program in Ecology and Evolution

Written under the direction of

Joanna Burger

and approved by

______

New Brunswick, New Jersey

October 2009

ABSTRACT OF THE THESIS

METAL CONCENTRATIONS (AS, CD, CR, PB, HG AND SE) IN DOLLY

VARDEN (SALVELINUS MALMA) FROM THE ALEUTIAN ISLANDS, ALASKA

By CHRISTIAN JEITNER

Dissertation Director: Joanna Burger

Concerns about contaminants in fish have increased in recent years,

especially in species consumed heavily in subsistence diets. Most studies of

contaminants in Alaskan subsistence foods have focused on mainland Alaska not the Aleutian Islands. Several islands along the Aleutian Archipelago of Alaska have supported military bases which may be a source of pollution, and the proximity of the Aleutian chain to Eastern Asia may increase its susceptibility to atmospheric deposition of heavy metals. This study compares levels of arsenic, cadmium, chromium, lead, mercury and selenium in the egg, kidney, liver and muscle of Dolly Varden (Salvelinus malma) from Umnak, Adak, and Amchitka

Islands in the Aleutian Chain of Alaska. I examined levels as a function of tissue, gender, collection site, and size. There were significant differences in the levels of metals as a function of tissue, with kidney having the highest levels of arsenic and cadmium, and kidney and liver having significantly higher levels of chromium

ii and mercury than the other tissues examined. Selenium and arsenic in muscle

and liver were highly correlated with both length and weight of fish. Arsenic and mercury in muscle were highly correlated with levels in liver, kidney and egg.

There were few significant gender differences in metal concentrations, with females having higher levels of chromium in muscle and cadmium in kidney than males. However selenium in liver was higher in males than females. On

Amchitka mean mercury levels were higher in both muscle (149 ppb; ng/g, wet weight) and liver (321 ppb) compared to fish from Adak and Umnak (muscle = 24 ppb and liver = 44 ppb). Dolly Varden collected from Cannikin Lake and Fox Lake on Amchitka were probably not sea run. This may explain the elevated mercury levels found in Dolly Varden from Amchitka Island. Landlocked Dolly Varden feed more heavily on smaller fish and fish eggs which places them at a higher trophic level than anadromous fish which primarily feed on amphipods. Selenium levels were highest in muscle (761 ppb) and liver (1,860 ppb) of fish caught in Cannikin

Lake on Amchitka Island. Overall, concentrations of the metal contaminants in

Dolly Varden were relatively low when compared with other studies on anadromous and marine fish from the region, and differences among collection sites may be due to trophic level differences between landlocked (Cannikin Lake) and sea-run Dolly Varden.

iii Acknowledgements

This work was conducted under the advisement and guidance of Dr.

Joanna Burger. I owe gratitude for both her encouragement and instruction. Also

my appreciation to Dr. Michael Gochfeld, and Dr. Keith Cooper, as members of a

helpful thesis committee. I also thank Dr. Judith Weis for providing comments

and guidance, Tara Shukla for assistance with metals analysis, Sean Burke,

Timothy Stamm, Ronald Snigaroff, Daniel Snigaroff, and Conrad Volz for assistance catching and dissecting fish. I thank the people who contributed to the

development and execution of the Amchitka Science Plan including Charles

Powers, David Kosson, Robert Patrick (Aleutian/Pribilof Island Association), and

the people of the villages of Nikolski, and Adak in the Aleutians. The research

was conducted under an approved Rutgers University Protocol, and supported

by NIEHS Center grant (P30ES005022), Consortium for Risk Evaluation with

Stakeholder Participation (Department of Energy, # DE-FC01-95EW55084, DE-

FG 26-00NT 40938), Wildlife Trust and EOHSI.

iv Table of Contents

Title Page ...... i

Abstract ...... ii

Acknowledgements ...... iv

Table of Contents ...... v

List of Tables ...... vii

List of Figures...... viii

1.0 - INTRODUCTION...... 1 1.1 Research Objectives...... 2 1.2 Bioaccumulation In Marine Organisms ...... 3 1.2.1 Arsenic ...... 4 1.2.2 Cadmium...... 6 1.2.3 Chromium...... 7 1.2.4 Lead ...... 8 1.2.5 Mercury ...... 9 1.2.6 Selenium ...... 11 1.3 Dolly Varden Life Cycle...... 13 1.4 Importance Of Dolly Varden...... 14 1.5 Human Health Risks From Eating Fish ...... 15

2.0 - METHODS ...... 17 2.1 Study Sites...... 17 2.1.1 Umnak Island ...... 17 2.1.2 Adak Island ...... 18 2.1.3 Amchitka Island...... 19 2.2 Field Procedures...... 20 2.3 Laboratory Analysis ...... 21 2.4 Statistical Analysis ...... 22

3.0 - RESULTS...... 24 3.1 Factors Contributing to Models ...... 24 3.2 Interisland Differences ...... 24 3.3 Metal Correlations...... 25 3.4 Tissue Correlations...... 26 3.5 Gender Differences...... 27

4.0 - DISCUSSION ...... 28 4.1 Locational Differences ...... 28 4.2 Size-Metal Relationships ...... 32

v 4.3 Tissue Differences ...... 34 4.4 Gender Differences...... 38 4.5 Geographical Comparisons ...... 39 4.6 Risk To Human Consumers...... 44 4.7 Risk To Wildlife Receptors...... 50 4.8 Conclusion ...... 54

Literature Cited ………………………………………………………………………..56

vi Lists of tables

Table 1. Multiple regression models on log transformed data for differences in levels of metals in Dolly Varden collected from the Aleutians...... 77

Table 2. Metal levels in muscle and liver of Dolly Varden collected from 3 islands in Alaska...... 78

Table 3. Metal levels in kidney and egg of Dolly Varden collected from 3 islands in Alaska ...... 79

Table 4. Correlation of size and contaminant levels in Dolly Varden from the Aleutians ...... 80

Table 5. Correlation between tissues for contaminant levels… ...... 81

Table 6. Contaminant levels in 4 organs (egg, kidney, liver, muscle) of Dolly Varden ...... 82

Table 7. Gender differences in Metal levels of Dolly Varden muscle, liver and kidney ...... 83

Table 8. Risk evaluation for human consumption of Dolly Varden from the Aleutians ...... 84

Table 9. Percent of Dolly Varden muscle samples above regulatory action levels…...... 85

vii List of figures

Figure 1. Map showing the islands where Dolly Varden were collected...... 86

Figure 2. Map showing the location of Dolly Varden collection on Adak...... 87

Figure 3. Map showing the locations of Dolly Varden collection on Amchitka .. 88

Figure 4. Map showing the location of Dolly Varden collection on Umnak ...... 89

Figure 5. Arsenic levels in Dolly Varden muscle by standard length ...... 90

Figure 6. Cadmium levels in Dolly Varden muscle by standard length ...... 91

Figure 7. Chromium levels in Dolly Varden muscle by standard length...... 92

Figure 8. Lead levels in Dolly Varden muscle by standard length ...... 93

Figure 9. Mercury levels in Dolly Varden muscle by standard length ...... 94

Figure 10. Selenium levels in Dolly Varden muscle by standard length ...... 95

viii 1

1.0 INTRODUCTION

There is a need for current information on metal levels in biota due to environmental disturbances associated with industrialization and global atmospheric transport. Concentrations of metal pollutants are likely to rise with increasing industrial emissions in Asia and monitoring is crucial as contaminants continue to accumulate through atmospheric deposition (Duce 1998; Pacyna and

Pacyna 2000). Metal concentrations in fish from the Aleutian Islands have received relatively little attention (Hall et al. 1976; Zhang et al. 2001; Burger et al.

2007a; Burger et al. 2007b; Burger et al. 2007c). Dolly Varden belong to a group of salmonid fish called char and are sought after by both subsistence and recreational anglers. A few studies have been conducted for contaminants, mainly mercury, in Dolly Varden, but most deal with fish populations near specific point sources such as mines and smelters (Deniseger et al. 1990; Gray et al.

2000). Many studies on metal concentrations in subsistence diets have dealt with marine mammals (Lockhart et al. 1992; Krone et al. 1999). Contaminants in wildlife are of greatest concern to remote populations in Alaska who rely on subsistence fishing. Between 30-90% of the diets of Aleuts consists of subsistence food because commercial foods are expensive and in remote villages grocery stores are poorly stocked or inaccessible (Patrick 2002).

1.1 RESEARCH OBJECTIVES

This paper examines the levels of arsenic, cadmium, chromium, lead, mercury, and selenium in the liver, kidney, muscle and eggs of Dolly Varden

(Salvelinus malma) from Umnak, Adak, and Amchitka Islands in the Aleutians

(Fig 1). The objectives of this research were 1) to compare levels in fish among locations and between genders; 2) to determine whether there were differences in metal levels as a function of fish size; 3) to determine whether there were differences in metal levels as a function of tissue; 4) To compare metal levels in fish with levels reported in other studies; 5) to determine whether metal levels in fish pose a risk to wildlife or people consuming them. All fish from Adak and

Umnak were collected by Aleuts at locations commonly fished by residents for food.

1.2 BIOACCUMULATION IN MARINE ORGANISMS

Metal contaminants enter freshwater and marine environments from

natural and anthropogenic sources. The amount of naturally occurring metals

released to the environment has increased due to human activities. In some

areas the levels of metal pollutants entering the environment may be harmful to

consumers, including humans. Chemicals must be in a bioavailable form in order

to produce toxic effects to an organism. This means that it must be able to move through or bind to an organism’s surface coating such as skin, gill, or gut

(Newman and Jagoe 1994), and must be absorbable from the environmental medium. Metals may bioaccumulate in organisms if they have a higher affinity for a tissue in the organism than for water (Neff 2002).

Most naturally occurring metals and metalloids are found in fish tissues at higher concentrations than ambient seawater (Neff 2002). Weathering and erosion of crustal rocks can be an important natural source of metals in marine ecosystems. In areas where anthropogenic inputs are low the concentration in fish tissues may represent natural background concentrations and are probably not toxic to organisms or their consumers (Neff 2002).

Bioaccumulation is the uptake and retention of a chemical from any possible external source (Neff 2002). For this to occur, the rate of uptake must be

greater than the rate of loss. If an organism is continually exposed to a chemical

a state of equilibrium may be reached where the rate of uptake is equal to the

rate of loss. The equilibrium concentration of a chemical in the tissues of a

marine organism can be measured as the bioaccumulation factor (BAF). This is

the ratio of the sum of uptake rate to the sum of the release rate (Farrington and

Westall 1986). Bioconcentration is a special case of bioaccumulation where

uptake of a chemical is from water alone and other sources of uptake are not

considered.

Most metal ions can cross biological membranes (skin, gut, and gills) of

marine organisms by passive diffusion down a concentration gradient (Simkiss

and Taylor 1989). Biomagnification may occur if a chemical increases in

concentration in the tissues of animals at increasing trophic levels. With

biomagnification the transfer of contaminants occurs primarily in the gut of the consumer where contaminants are absorbed from the food and transferred to the tissues of the consumer (Neff 2002). Eventually the concentration of the

chemical in the consumer will exceed levels found in prey items. The

biomagnification factor is the ratio of the concentration of a contaminant in the

tissues of the consumer to its concentration in the food (Leblanc 1995). Generally

most inorganic forms of metals do not biomagnify in marine food webs (Brown

and Neff 1993).

1.2.1 ARSENIC

Anthropogenic sources of arsenic include smelters, refineries, coal

burning, manufacturing, waste incineration, and mining. Deposition is an

important source of arsenic to the ocean (Jickells 1995). Arsenate, As(V), is the

dominant form of inorganic arsenic in seawater (Byrd 1990) and can make up

5 between 1.6% and 13.2% of total arsenic in surface waters of the continental shelf of the United States (Andreae et al. 1983).

Most marine organisms do not readily bioaccumulate inorganic arsenic from seawater or food (Francesconi and Edmonds 1997). Marine plants can bioaccumulate inorganic arsenic and transform it to an organic form (Vidal and

Vidal 1980; Sanders 1983). Organic forms of arsenic can be bioaccumulated by marine animals (Edmonds et al. 1992), however this form is not toxic or carcinogenic to marine animals or consumers (Vahter et al. 1983; Sabbioni et al.

1991). Both marine mammals and terrestrial mammals are able to excrete organic arsenic ingested in their food (Meador et al. 1993; Zeisler et al. 1993).

The organic form arsenobetaine is the most abundant form of arsenic in the tissues of most marine animals and can represent 50% to 95% of the total arsenic in fish (Francesconi and Edmonds 1993).

Inorganic arsenic is more toxic to marine plants than marine animals, but usually accounts for less than 1.0% of the total arsenic found in the muscle of marine fish (Edmonds and Francesconi 1993). Total arsenic concentrations are generally higher in muscle of demersal fish than in pelagic species (Burger et al.

2007a; Neff 2002). Inorganic arsenic is generally found at concentrations below

500 ppb wet weight in fish muscle from unpolluted marine environments

(Edmonds and Francesconi 1993). Therefore, arsenic levels found in most edible portions of fish are below the EPA critical value for human consumption in fish of

1,000 ppb wet weight.

1.2.2 CADMIUM

Cadmium occurs naturally in the earth’s oceans and crust and can be released through erosion and volcanic eruptions. Anthropogenic sources of cadmium include fertilizers, combustion of fossil fuels, and production of iron and steel (Van Assche, 1998). Cadmium levels in Greenland snow peaked in the

1960’s, but has steadily declined, suggesting a decline in atmospheric levels due to improved technology for pollution control and disposal (Boutron et al. 1991).

Cadmium may enter the aquatic ecosystem from atmospheric deposition and may be absorbed directly by fish and invertebrates from the water (AMAP

1998). Upwelling may be an important source of cadmium in marine organisms, particularly in Antarctica (Bargagli et al. 1996). Cadmium is soluble in water as chloride and sulfate salts. The oceans contain about 68 million metric tons of cadmium (Bryan 1976). Much of the cadmium entering the oceans may be of anthropogenic origin (Grousset et al. 1995).

Mean concentrations of cadmium in the open ocean range from 1 to 100 ng/L, however levels as high as 5,000 ng/L have been reported in estuaries receiving drainage from metal mining areas (Klumpp and Peterson 1979;

Schuhmacher et al. 1995). Cadmium is most bioavailable in the form of Cd+2, however this form of cadmium usually represents less than 3% of the total dissolved cadmium in seawater (Mason et al. 1988; Fernando 1995). The form of cadmium present in the ocean may be influenced by biological activity of phytoplankton (Kudo et al. 1996). Food may be the main source of cadmium in marine fish (Ni et al. 2000). There does not appear to be a trend of cadmium

concentrations based on trophic level (Neff 2002) suggesting that cadmium may

not biomagnify in marine organisms.

1.2.3 CHROMIUM

Chromium occurs naturally in rocks and topsoil but is also released from

the combustion of fossil fuels and from steel production. Treated domestic sewage, electroplating factories, and leather tanneries may also be important

sources of chromium. Trivalent chromium, Cr (III) is an essential trace nutrient,

but hexavalent chromium, Cr (VI) may be an important environmental

contaminant because of its carcinogenicity, toxicity, and potential to be mobilized

by anthropogenic activities (Iyengar 1991). Most of the chromium in the oceanic

surface waters is hexavalent chromium, Cr (VI) (Van der Weijden and Reith

1982). Chromium (VI) can be reduced by marine organisms to chromium (III)

(Nakayama et al. 1981). Concentration of total dissolved chromium in the ocean

surface ranges from 100 to 550 ng/L and usually decreases with depth (Murray

et al. 1983; Mayer 1988; Ciceri et al. 1992).

There is relatively little published data on the bioaccumulation of

chromium by marine organisms. As an essential micronutrient, most marine

organisms have developed mechanisms for accumulating chromium from water

and food (Simkiss and Taylor 1989). Chromium (III) is bioavailable to infaunal

invertebrates and sediment bacteria (Loutit and Pillidge 1986; Bremer and Loutit

1986). Chromium shows no clear relationship between trophic level and body

burden and is not likely to biomagnify in marine food webs (Neff 2002).

1.2.4 LEAD

Lead enters the ecosystem mainly through atmospheric deposition and may enter the food web through primary production and low trophic level organisms (Duce 1998). An estimated 89,100 tons of lead enter the oceans annually from atmospheric deposition (Jickells 1995). This is largely derived from the burning of leaded gasoline and metal smelters (Veron et al. 1998).

Concentrations of lead in the atmosphere have decreased in recent years with the removal of lead gasoline in North America (Veron et al. 1998).

Concentrations of lead in ocean surface waters range from 2 to 200 ng/L

(Neff 2002). Usually less than 5% of the inorganic lead in seawater is in the free ionic form which is considered the most bioavailable and toxic species of inorganic lead (Freedman et al. 1980). Marine fish are able to bioaccumulate lead from seawater (Talbot 1987). In invertebrates lead may be stored in various tissues, usually the kidney or hepatopancreas, as metal-rich granules which have limited bioavailability to the animal or its predators (Nott and Nicolaidou 1994;

Regoli and Orlando 1994).

Freshwater fish may be able to bioaccumulate lead from water across the gills (Tao et al. 1999). Most marine organisms primarily accumulate lead from the water and lead is not transferred efficiently through the marine food chain (Szefer

1991), however lead may be transferred more efficiently from marine animals to mammalian consumers (Regoli and Orlando 1994). Regoli and Orlando (1994) found that lead in mussels may be present mostly in the form of non-bioavailable

metal granules, but when these mussels are fed to mice some of the lead is

bioaccumulated. In Greenland, mussels had higher lead levels than fish,

seagulls, and ringed seals from the same ecosystem (Dietz et al. 2000). Smith et

al. (1990) studied lead in sea otters (Enhydra lutris) from the Aleutian Islands and

found that concentrations of lead have not increased in otter tissues due to

industrialization, but the source of the lead has changed from volcanic rocks to

Asian and Canadian industrial sources. These studies indicate that lead is not biomagnified through the marine food chain and often highest concentrations of lead are found at the lowest trophic levels.

1.2.5 MERCURY

Mercury is contained in rock and can be released naturally through degassing of the earth’s crust, volcanoes, and erosion. Anthropogenic activities such as coal burning, trash incineration and industrial emissions have increased the release of mercury into the environment (EPA 1998). Anthropogenic releases of mercury to marine and fresh waters may amount to 600 to 8,800 metric tons/year (Lindberg et al. 1987). As much as 70% to 80% of the total anthropogenic emissions to the atmosphere comes from the burning of fossil fuels and waste incineration (Pacyna and Keeler 1995). The oceans contain a total of approximately 68 million metric tons of mercury (Bryan 1979).

Mercury is methylated by microorganisms in fresh and marine sediments

(Olson and Cooper 1976; Gagnon et al. 1996). Methylmercury (MeHg) is bioaccumulated more readily than inorganic mercury (Mason et al. 1995; Wood

1987). Organic mercury complexed with organic matter in sediment is highly bioavailable (Gagnon and Fisher 1997). Methylmercury enters the food web in sediment dwelling marine organisms and is bioaccumulated by higher trophic level animals (Neff 2002). Methylmercury may also be released much slower from tissues of marine organisms than inorganic mercury (Trudel and

Rasmussen 1997). This may explain why older marine animals tend to have higher levels of methylmercury (Thompson 1990). Naidu et al. (2001) reported mean total mercury and methylmercury levels of 7 ppb in Dolly Varden muscle samples, indicating that nearly 100% of total mercury in Dolly Varden muscle is organic.

Levels of total mercury in the North Atlantic range from 0.10 to 0.50 ng/L

(Guentzel et al. 1996). In the ocean, the concentration of organic mercury tends to increase with depth. This is probably due to the oxidation of organic mercury to elemental mercury by aerobic bacteria in oxygenated surface waters (Rolfhus and Fitzgerald 1995). Much of the mercury in hypoxic marine sediments is not bioavailable to benthic animals (Schaanning et al. 1996). Methylmercury and total mercury may both biomagnify in marine food webs (Bargagli et al. 1998), however as trophic level increases a greater percentage of total mercury is often methylmercury (Schafer et al. 1982; Neff 2002).

Mercury concentrations increased from lowest to highest trophic level in a study of the Aleutian food web (Burger et al. 2007c). In their study, four species of marine algae had mercury levels below 5 ppb and nine species of invertebrates had mercury levels ranging between 5 and 101 ppb. They tested 15

11 species of fish, with the lowest levels found in sockeye salmon (Oncorhynchus nerka), with a mean of 42 ppb. In fish the highest mercury levels were found in marine bottom fish, with great sculpin (Myoxocephalus polyacanthocephalus) having a mean mercury concentration of 366 ppb.

In Antarctica, Bargagli et al. (1998), found a similar trophic level increase with phytoplankton < zooplankton and benthic primary consumers < detritivorous and opportunistic benthic invertebrates < epipelagic fish < demersal fish and plankton feeding seabirds < fish eating penguins < predatory birds < seals.

Similarly, mercury in the pelagic food chain off of California increased with increasing trophic level with krill < fish < marine birds < marine mammal

(Sydeman and Jarman 1998).

1.2.6 SELENIUM

Selenium is technically a metalloid and is an essential micronutrient in animals (Eisler 2000). It is a widely distributed mineral that can be found in most rocks and has several industrial uses including electronics, glass, plastics, and paints. It is released to the environment both naturally and during the combustion of fossil fuels. Selenium levels have been found in harmful levels in cooling reservoirs near coal-fired power plants (Lemly 1996, Baumann and Gillespie

1986) and uranium and coal mines (Casey & Siwik 2000). Selenium is found in a wide verity of foods including fruits, vegetables, grains, nuts, dairy products, meats, and poultry (Schubert et al. 1987). The highest levels found in foods are

12 in Brazil nuts, with a mean of 14,700 ppb and a maximum over 250,000 ppb

(Schubert et al. 1987; Secor and Lisk 1989).

Selenium enters the aquatic environment from atmospheric deposition and soils and uptake by biota can occur from water or diet (ATSDR 2003). Sodium selenate is among the most mobile forms of selenium because of its high solubility and inability to adsorb to soil particles (Klaassen et al. 1986; ATSDR

2003). Selenium is a primary element of concern because it is easily transferred from water and sediment to aquatic plants and invertebrates, and may bioaccumulate in higher trophic level organisms (Furr et al. 1979). It has been detected in oceans at an average of 90 ppb (Schutz and Turekiam 1965) and benthic bacteria and fungi are capable of methylating elemental and inorganic selenium salts (Chau et al. 1976).

Selenium can be accumulated by aquatic organisms (Rudd and Turner

1983; Saiki and Lowe 1987) and transfer in fish can occur in the gills, epidermis, or gut, however dietary exposure may be more important (Dallinger et al. 1987).

Selenium biomagnifies in aquatic organisms with: fish > benthic insects > annelids > molluscs and crustaceans > periphyton (Ohlendorf et al. 1986a).

Selenium is thought to be protective for mercury exposure (Satoh et al. 1985;

Bjorkman et al. 1995).

1.3 DOLLY VARDEN LIFE CYCLE

Dolly Varden belong to a group of salmonid fish called char and were once thought to be a variety of Arctic char (Salvelinus alpinus). It wasn’t until the

1950’s that Dolly Varden was formally recognized as a distinct species, although this remains controversial and some Russian ichthyologists still do not accept this. In 2001 U.S. Fish and Wildlife Service proposed listing Dolly Varden as threatened in Washington State because it has a similar appearance to bull trout

(Salvelinus confluentus), which is listed as threatened. This was suggested because even law enforcement personnel have difficulty differentiating between the two species.

Dolly Varden are generally anadromous, breeding in fresh water, moving to coastal waters in late May or June, and returning to overwinter in freshwater prior to freeze-up (Craig and McCart 1976). Craig (1989) described Dolly Varden as facultative anadromous because the entire population does not necessarily migrate to coastal waters. Some males in a population may remain in streams for the duration of their lives, never reaching the large size of sea run fish, but they still participate in spawning (McCart 1980). Coastal waters may contain Dolly

Varden from many different natal streams (Underwood et al. 1995). When feeding in coastal waters, Dolly Varden from the Aleutian Islands generally remain within 1 km of the island where they spawn (Valdez et al. 1977).

Dolly Varden remain in streams for several years before entering coastal waters for about 1.5-2.5 months each summer to feed (Craig 1989). While at sea their abundances may be associated with invertebrate abundances (Cannon et

14 al. 1987). They usually reach maturity at age 5 or 6 after having spent 3 to 4 summers at sea. Once reaching maturity, Dolly Varden return to spawn in the stream from which they originated (Alaska Department of Fish & Game 2006).

Due to damage inflicted while fighting, males suffer a high mortality rate after spawning and only about 50% live to spawn a second time (Alaska Department of Fish & Game 2006). On Amchitka spawning peaks between October and

November (Valdez et al. 1977). Eggs develop slowly in the cold water and hatching occurs four to five months after fertilization (Alaska Department of Fish

& Game 2006). Dolly Varden live about 8 years, reaching 46-91 cm and may weigh up to 18 kg (Eschmeyer et al. 1983). In coastal waters the primary prey of anadromous fishes are mysids and amphipods, which often make up over 90% of their diet (Craig 1989).

1.4 IMPORTANCE OF DOLLY VARDEN

Dolly Varden are an important resource for many residents of Alaska, and in some Alaskan communities can make up over 80% of the subsistence fish catch (U.S. Fish & Wildlife Service 2005). They were once thought to be a trash fish and there was a bounty put on their tails for supposedly eating salmon fry and eggs. After nearly 6 million were killed between 1921 and 1940 the U.S.

Bureau of Fisheries discovered most of the tails submitted for the bounty were from trout and coho salmon so the program was terminated. They are now an important sport fish throughout Alaska, thriving in small and medium size streams

15 that enter saltwater. Their popularity as a sport fish is increasing as restrictions are placed on salmon.

In this study all Dolly Varden from Adak and Umnak, and 75% of the fish from Amchitka, were caught by Aleut fishermen. In the villages of Adak and

Nikolski (Umnak Island) one or two fishermen often catch them by rod and reel and distribute them to other residents. A study in False Pass, Alaska found that

75% of residents ate Dolly Varden, and sharing was common, with 50% receiving

Dolly Varden from other residents (Fall et al. 2006). In addition to the species importance to human consumers, Dolly Varden are an important source of energy exchange between the marine environment and freshwater ecosystems

(Neuhold and Helm 1971) and are consumed by birds including Bald Eagles

(Haliaeetus leucocephalus) (Anthony et al. 1999).

1.5 HUMAN HEALTH RISKS FROM EATING FISH

Fish are a low-fat source of protein and are high in omega-3 fatty acids that reduce cholesterol levels (Daviglus et al. 2002). However levels of contaminants in some fish are high enough to potentially affect the fish themselves or top-level predators consuming them (Stern 1993; NRC 2000).

Salmonid species are considered a healthy choice because they are generally high in omega-3 fatty acids and low in contaminants (Dewailly et al. 2007). The primary contaminants of concern in fish are polychlorinated biphenyls (PCBs) and methylmercury, which in some species are above levels known to cause adverse health effects in people consuming large quantities (Stern 1993; NRC

2000; Hites et al. 2004; Burger et al. 2005a). Fish consumption is the only significant source of methylmercury exposure for the public (Rice et al. 2000) and communities consuming large quantities of fish may be at risk from chronic exposure to methylmercury (Grandjean et al. 1997).

2.0 METHODS

2.1 STUDY SITES

Geographically the Aleutian Islands span from North America to Asia, and

are the defining border between the North Pacific and the Bering Sea (Fig 1).

This region supports one of the world’s most productive fisheries and local populations rely heavily on subsistence fishing. This region is extremely remote,

far from industrial or agriculture activities. Several of the islands in the Aleutian

chain have a history of intensive military activity which are potential sources of

contamination (ATSDR 2002). Many of these military sites in Alaska were

abandoned once military operations ceased and remain contaminated due to the

high cost of transporting waste from remote locations (U.S. Fish & Wildlife

Service 2000).

2.1.1 UMNAK ISLAND

Umnak Island, part of the Fox Island group, is located 1,450 km southwest

of Anchorage. The town of Nikolski is located on Nikolski Bay on the southwest

end of Umnak Island. Nikolski currently has about 50 Aleut residents and is the

oldest continuously inhabited village in North America, with over 4,000 years of

virtually continuous occupation. Archaeological evidence from Ananiuliak Island

north of Nikolski Bay dates as far back as 8,500 years (Beringsea.com 2006). In

1941, Fort Glen Naval Base was established on Umnak Island at Otter Point. In the 1950’s the Air Force constructed a White Alice radar communication site on

Umnak, which was abandoned in 1977. The island has a runway that is owned

18 by the U.S. Air Force. Residents of Nikolski rely heavily on subsistence foods including fish, birds, and marine mammals (Beringsea.com 2006).

2.1.2 ADAK ISLAND

Adak Island is located approximately 1,850 km west-southwest of

Anchorage, Alaska, and is the westernmost town in the United States. It has been in the National Wildlife Refuge system since 1913 (ATSDR 2002). Adak has been the site of military activity since the beginning of the United State’s involvement in World War II in 1942. Naval Air Facility Adak, located on the northern half of the island once stationed over 6,000 military personnel

(Beringsea.com 2007). In 1997 this facility closed and was traded to the Aleut

Corporation for lands located throughout the Aleutian Islands (ATSDR 2002;

Beringsea.com 2007).

In 1994 the island was placed on the U.S. Environmental Protection

Agency’s National Priorities List as a Superfund site after approximately 185 chemically-contaminated sites were identified (U.S. Navy et al. 1999). The Navy has spent over $200 million on chemical contamination remediation issues on

Adak. Adak currently has fewer than 300 residents, most residing in the town of

Adak, which is located between the airport and Kuluk Bay. The Adak Fisheries

Development Council (AFDC) is currently processing crab, cod, halibut and other bottom fish and has plans to expand the islands commercial fishery (Adak Island

2007).

2.1.3 AMCHITKA ISLAND

Amchitka is located in the Rat Island group, approximately 2,150 km west

southwest of Anchorage, Alaska. In the 1940’s the United States built three

runways on Amchitka which were used heavily until the end of World War II

(University of Alaska Fairbanks 2004). Amchitka supported over 13,000 United

States Air Force personnel throughout World War II. Between 1950 and 1961

Amchitka was used in the Distant Early Warning network (University of Alaska

Fairbanks 2004). Amchitka was used as a nuclear test site for the Vela Uniform

Program. Project Long Shot, an 80 kiloton blast, was detonated in 1965 at a

depth of 710 meters. Project Milrow, detonated in 1969, had a yield of 1,000

kilotons. Project Cannikin, the largest underground nuclear test ever conducted

by the United States, was a test of the Spartan missile warhead. Cannikin was

detonated in 1971 at a depth of 1,791 meters (University of Alaska Fairbanks

2004). With a yield of 5,000 kilotons (5 megatons), this test caused faulting which

dammed White Alice Creek, filling portions of the explosion cavity and collapsed

chimney, forming Cannikin Lake (Gonzalez et al. 1974). Between 1986 and 1993

Amchitka Island was used for construction and operation of Relocatable Over the

Horizon Radar (University of Alaska Fairbanks 2004).

In the late 1990s a major environmental demolition and remediation was

conducted in which many of the remaining military buildings were removed. In

2001 the DOE began capping twelve mud pits designed to hold drilling mud

produced during the excavation of holes for underground atomic testing (Giblin et al. 2002). During this process water was pumped off of the mud pits to provide

20 access to drilling mud. The water being removed was treated to comply with

Alaska Department of Environmental Conservation discharge standards before being released to a nearby body of water. Once the water was removed the DOE filled the pits with soil from other areas on the island and capped the soil to isolate drilling mud from the environment. Finally the geosynthetic liner was buried with soil and revegetated with native seeds.

Today Amchitka is uninhabited, but potential fish consumers include crewmen from passing vessels, on-site workers, and Aleut fishermen and/or hunters (Department of Energy / Nevada Operations Office 2001).

2.2 FIELD PROCEDURES

Under appropriate permits from the State of Alaska’s Department of Fish and Game (CF-04-034), Dolly Varden were collected from three islands in the

Aleutians (Umnak, Adak, and Amchitka; Fig 1). Dolly Varden were collected by rod and reel in June and July 2004 on Adak and Amchitka Islands and in May

2005 on Umnak Island. On Adak, they were caught by an Aleut resident in

Sweeper Creek (N 51.856; W 176.654) which is located at the base of the airport runway and flows into Sweeper Cove (Fig 2). Fish from Amchitka were collected from Fox Lake (N 51.39; E 179.28), located at the base of Fox Runway which was used heavily during World War II (Fig 3). Fox Lake was connected to the sea by a shallow stream flowing into Constantine Harbor. Fish were also collected on

Amchitka from Cannikin Lake (N 51.47; E 179.11), a landlocked lake which was formed by the 1971 underground atomic test. On Umnak fish were collected from

Sheep Creek (N 52.96; W 168.84), near the town of Nikolski by an Aleut resident

(Fig 4).

Over 80% of all fish in this study were caught by Aleut fishermen. When collecting Dolly Varden, researchers also fished in the same manner and places as the Aleut fishermen. Samples from Umnak and Adak were collected only for this study, but samples from Amchitka were part of research by the Consortium for Risk Evaluation with Stakeholder Participation (CRESP) to examine radionuclide levels in marine biota for the Department of Energy (Powers et al.

2005; Burger et al. 2007d). Dolly Varden were immediately measured (standard length), weighed, dissected, and sexed. Samples of muscle and liver were taken from all 75 fish, however only 43 fish had kidneys that were large enough to analyze. Eggs were taken from the 27 gravid females out of 32 total females.

Samples were frozen and shipped to the Environmental and Occupational Health

Sciences Institute (EOHSI) of Rutgers University for metal analysis.

2.3 LABORATORY ANALYSIS

At EOHSI, a 2.0 g (wet weight) sample of fish tissue was digested in

Ultrex ultrapure nitric acid in a microwave (CEM, MDX 2000), using a digestion protocol of three stages of ten minutes each under 50, 100, and 150 pounds per square inch (3.5, 7, and 10.6 kg/cm2) at 70X power. Digested samples were subsequently diluted to 25 ml with deionized water. All laboratory equipment and containers were washed in 10% HNO3 solution and rinsed with deionized water prior to each use.

Mercury was analyzed by cold vapor technique using a Perkin Elmer

FIMS-100 mercury analyzer, with an instrument detection level of 4 ppb, and a method detection level of 10 ppb. Total arsenic, cadmium, chromium, lead, and selenium were analyzed using a Perkin Elmer 5100 graphite furnace atomic absorption spectrometer with Zeeman correction. Concentrations are expressed in parts per billion (ppb=ng/g) on a wet weight basis. Values are for total mercury, not methylmercury, but in most species about 90% of total mercury is methylmercury (Bloom 1992). DORM-2 certified dogfish muscle, provided by the

National Institute of Standards and Technology (NIST), was used as a reference material. Recoveries between 90-110% were accepted to validate the calibration.

All specimens were run in batches of 24 that included 2 blanks, one spiked specimen, and one duplicate specimen. The accepted recoveries for spikes ranged from 85% to 115%. No batches were outside of these limits.

2.4 STATISTICAL ANALYSIS

For analysis, concentrations below the method detection level were replaced with half the detection limit. Kruskal Wallis non-parametric one way analysis of variance (generating a X2 statistic) was used to examine differences among tissues, genders and sites (SAS, version 9.1, 2005). ANOVA with Duncan

Multiple Range test was used on log-transformed data to identify the significant differences. Kendall-tau correlations were used to examine relationships among metals, length, weight, and organs. Tables 2, 3, 6, and 7 provide geometric as well as arithmetic means for comparison with other studies.

Multiple regression procedures were used to determine if location, length,

weight or organ contributed to explaining the variations in concentrations of

metals. Multiple regression determines which independent variables are being

used to explain the variation in a single dependent variable. R2 determines how

well the independent variables explain the variation in the dependent variable.

The level for significance was designated as P < 0.05. Finally I evaluated potential risk based on levels found in Dolly Varden and the U.S. Environmental

Protection Agency’s (EPA) reference dose.

3.0 RESULTS

3.1 FACTORS CONTRIBUTING TO MODELS

Regression models indicated that between 8% and 81% of the variation in

levels of arsenic, cadmium, chromium, lead, mercury, and selenium in Dolly

Varden were explained by island (all metals except chromium and selenium),

length (arsenic, lead, and mercury), weight (cadmium, chromium, mercury, and

selenium), and organ (all metals; Table 1). The best regression models

accounted for 48% (r2 = 0.48) of the variation in arsenic using island and organ,

while 81% of the variation in cadmium was explained by island, weight and

organ, and 38% of the variation in chromium was explained by weight and organ.

The best regression models accounted for only 8% of the variation in lead levels

using island, length and organ, while 62% of the variation in mercury was

explained by island, length, weight, and organ, and 43% of the variation in

selenium was explained by weight and organ.

3.2 INTERISLAND DIFFERENCES

There were significant interisland differences in the weight and standard

length of Dolly Varden. The longest fish were from Umnak, while the heaviest were caught in Cannikin Lake on Amchitka Island (Table 2). Fox Lake on

Amchitka Island had the smallest fish (both shortest and lightest).

There were significant interisland differences for metals in muscle, liver,

kidney and egg. Adak and Umnak had significantly higher levels of arsenic in

25 both muscle and liver than fish from Cannikin Lake and Fox Lake (Table 2).

Arsenic levels in kidney and egg were highest in fish from Umnak, Adak, and

Cannikin Lake (Table 3). Adak and Cannikin Lake had the highest levels of cadmium in muscle. Adak and Umnak had significantly higher levels of cadmium in liver than fish from Cannikin Lake and Fox Lake. Cadmium levels in kidney were highest in fish from Umnak and Cannikin Lake while levels in egg were highest from Adak. Chromium in muscle was highest in fish from Umnak and chromium in liver was highest in fish from both Umnak and Fox Lake. Chromium in kidney was highest in fish from Adak and chromium in egg did not differ significantly among locations. Adak had the highest levels of lead in liver while

Umnak had the highest levels of lead in muscle. Lead in kidney did not differ among locations but lead in egg was highest in fish from Adak and Cannikin

Lake. Mercury was highest in muscle, liver and kidney of fish caught in Cannikin

Lake and Fox Lake on Amchitka Island. Selenium was higher in both muscle and liver of fish from Cannikin Lake compared to fish from Adak, Umnak, and Fox

Lake. Selenium levels in kidney where highest in fish from Umnak and Cannikin

Lake.

3.3 METAL CORRELATIONS

There was a positive correlation between length and weight, however metals did not uniformly correlate with fish size (Table 4). Because of the small sample size from Adak, correlations are given for all fish combined as well as sea run (Umnak and Adak) and landlocked (Amchitka) separately. For all fish

combined selenium and arsenic were positively correlated with both length and

weight in muscle and liver. Cadmium in liver was positively correlated with

selenium, arsenic, length, and weight and negatively correlated with mercury.

Chromium in liver was negatively correlated with length and weight. Mercury in

muscle and liver was negatively correlated with arsenic and mercury in liver was

negatively correlated with length. Selenium in liver was positively correlated with

arsenic and negatively correlated with chromium. Chromium in muscle was

positively correlated with lead but negatively correlated with mercury and

selenium.

Many of the significant correlations with all fish combined correspond with correlations for Amchitka. This may be due to there being more than twice as many fish sampled from Amchitka than Umnak and Adak combined. One important difference when fish from Amchitka were correlated separately was that mercury in muscle from Amchitka was positively correlated with both weight and length.

3.4 TISSUE CORRELATIONS

Arsenic in muscle was highly correlated with levels in liver, kidney and egg

(Table 5). Arsenic levels in kidney correlated with levels in egg and levels in liver correlated with both kidney and egg. Cadmium levels in liver correlated with levels in muscle, kidney and egg. Chromium levels in muscle only correlated with liver. Lead levels in muscle were negatively correlated with egg but lead levels in kidney positively correlated with egg. There were significant positive correlations

between the levels of mercury in muscle, liver, kidney, and egg. Selenium levels

in muscle correlated with liver, kidney and egg. Selenium levels in liver also

correlated with kidney.

Among organs there were significant differences in all metals except lead

(Table 6). The highest levels of arsenic and cadmium were found in the kidney.

Kidney and liver had significantly higher levels of chromium and mercury than

muscle and egg. Muscle had the lowest levels of arsenic, cadmium, chromium

and selenium.

3.5 GENDER DIFFERENCES

There were few significant gender differences in metal concentrations

(Table 7). In muscle chromium was higher in females than males. Selenium in

liver was higher in males than females. Cadmium in kidney was higher in females

than males.

4.0 DISCUSSION

4.1 LOCATIONAL DIFFERENCES

One of the objectives of this study was to compare contaminant levels in

Dolly Varden among the four collection sites. All three islands had military bases,

Amchitka and Umnak through the 1940’s and Adak until 1997. Cannikin Lake on

Amchitka Island is unique because it was created by an underground nuclear test. Adak and Umnak Islands are inhabited by Aleut communities which consume Dolly Varden from the creeks sampled. I expected that any differences in contaminant levels might relate to human activities.

Significant locational differences were found for all metals in muscle and liver (see Table 2). Some of these locational differences may be influenced by significant differences in the sizes of fish among collection sites. However, the smallest fish (both shortest and lightest) were caught from Fox Lake on Amchitka which had higher mean mercury levels than fish from Umnak and Adak. Fish from Umnak were longer than Adak and Amchitka. This may be because they were caught in May before Dolly Varden typically begin their migration to the sea.

Fish from Adak were taken in June and July so most of the larger fish would have been out at sea. Cannikin Lake is landlocked which may have resulted in heavier fish being caught late in the summer.

Mean mercury concentrations were about six times higher in muscle and liver from both lakes on Amchitka than in those from Umnak or Adak. This may be due to trophic level differences between sea run and landlocked fish. In Arctic

29 char, sea run populations generally have low mercury levels, however some landlocked char have mean concentrations that exceed 200 ppb (Muir and

Lockhart 1993). Landlocked fish feed more heavily on smaller fish and fish eggs which would place them at a higher trophic level than anadromous fish which feed mainly on marine invertebrates.

Neuhold and Helm (1971) studied feeding habits of Dolly Varden on

Amchitka Island in 1967 and 1968. Stream fish fed most heavily on aquatic insects while fish in lakes with access to the sea fed on crustaceans and aquatic insects (Neuhold and Helm 1971). The diets of fish feeding in landlocked lakes lacked crustaceans, and the primary foods were aquatic insects, fish, and fish eggs (Neuhold and Helm 1971). Dolly Varden fed on spawn of threespine stickleback (Gasterosteus aculeatus), Aleutian sculpin (Cottus aleuticus), and pink salmon (Oncorhynchus gorbuscha) (Neuhold and Helm 1971). This may explain the elevated mercury levels found in Dolly Varden from Amchitka Island.

Cannikin Lake is landlocked, however at the time of sample collection a small creek was present that connected Fox Lake to Constantine Harbor. The Dolly

Varden in Fox Lake may not have been sea run fish either due to the narrow creek being inaccessible or the broken dyke at the mouth of the creek at one time may have cut off access to the sea, creating a non-migratory population.

Alternative life histories are common in salmonid fishes and both anadromous and non-migratory populations may occur in the same stream (McKeown 1984).

Over 50% of muscle samples from Amchitka were below the detection limit of 2 ppb for arsenic. All of the muscle samples from Umnak and Adak were

above the detection limit for arsenic. Feeding habits may explain the lower

arsenic levels found in Dolly Varden from both Amchitka lakes, compared with

those from Umnak and Adak. Concentrations of total arsenic are typically high in

invertebrates which feed on marine algae or organic detritus that is often high in

organic arsenic (Neff 1997). Arsenic levels are generally higher in planktivorous

species (Hunter et al. 1981, Maher 1985) and anadromous fishes feed heavily on mysids and amphipods while at sea (Craig 1989).

Cadmium in liver was higher in fish from Umnak and Adak than Amchitka.

This may also be due to differences in feeding habits. Rainbow (1989) found that

cadmium readily accumulates in oceanic amphipods (Thermisto gaudichaudii).

Chromium in liver was highest in fish from Umnak and Fox Lake. However

chromium in muscle was higher in fish from Umnak than the other three collection sites. Drilling mud, used while excavating holes for the three nuclear tests on Amchitka, contained chrome lignosulfonate, chrome lignite, and as much as 8% oil (Department of Energy / Nevada Operations Office 2001). Twelve mud pits designed to hold up to 2,250,000 gallons of liquid were constructed near drilling sites to serve as sumps for drilling mud (Valdez et al. 1977). Between

1968 and 1971 there were several spills of drilling mud, some as large as

1,125,000 gallons (Valdez et al. 1977). Several spills in Clevenger Creek and

White Alice Creek were large enough to completely eliminate fish and macroinvertebrates (Valdez et al. 1977).

In 2001 the DOE began capping these mud pits on Amchitka (Giblin et al.

2002). During this process water was pumped off to provide access to drilling

31 mud. The Department of Energy / Nevada Operations Office (2001) analyzed chromium levels in two Dolly Varden muscle samples from Cannikin Lake and reported values of 226 and 499 ppb. All of our muscle samples from Cannikin

Lake were below 20 ppb. Several muscle samples from Fox Lake were above

100 ppb and two liver samples from Fox Lake had chromium concentrations over

2,000 ppb. Elevated chromium levels in fish from Fox Lake may be caused by drilling mud spills since Clevenger Lake and the Borrow mud pits are only about

2 kilometers from Fox Lake. However Valdez et al. (1977) noted several spills that also contaminated White Alice Creek, which later formed Cannikin Lake, and

Dolly Varden from Cannikin Lake had the lowest chromium levels compared to the other three locations.

ATSDR (2002) reported elevated levels of lead in whole Dolly Varden from

Sweeper Creek, Adak, with a maximum level of 1,300 ppb wet weight. The lowest levels of lead in muscle were in Dolly Varden from Sweeper Creek, Adak.

However Sweeper Creek had much higher lead levels in liver than the other two islands. The highest levels of lead in muscle were in fish from Umnak. This could be due to anthropogenic activities, local geology, or differences in lead levels in prey. Burger et al. (2007b) compared lead levels in Pacific cod (Gadus macrocephalus) from Umnak, Adak, Amchitka, and Kiska Islands. As with Dolly

Varden, they also reported the lowest lead levels in muscle of Pacific cod from

Adak.

Selenium levels were highest in muscle and liver of fish from Cannikin

Lake. Cannikin Lake is unique among the collection sites because it was formed

as a result of an underground nuclear test and is up to a mile wide and 60 feet

deep, making it one of the largest lakes on Amchitka Island. The size of Cannikin

Lake may support larger and older fish. Selenium levels in both muscle and liver

were positively correlated with fish length and weight and the heaviest fish were

caught in Cannikin Lake. Several studies have reported a positive correlation of

selenium and length, weight, or age of fish (Leonzio et al. 1982; Mackay et al.

1975). Thus, elevated selenium levels in fish from Cannikin Lake may be due to

fish size or age.

4.2 SIZE-METAL RELATIONSHIPS

Essential metals are generally regulated at fairly constant concentrations

even when levels are elevated in ambient seawater and food (Chapman et al.

1996). However concentrations of some contaminants increase in fish tissues

over time (Scott and Armstrong 1972). Kidney and liver often have increasing

concentrations of some metals with increasing weight, length, and age (Scott and

Armstrong 1972; Bohn 1975; Bohn and Fallis 1978; Jackson 1991; Thompson

1990). Age, determined by otolith examination, is the more preferred variable

(Derksen and Green 1987), but if age is not available fish length and body weight

can be used as a surrogate for age (Norstrom et al. 1976). Some studies of

invertebrates suggest that metals accumulated in the kidney and liver are biologically inert and not bioavailable to consumers of the marine organism (Nott and Nicolaidou 1994; Wallace and Lopez 1997). Growth may dilute the net accumulation of metals over time causing metal concentrations in tissues to

increase less, remain constant, or decrease gradually during long-term exposure

(Fischer 1988; Lytle and Lytle 1990; Jorgensen and Pedersen 1994).

A positive correlation has been reported with arsenic and body weight in

marine fish (Bohn 1975; Bohn and Fallis 1978). However Pakkala et al. (1972)

found no correlation with arsenic and age in lake trout (Salvelinus namaycush).

In this study fish weight and length correlated positively with arsenic levels in

both muscle and liver, suggesting that arsenic may bioaccumulate in Dolly

Varden.

Some studies have shown an increase in cadmium with increasing fish

weight and length, however this has not been extensively studied (Thompson

1990). In Pacific cod, cadmium in muscle correlated with fish weight but not age and cadmium in liver was negatively correlated with length, weight, and age, suggesting that cadmium may be lost or diluted as fish grow (Burger et al.

2007b). Cadmium concentrations in Dolly Varden muscle and liver correlate with fish weight, however only muscle cadmium correlated with fish length.

Chromium levels in muscle did not correlate with fish length or weight and chromium in liver was negatively correlated with fish length and weight, suggesting that chromium may not accumulate in Dolly Varden.

Muir et al. (2005) reported a positive correlation of lead with length but not weight in landlocked Arctic char. There were no significant correlations between lead levels in Dolly Varden and fish size across the sites.

Mercury concentrations in fish usually increase with age and size

(Jackson 1991; Scott and Armstrong 1972, Thompson 1990). Mercury in Pacific

cod muscle correlated with length, weight, and age, however mercury in liver did

not (Burger et al. 2007b). Jewett et al. (2003) reported higher mercury levels in

larger fish for Arctic grayling (Thymmallus arcticus), northern pike (Esox lucius),

and lake whitefish (Coregonus clupeaformis). Muir et al. (1995) found that

mercury concentrations in lake trout and Arctic char were significantly related to

fish weight, but only weakly correlated with fish age. In our study, when fish from

all locations were pooled together, mercury in muscle did not correlate with fish

length or weight and mercury in liver was negatively correlated with fish length.

The negative correlation for mercury and length in liver probably reflects trophic

level differences between landlocked and sea run fish rather than differences in

mercury levels due to fish length. When correlations were run by location,

mercury in muscle of fish from Amchitka correlated with length and weight. This

may be due to the low mercury levels found in fish from Umnak and Adak.

Similarly, Park and Curtis (1997) found that at low mercury levels the size

relationships may not hold.

Burger et al. (2007) found no significant correlations for selenium as a

function of size or age in Pacific cod muscle and selenium in liver was negatively

correlated with length, weight, and age. MacKay et al. (1975) reported a positive

correlation of selenium and fish size in Black Marlin (Makaira indica). Selenium levels were highly correlated with length and weight in muscle and liver of Dolly

Varden from Amchitka.

4.3 TISSUE DIFFERENCES

Some bioaccumulated metals are retained in some tissues, particularly the kidney, liver, or digestive gland of marine animals in solid, inert, non-bioavailable granules (Simkiss and Taylor 1989). Females may be able to rid their body of contaminants through their eggs (Burger 2007). In Dolly Varden arsenic and mercury in muscle and arsenic, cadmium, mercury and selenium in liver correlated with levels in eggs. This suggests that females are transferring contaminants to their eggs.

Arsenic may accumulate in the liver, kidney, gallbladder, and scales of fish, but is less likely to accumulate in the muscle (Pedlar and Klaverkamp 2002;

Pedlar et al. 2002; Oladimeji et al. 1984). Sea mullet (Mugil cephalus), which feed mainly on detritus and algae, contain highest concentrations of total arsenic in the liver followed by kidney, gonad, intestine and muscle (Maher et al. 1999).

Of the four Dolly Varden tissues analyzed, kidney had the highest arsenic levels followed by liver, egg, and muscle (Table 4). Arsenic levels were also highly correlated in all four tissues analyzed (Table 5). Therefore, a fish with high arsenic concentrations in muscle also had elevated levels in liver, kidney, and egg.

Cadmium concentrations in fish muscle are generally low, however it can accumulate in the kidney, digestive gland, and liver of marine biota (Thompson

1990, Hollis et al. 2001). Cadmium concentrations in the kidney and digestive gland are generally about 10 fold higher than levels in muscle (Neff 2002).

Rainbow trout (Salmo gairdneri) and lake whitefish retained cadmium from the water in their gills and kidney, whereas cadmium in food was accumulated in the

kidney, gut, and liver (Harrison and Klaverkamp 1989). Cadmium concentrations

in muscle tissue were very low and the highest cadmium levels were in the

kidney.

Thomann et al. (1997) found that whole body cadmium concentrations

reach equilibrium in about 50 days, however cadmium continued to accumulate

in the kidney of rainbow trout. Dillon and Gibson (1985) found that hatching rate

was reduced in flounder eggs containing between 60 and 160 ppb cadmium.

Cadmium levels in Dolly Varden eggs were well below this level. Cadmium levels

in muscle were weakly correlated with levels in liver, however levels in kidney

were highly correlated with levels in liver. Burger et al. (2007a) found a similar

relationship between cadmium in liver and kidney for both great sculpin and

flathead sole (Hippoglossoides elassodon).

Fish organ tissues usually do not contain significantly higher levels of

chromium than muscle (Neff 2002). However tilefish (Lopholatilus

chamaeleonticeps), have higher chromium levels in kidney than muscle and liver

(Steimle et al. 1990). As with tilefish, chromium concentrations in Dolly Varden

kidney and liver were higher than muscle and egg. Similarly, great sculpin had

higher chromium levels in kidney and liver than muscle and flathead sole had

highest chromium levels in kidney (Burger et al. 2007a). These studies suggest

that chromium may accumulate in the kidney of fish. Chromium levels in Dolly

Varden muscle correlated with levels in liver, however this was the only significant correlation for chromium among organs.

Lead levels are typically low in marine fish muscle and may accumulate in

the liver and kidney (Thompson 1990), but generally do not biomagnify in fish

(Settle and Patterson 1980). In many sharks lead concentrations in muscle are

similar or slightly lower than concentrations in liver (Vas 1991). Burger et al.

(2007a) reported higher lead levels in kidney than liver and muscle of flathead

sole and great sculpin from Adak Island. Lead concentrations in Dolly Varden did

not differ significantly among the four tissues analyzed.

Mercury in fish is generally higher in the liver followed by kidney and

muscle (Thompson 1990). This was true in Dolly Varden (see Table 4). Elevated

mercury concentrations in fish eggs may result in decreased fertilization success, decreased reproductive success and altered sex ratios (Matta et al. 2001).

Zhang et al. (2001) reported that mean levels of total mercury in muscle

ranged from 34 to 96 ppb (wet weight) in chum (Oncorhynchus keta), coho

(Oncorhynchus kisutch), chinook (Oncorhynchus tshawytscha), and sockeye

salmon collected from four major rivers throughout western Alaska. They noted

that mercury levels in salmon liver tended to be higher than muscle, with means

ranging from 54 to 112 ppb, while eggs were lower with a mean of 7.7 ppb

(Zhang et al. 2001). Mean mercury concentrations in Dolly Varden eggs were

over four times higher than levels reported in salmon eggs by Zhang et al.

(2001). The mean mercury concentration for eggs in sea run Dolly Varden from

Adak and Umnak was 8 ppb, similar to the 7.7 ppb reported in salmon eggs by

Zhang et al. (2001). However the mean mercury level for eggs from landlocked

fish on Amchitka was 58 ppb.

Mercury levels were highly correlated in Dolly Varden muscle, liver,

kidney, and eggs. Thus, it may be possible to use egg as a non-lethal indicator of

mercury contamination in Dolly Varden. Burger et al. (2007a) also reported positive correlations for mercury between muscle, liver, and kidney of great sculpin and flathead sole, however this study did not report levels in eggs.

Selenium in fish is often highest in the liver, followed by eggs and muscle

(Kennedy et al. 2000). In this study selenium concentrations did not differ significantly among egg, kidney, and liver, however muscle was much lower.

Burger et al. (2007a) also found lower levels of selenium in muscle than kidney and liver of great sculpin and flathead sole from Adak. Selenium in Dolly Varden muscle correlated with liver and levels in liver correlated with egg and kidney.

4.4 GENDER DIFFERENCES

The uptake, fate, and effects of contaminants can be influenced by gender due to differences in genetics, physiology, morphology, growth, and behavior

(Burger 2007). Both males and females can rid their bodies of contaminants through bile, urine, and sloughing of epidermal structures such as scales, however females can also transfer contaminants to their eggs (Burger 2007).

There is little data available on gender differences in fish, partly because gender is not easily determined by external examination for many species. Gender differences in size, morphology, and behavior can affect foraging, resting, breeding, and migratory behavior (Becker and Wink 2003). Few gender related differences were found in Dolly Varden (Table 7). Females had significantly

39 higher levels of chromium in muscle and cadmium in kidney than males. Males had significantly higher levels of selenium in liver than females.

Burger and Gochfeld (2007) found no significant gender differences in levels of mercury or selenium in Pacific cod from the Aleutian Islands, Alaska.

In Largemouth bass (Micropterus salmonides) males had higher levels of mercury in muscle (Lange et al. 1994). Jewett et al. (2003) found no differences in mercury levels of northern pike between sexes, however female Arctic grayling had higher levels of mercury than males. The authors suggested that higher mercury levels in female grayling was due to size differences, since females were larger than males. The higher selenium levels in livers of male Dolly Varden may also be due to size differences, because males were significantly heavier than females and selenium in liver was positively correlated with weight. The higher levels of chromium in muscle of female fish may also be due to size differences. In fish from Amchitka weight was negatively correlated with chromium levels in muscle and the females weighted less than males.

4.5 GEOGRAPHICAL COMPARISONS

ATSDR (2002) reported slightly elevated levels of arsenic in Dolly Varden from Sweeper Creek, Adak. As a result, the Navy posted signs along Sweeper

Creek and Sweeper Cove prohibiting consumption of fish from these areas until removal of contaminated sediment was completed. By 2002 the sediment had been removed, and the Navy was considering if advisories should be lifted

(ATSDR 2002). ATSDR (2002) found levels of arsenic as high as 100 ppb wet

weight in Dolly Varden muscle samples from Sweeper Creek. In our study

arsenic levels as high as 500 ppb were found in Dolly Varden muscle from

Sweeper Creek, Adak and 400 ppb from Sheep Creek, Umnak (Fig 5).

Overall, mean arsenic levels in Dolly Varden were low compared to levels reported in Dolly Varden from mainland Alaska and other fish species. Rudis

(1996) reported arsenic levels of 460 ppb (wet weight) in whole Dolly Varden

from Ready Bullion Creek, near Juneau, Alaska, a highly mineralized area and

site of former mining activity. Rudis (2001) reported a mean arsenic level of

1,880 ppb (dry weight, about 435 ppb wet weight) in a composite containing six

Dolly Varden and one prickly sculpin (Cottus asper) from Sherman Creek, near

Kensington Mine in Southeast Alaska. Bohn and Fallis (1978) reported mean

arsenic levels in muscle of 500 ppb (dry weight, wet weight approximately 116

ppb) and mean levels in liver of 700 ppb (dry weight, wet weight approximately

163 ppb) in Arctic char from Kuhulu Lake, Northwest Territories. These levels

are similar to the mean levels I found in muscle from Adak and Umnak, however

liver samples from Adak were much higher.

Low cadmium levels have been reported in fish throughout Northern

Canada (Lockhart et al. 1992). Cadmium concentrations as high as 5,800 ppb

(dry weight; wet weight approximately 1,349 ppb) were reported in menhaden

(Brevoortia patronus) muscle from a contaminated estuary in Louisiana

(Ramelow et al. 1989). In Arctic char from Kuhulu Lake, Northwest Territories,

cadmium was not detectible in muscle, but liver samples averaged 2,000 ppb

(dry weight, wet weight approximately 465 ppb; Bohn and Fallis 1978). Burger et

41 al. (2007a) reported cadmium levels in muscle and liver of flathead sole from

Adak at 4.0 and 4,900 ppb (wet weight) respectively. The Department of Energy /

Nevada Operations Office (2001) analyzed two Dolly Varden muscle samples from Cannikin Lake for cadmium, one was below the detection limit of 50 ppb and the other was 54 ppb, just above detection, higher than our mean of 4.5 ppb.

The highest cadmium value in muscle, 77 ppb, was from Cannikin Lake (Fig 6).

Crayton (2000) reported chromium in Pacific cod livers from Amchitka

Island ranging between <70 and 1,330 ppb. Our mean for chromium in muscle of

Dolly Varden was 23 ppb, lower than levels found in great sculpin and flathead sole from Adak (90 and 95 ppb, respectively; Burger et al. 2007a). Muir et al.

(2005) reported mean chromium levels that ranged from 27 to 135 ppb in muscle of landlocked Arctic char from 6 lakes in the Canadian Arctic archipelago. Almost

70% of our muscle samples were below their lowest level in Arctic char of 27 ppb

(Fig 7).

Crayton (2000) reported lead levels in rock greenling (Hexagrammos lagocephalus) liver samples from Amchitka ranging from 600 to 14,000 ppb (dry weight, approximately 114 to 2,600 ppb wet weight). Rudis (1996) reported lead levels of 3,570 ppb in whole Dolly Varden from Ready Bullion Creek, Alaska which may be elevated due to former mining. Schmitt (2004) reported geometric means for lead in whole brown trout (Salmo trutta) from the Upper Missouri River at 70 ppb in 1986 and 10 ppb in 1995. The geometric mean for 315 composites of U.S. freshwater fish collected in 1984 was reported at 110 ppb and rainbow trout (Oncorhynchus mykiss) from Kenaia River in Soldatna, Alaska had lead

concentrations of 10 ppb (Schmitt and Brumbaugh 1990). However, levels in

whole fish may be higher than would be expected in muscle alone. Muir et al.

(2005) reported mean lead levels that ranged from 6 to 35 ppb in muscle of 120 landlocked Arctic char from 6 lakes in the Canadian Arctic archipelago. Overall our mean lead levels in muscle were relatively low at 22 ppb. However lead in

Dolly Varden muscle from Umnak Island was as high as 233 ppb (Fig 8).

Smith and Armstrong (1975) reported a mean total mercury level of 49 ppb in muscle of Arctic char, which they describe as a principle food item for Inuit people living in the village of Holman on the western Victoria Island, N.W.T. In our study, Dolly Varden from Umnak and Adak had mercury levels that were less than half those found in Arctic char. However on Amchitka mercury levels were over three times higher than Arctic char.

Northgate Minerals Corporation (2005) reported mean mercury levels at

38 ppb (wet weight) in Dolly Varden muscle from Attycelley Lake in BC, Canada.

Naidu et al. (2001) reported mean total mercury and methylmercury levels of 7 ppb in Dolly Varden muscle samples from Kuskokwim, near the Eastern Bering

Sea, indicating that nearly 100% of total mercury in Dolly Varden muscle is organic. The Dolly Varden sampled by Naidu et al. (2001) were probably sea run because they were caught in rivers opening into the Bering Sea. The mean mercury levels in muscle from sea run fish in our study was 23 ppb, but over 150 ppb in fish from Amchitka. Naidu et al. (2001) also analyzed 137 salmon

(Oncorhynchus spp.) for total mercury, methylmercury, and selenium. Total mercury in salmon muscles ranged from 25-137 ppb and they found no

correlation between selenium, lipids or omega-3 fatty acids and total mercury or

methylmercury (Naidu et al. 2001). In our study 59% of muscle samples from

Amchitka were higher than their highest salmon sample of 137 ppb (Fig 9). I also found no correlation between selenium and total mercury in muscle or liver.

Gray et al. (2000) found mercury levels up to 620 ppb in muscle and 1,300

ppb in liver from Dolly Varden collected near abandoned mercury mines in

southwestern Alaska. Mercury levels in similar fish caught in baseline streams

were all below 200 ppb (Gray et al. 2000).

Mercury levels in Dolly Varden from our study were relatively low when

compared to other freshwater fish species. Northern pike from Yukon and

Kuskokwim rivers had mercury concentrations of 1,500 and 630 ppb respectively,

while Arctic grayling sampled from the same two rivers had concentrations of 260

and 80 ppb (Jewett et al. 2003). The higher mercury levels found in Northern pike

may be due to the fact that this species is piscivorous and feeds at a higher

trophic level than grayling. Thus, mercury levels in Dolly Varden from this study

in the Aleutians were much lower than levels found in Northern pike. Dolly

Varden from Umnak and Adak had lower mercury levels than Arctic grayling

while Dolly Varden from Amchitka had similar levels to those in Arctic grayling.

Kennedy et al. (2000) reported mean selenium levels in cutthroat trout

(Oncorhynchus clarki lewisi) from a river with elevated selenium due to coal

mining at 36,600, 21,200, and 12,500 ppb dry weight (about 8,500, 5,000, and

3,000 ppb wet weight) in liver, eggs, and muscle, respectively. Higher than our

highest selenium value in Dolly Varden muscle of 1144 ppb (Fig 10). Burger et al.

(2007b) reported a mean for selenium of 183 ppb in muscle of Pacific cod

collected near Nikolski, Adak, Amchitka, and Kiska. Our mean for selenium in

Dolly Varden muscle was 349 ppb. The Department of Energy / Nevada

Operations Office (2001) analyzed two Dolly Varden muscle samples from

Cannikin Lake for selenium and reported levels of 720 ppb which is similar to our

mean for Cannikin Lake of 760 ppb.

4.6 RISK TO HUMAN CONSUMERS

One objective of this study was to determine if levels of these metals in

Dolly Varden were sufficiently high to pose a risk to human consumers. Dolly

Varden are an important resource for many residents of Alaska, and in the

Aleutian villages one or two fishermen often catch several Dolly Varden and

distribute them to other residents (U.S. Fish & Wildlife Service 2005; Fall et al.

2006). Fish are a low-fat source of protein and are high in omega-3 fatty acids

that reduce cholesterol levels (Daviglus et al. 2002). However levels of

contaminants in some fish are high enough to potentially affect the fish themselves or top-level predators consuming them (Stern 1993; NRC 2000). The

U.S. EPA has set chronic oral reference doses (RfD), expressed in milligrams per kilogram of body weight per day, which can be consumed on a daily basis over a 45 year life span without adverse effects, however there is no RfD value for lead. I calculated the hazard quotient to determine if the U.S. EPA RfD values would be exceeded assuming one 8 ounce (228 g) Dolly Varden meal is consumed daily (Table 8).

In humans arsenic is carcinogenic and ingesting high doses can result in death (ATSDR 2005). Exposure to low doses in food can cause hyperpigmentation, skin lesions, and keratosis (EPA 1992). Arsenic is thought to be an essential micronutrient for all plants and animals (Uthus 1992). Arsenic levels can vary widely among tissues, species, and geographic locations (Neff

2002).

Humans can readily accumulate both organic and inorganic forms of arsenic from food (Buchet et al. 1994). However organic arsenic is not toxic or carcinogenic to marine animals or their consumers (Vahter et al. 1983; Sabbioni et al. 1991). Marine mammals and terrestrial mammals, including humans, are able to excrete organic arsenic ingested in their food (Meador et al. 1993; Zeisler et al. 1993). More than 90% of the total arsenic found in seafood is the less toxic organic form (Edmonds and Francesconi 1993; Eisler 1994). The U.S. EPA set a human health criterion for total arsenic in seawater from which fishery products are harvested for human consumption of 17.5 ng/L (EPA 1988). In unpolluted ocean waters arsenic concentrations range from 500 to 3,000 ng/L, with a mean of about 1,700 ng/L (Andreae and Andreae 1989; Li 1991). Thus, the human health criterion for arsenic in seawater is about two orders of magnitude lower than the average concentration of arsenic in unpolluted seawater.

The EPA critical value for human consumption of arsenic in fish is 1.0 ug/g which is equivalent to 1,000 ppb wet weight (EPA 1989). The highest arsenic concentrations in our study were 500 ppb in muscle and 1,700 ppb in liver, both from the same fish caught in Sweeper Creek, Adak, indicating that arsenic levels

in livers of some Dolly Varden could pose a risk if consumed. Although most

recreational fishers gut their fish, thus avoiding the liver, many people consume whole fish in soups or stews.

The EPA chronic oral reference dose for arsenic is 0.3 ug/kg/day. If a

human weighing 70 kg eats one eight ounce meal (228g) of Dolly Varden

muscle from Umnak or Adak each day they will exceed the EPA chronic oral

reference dose by a factor of 2 (Table 8). However this study only tested for total

arsenic and most of the arsenic in seafood is in nontoxic organic forms

(Francesconi and Edmonds 1993). Thus, it is doubtful that arsenic in Dolly

Varden from any of the islands sampled will cause harm to human consumers.

Cadmium is a nonessential element which can be toxic at high

concentrations. Much of the cadmium in marine invertebrates may be in the form

of solid concretions which is not bioavailable to consumers (Nott and Nicolaidou

1994). Some forms of cadmium may also be mutagenic or carcinogenic in

mammals (Kazantzis 1987). Chronic exposure to cadmium may cause kidney

dysfunction and bone disease (Neff 2002). The critical value of cadmium for

human consumption in fish is 100 ppb (Eisler 1985; EPA 1989). All muscle and

egg samples were below 100 ppb. It is unlikely that a person consuming one 8

ounce meal of Dolly Varden per day would exceed the U.S. EPA reference dose

for cadmium. However, cadmium levels were higher in the kidney and liver. 75%

of all kidney samples and 25% of all liver samples were above the critical value

of cadmium for human consumption (100 ppb).

Trivalent chromium is an essential nutrient that can be toxic in large doses

(Eisler 1986), while hexavalent chromium is a human carcinogen (ATSDR 2000).

The critical value of chromium for human consumption in fish is 1.0 ug/g which is equivalent to 1,000 ppb wet weight (EPA 1989). Muscle samples from Dolly

Varden in our study were well below this value. However there were two liver samples from Fox Lake on Amchitka with levels over 2,000 ppb, above the critical value for human consumption in fish. A person eating one 8 ounce meal of Dolly Varden per day would not exceed the U.S. EPA reference dose for chromium.

In humans lead is known to cause neurobehavioral, developmental, and blood enzyme effects and there is evidence that lead is a carcinogen (EPA

1992). The critical value of lead for human consumption in fish is 0.5 ug/g which is equivalent to 500 ppb wet weight (EPA 1989). However levels as low as 100 ppb have been associated with learning deficits in some vertebrates (Eisler

1988). No risk-based concentration has been published for inorganic lead in edible tissues of marine animals for human consumption, however even small amounts of lead consumed by humans, especially children, are considered hazardous (Neff 2002). International guidelines for lead in tissues of fishery products generally range from 500 to 10,000 ppb (Melzian 1990). In Dolly Varden lead levels were well below the adverse effects level and did not differ significantly among organs.

Mercury is a non-essential element for humans and is known to biomagnify at higher trophic levels (Ratkowsky et al. 1975, Bryan 1979,

Thompson 1996). Methylmercury is more toxic than elemental or inorganic mercury (ATSDR 1999) and in many studies over 90% of the total mercury in fish is methylmercury (Bloom, 1992). Nearly 100% of the total mercury in northern pike and Arctic grayling is methylmercury (Jewett et al. 2003; Egeland et al.

1998). Naidu et al. (2001) reported a mean of 7 ppb for total and methylmercury in 3 Dolly Varden sample from Kuskokwim River in western Alaska, suggesting that methylmercury may constitute 100% of total mercury in Dolly Varden. Fish consumption is the main source of human exposure to methylmercury (Rice et al.

2000). High levels of methylmercury in fish can represent a potential risk to human consumers (Wolfe et al. 1998). In humans methylmercury can cause neurological and developmental disorders (NRC 2000) and there are federal and state advisories for pregnant women and young children to reduce fish consumption (EPA 2004).

The federal legal limit for methylmercury in seafood sold in the United

States is 1 ug/g which is equivalent to 1,000 ppb wet weight (US FDA 2001). In

Canada the recommended maximum level of mercury in fish for subsistence fisheries is 200 ppb (Health and Welfare Canada, 1984). In our study all muscle samples from Dolly Varden collected on Adak and Umnak were below 100 ppb

(Table 9). These are the two locations with Aleut residents who frequently consume Dolly Varden. Amchitka, which currently does not have any residents, had much higher mercury levels. Only 27% of muscle samples from Amchitka were below 100 ppb while 47% were between 100 and 200 ppb, 12% between

200 and 300 ppb, 12% between 300 and 400 ppb, and 2% over 500 ppb. Thus,

on Amchitka, 26% of muscle samples were above 200 ppb, the recommended

maximum mercury level for subsistence fish and 2% had mercury levels above

500 ppb, the action level for many states and countries, however none were above 1,000 ppb the action level of the U.S. FDA.

The World Health Organization set the provisional daily intake of methylmercury at 0.23 ug/kg body weight/day (JECFA 2003). The EPA chronic oral reference dose for mercury is 0.1 ug/kg/day. If a subsistence fisher or site worker ate one 8 ounce meal a day of Dolly Varden from Amchitka Island, they would exceed the U.S. EPA reference dose for mercury by a factor of 5.

Selenium is an essential micronutrient but can be toxic at high levels

(Coyle et al. 1993). Exposure to high levels of selenium can cause selenosis and common symptoms are neurological effects, brittle hair, and deformed nails

(ATSDR 2003). Selenium is not classified as a carcinogen in humans. Fishermen who regularly consume fish from waterways with elevated selenium levels may increase their selenium body burden, but no reports of selenosis have been attributable to this (ATSDR 2003). Selenium may be capable of inhibiting the negative effects of mercury by rendering it less bioavailable (Bjorkman et al.

1995).

Fish accumulate selenium mainly through their diet (Hermanutz et al.

1992). The critical value of selenium in fish for human consumption is 2.0 ug/g which is equivalent to 2,000 ppb wet weight (EPA 1989). In our study all muscle samples were well below the critical value for human consumption. However the

mean value for selenium in liver samples from Cannikin Lake was 1,860 ppb,

slightly less than the critical value for human consumption, and 33% of liver samples from Cannikin Lake were above this level. The EPA chronic oral reference dose for selenium of 5 ug/kg/day is not likely to be exceeded by eating

Dolly Varden from any of the islands studied.

4.7 RISK TO WILDLIFE RECEPTORS

Inorganic arsenic is more toxic to marine plants than marine animals and its toxicity varies greatly among marine organisms (Neff 2002). The published data for toxicity of arsenic to marine animals is limited. Embryonic stages appear

to be most sensitive to arsenic. Purple sea urchin (Strongylocentrotus

purpuratus) embryos exposed to concentrations of arsenate as low as 11,000

ng/L had increased developmental abnormalities (Garman et al. 1997). Arsenate

was found to be acutely toxic to mysids (Mysidopsis bahia) at concentrations of

2,300 ng/L (Gentile 1981). The U.S. EPA chronic water quality criteria for arsenic to protect marine life 36,000 ng/L (EPA Region III 2000). Organic forms of arsenic can be bioaccumulated by marine animals (Edmonds et al. 1992), however this form is not toxic or carcinogenic to marine animals (Vahter et al.

1983; Sabbioni et al. 1991). Thus, arsenic levels found in Dolly Varden are not likely to have adverse effects on wildlife consumers.

Ionic cadmium is accumulated mainly through the gills of marine organisms (Sidoumou et al. 1997). Cadmium can also be accumulated in marine invertebrates and fish from their food (Reinfelder and Fisher 1994; Canli and

Furness 1995; Wang and Fisher 1997). Sullivan et al. (1984) fed cadmium-

contaminated oysters to mice. The mice retained only 0.83% of the cadmium in their tissues, with most accumulating in the liver and kidney. Thus, trophic transfer of cadmium from a primary consumer to a secondary consumer may be very inefficient. Harrison and Klaverkamp (1989) found that rainbow trout and lake whitefish can accumulate cadmium from both water and food, however the absorption efficiency from food is about an order of magnitude higher.

Mysids are extremely sensitive to cadmium, with median lethal concentrations between 15,000 and 20,000 ng/L (Gentile et al. 1982). Cadmium concentrations between 500 and 10,000 ng/L can cause decreased growth rates, depressed respiration, molt inhibition, shortened life-span, altered enzyme activity, and abnormal muscular contractions in marine animals (Eisler 1985).

Cadmium levels exceeding 1,000 ppb in diets of fish may have adverse effects

(Eisler 1985). Cadmium levels in Dolly Varden were well below this level.

Hexavalent chromium is moderately toxic to marine organisms. The EPA chronic water quality criteria for chromate in seawater is 50,000 ng/L (EPA 1992).

Some marine invertebrates appear to be unaffected by chronic exposure to

250,000 ng/L chromate, however exposure of 16,000 to 38,000 ng/L may reduce brood size in polychaete (Neanthes arenaceodentata) (Oshida et al. 1981;

Oshida and Word 1982). Total chromium levels of 10,000 ppb in the diets of birds and mammals may cause adverse effects (Eisler, 1986). Chromium levels in muscle of most fish species are below 5,000 ppb (Neff 2002). Chromium levels in

Dolly Varden were well below the effects level for birds and mammals.

Lead levels as low as 100 ppb have been associated with learning deficits

in some vertebrates (Eisler 1988). Inorganic lead is moderately toxic to marine

organisms and can cause neurological dysfunction, altered behavior and learning

ability, kidney disease, and immune suppression (Neff 2002). The acute toxicity

level of lead to mysids (Mysidopsis bahia) is very high (3,139,000 ng/L), however

chronic exposure to concentrations as low as 25,000 ng/L can affect reproduction

(Lussier et al. 1985). Lead concentrations in tissue of mussels over 10,000,000 ppb (dry weight) may impair feeding and growth (Schulz-Baldes 1974). The

chronic water quality criteria for inorganic lead for protection of marine life is

8,500 ng/L (EPA 1992). Levels of 50,000 ppb in the diet may affect reproduction

and levels as low as 100 ppb are associated with learning deficits in some

vertebrates (Eisler 1988). Lead concentrations in muscle tissue of most fish

species are generally less than 1,000 ppb (Neff 2002). Mean lead levels in Dolly

Varden were very low, at 22 ppb, and are unlikely to pose a threat to wildlife

consumers. Lead levels are generally low in animals at the top trophic levels in marine food chains (Neff 2002). However metallic lead is highly toxic when ingested by marine birds and mammals, and ingestion of lead shot and fishing weights by marine birds may be a major source of lead poisoning (Mateo et al.

1997).

Mercury is a known mutagen, teratogen, and carcinogen (Eisler 1987).

Organic mercury is one of the most toxic metals to marine organisms (World

Health Organization 1989). For marine and freshwater fish, acutely lethal concentrations of inorganic mercury in water range from 400 to 23,000,000 ng/L

(World Health Organization 1989), however methylmercury may be 10 to 100

times more lethal than inorganic mercury (Boening 2000). Concentrations of

inorganic mercury as low as 500 ng/L may be capable of inhibiting growth in

marine microalgae (Langston 1990). Methylmercury is a neurotoxin and fish from polluted waters exhibit neuropathological lesions and altered behavior (George

1990). Methylmercury penetrates the intestinal barrier in plaice (Pleuronectes platessa) and accumulates in muscle tissue (Pentreath 1976a; Pentreath 1976b).

In rainbow trout fed contaminated food, 23% of inorganic mercury and 84% of organic mercury was accumulated (Boudou and Rebeyre 1985). Dietary mercury concentrations of 50 to 500 ppb may adversely affect sensitive birds (Eisler

1987). The mean mercury level in muscle of Dolly Varden from Amchitka was

157 ppb, within the range known to adversely affect sensitive birds.

In fish excessive levels of selenium can cause reduced growth, tissue damage, reproductive effects and increased mortality (Hodson et al. 1980;

Hodson and Hilton 1983). In fish teratogenesis is a biomarker of selenium toxicity and deformities include lordosis (concave curvature of lumbar and caudal regions of spine), kyphosis (convex curvature of thoracic region of the spine), scoliosis

(lateral curvature of the spine) and head, mouth, gill cover, and fin deformities, in addition to brain, heart, and eye problems (Ohlendorf et al. 1986b; Lemly 1993a;

Lemly 1997). The critical value for selenium in fish for the protection of piscivorous wildlife is 600 ppb while levels of 2,600 ppb are associated with adverse effects in the fish themselves (Lemly 1993b; Lemly 1996). In our study

54 the mean selenium level in Dolly Varden muscle from Cannikin Lake was above the threshold for protection of piscivorous wildlife of 600 ppb.

Fish from sites contaminated by selenium from coal fly ash may have concentrations 2 to 3 times higher than unpolluted areas (Besser et al. 1996). In the Kesterson National Wildlife Refuge in San Joaquin Valley, California, elevated levels of selenium as high as 170,000 ppb were found in mosquito fish

(Ohlendorf et al. 1986b). High selenium levels in Kesterson were caused by an

85-mile subsurface agricultural water drain that terminated in a series of evaporation ponds called Kesterson Reservoir. Because the high selenium levels produced death and deformities in fish and waterfowl, delivery of subsurface water to Kesterson was terminated in 1986 (Lewis 1988).

Selenium levels between 8,800 and 10,500 ppb (wet weight) in rainbow trout eggs may cause developmental abnormalities in approximately 15% of the population (Holm et al. 2005). Kennedy (2000) found no toxic response to elevated selenium levels in cutthroat trout and suggested that fish may be able to evolve a tolerance to elevated tissue selenium concentrations.

4.8 CONCLUSION

Overall, metal concentrations in Dolly Varden from Umnak, Adak and

Amchitka are relatively low when compared to other fish species from the

Aleutians and Dolly Varden from other locations. Metal levels may be elevated in a few individual fish, but mean levels in muscle were well below the critical value for human consumption for all elements analyzed. Dolly Varden from Amchitka

55 may have elevated levels of mercury when compared to fish from Umnak and

Adak, however this is probably due to differences in trophic level rather than local geology or anthropogenic activities. For some metals and locations, liver concentrations exceeded critical values, while muscle did not, indicating there may be concern when whole fish are consumed. Although most recreational fishers gut their fish, thus avoiding the liver, many people consume whole fish in soups or stews.

Mercury levels were highest in fish from Amchitka Island and may pose a risk to people regularly consuming Dolly Varden from these lakes. Selenium levels were highest in muscle (761 ppb) and liver (1,856 ppb) of fish caught in

Cannikin Lake on Amchitka Island and may pose a risk to piscivorous wildlife.

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Table 1. Multiple regression models on log transformed data for differences in levels of metals in Dolly Varden collected from the Aleutians. NS = not significant.

arsenic cadmium chromium lead mercury selenium

Model F 27.3 123 18.0 2.8 48.4 22.1

df7 7 7777

P <0.0001 <0.0001 <0.0001 0.01 <0.0001 <0.0001

r2 0.48 0.81 0.38 0.08 0.62 0.43 Factors entering (F, p) island 47.4 (<0.0001) 9.9 (<0.0001) 2.3 (NS) 4.1 (0.02) 109 (<0.0001) 0.4 (NS)

length 0.05 (NS) 3.5 (NS) 1.5 (NS) 4.5 (0.03) 18.8 (<0.0001) 0.8 (NS)

weight 2.9 (NS) 6.5 (0.01) 6.4 (0.01) 1.7 (NS) 8.0 (0.005) 3.8 (0.05)

organ 13.0 (<0.0001) 272 (<0.0001) 34.2 (<0.0001) 3.4 (0.02) 30.8 (<0.0001) 38.9 (<0.0001) 77 78

Table 2. Metal levels (ppb, wet weight)(ng/g) in muscle and liver of Dolly Varden collected from 3 islands (east to west) in Alaska. Given are arithmetic means ± SE (geometric means below) with Kruskal-Wallis Chi Square values and p values. Duncan values are given in parenthesis.

Umnak Adak Amchitka Sheep Creek Sweeper Creek Cannikin Lake Fox Lake X2(p) n=16 n=8 n=21 n=30 standard length (cm) 33.4 ± 0.8 28.6 ± 2.5 32.0 ± 1.1 24.4 ± 0.8 36.7 (<0.0001) weight (g) 372 ± 37.7 356 ± 64.7 478 ± 47.6 197 ± 17.5 30.3 (<0.0001)

MUSCLE arsenic 173 ± 27.4 227 ± 44.0 17.8 ± 5.07 8.01 ± 2.62 51.6 (<0.0001) 143 202 2.85 0.64 (A) (A) (B) (B) cadmium 0.95 ± 0.42 4.87 ± 2.74 4.50 ± 3.64 0.22 ± 0.11 16.2 (0.001) 0.09 0.82 0.17 0.02 (B,C) (A) (A,B) (C) chromium 42.2 ± 5.66 15.4 ± 7.83 3.6 ± 1.11 28.7 ± 6.94 24.7 (<0.0001) 37.0 1.91 0.62 3.84 (A) (B) (B) (B) lead 65.2 ± 14.9 0.08 ± 0.00 4.58 ± 2.22 17.2 ± 6.28 22.4 (<0.0001) 17.5 0.08 0.36 0.82 (A) (C) (B,C) (B) mercury 23.7 ± 5.29 23.2 ± 8.48 158 ± 14.7 156 ± 24.8 26.1 (<0.0001) 17.3 10.7 122 77.5 (B) (B) (A) (A) selenium 291 ± 36.6 188 ± 52.6 761 ± 46.8 135 ± 23.3 48.3 (<0.0001) 258 80.6 727 32.7 (A,B) (B,C) (A) (C)

LIVER arsenic 270 ± 41.9 621 ± 236 37.2 ± 4.24 22.3 ± 5.17 46.6 (<0.0001) 234 423 25.3 3.28 (A) (A)(B) (C) cadmium 156 ± 29.5 128 ± 31.4 54.7 ± 3.86 41.0 ± 6.41 38.3 (<0.0001) 132 112 51.7 31.5 (A) (A) (B) (C) chromium 79.5 ± 21.9 29.4 ± 9.79 30.9 ± 7.99 294 ± 184 21.0 (0.0001) 53.5 24.1 21.6 61.0 (A) (B) (B) (A) lead 7.80 ± 3.40 93.3 ± 59.1 11.5 ± 2.75 16.2 ± 6.56 12.2 (0.007) 0.83 43.1 3.48 2.72 (B) (A) (B) (B) mercury 43.7 ± 7.27 43.3 ± 6.58 276 ± 18.9 352 ± 41.5 43.9 (<0.0001) 38.1 40.8 259 284 (B) (B) (A) (A) selenium 1160 ± 69.2 1290 ± 152 1860 ± 97.2 778 ± 68.7 43.0 (<0.0001) 1130 1240 1800 658 (B)(A,B) (A) (C) 79

Table 3. Metal levels (ppb, wet weight)(ng/g) in kidney and egg of Dolly Varden collected from 3 islands (east to west) in Alaska. Given are arithmetic means ± SE (geometric means below) with Kruskal-Wallis Chi Square values and p values. Duncan values are given in parenthesis.

Umnak Adak Amchitka Sheep Creek Sweeper Creek Cannikin Lake Fox Lake X2(p) n=14 n=6 n=10 n=13

KIDNEY arsenic 243 ± 55.9 358 ± 86.1 225 ± 40.3 57.3 ± 12.7 19.8 (0.0002) 177 300 186 28.6 (A) (A) (A) (B) cadmium 303 ± 43.2 129 ± 37.1 199 ± 19.7 116 ± 20.5 15.3 (0.002) 252 90.1 188 93.9 (A) (B) (A) (B) chromium 56.2 ± 7.9 278 ± 121 77.1 ± 19.3 85.1 ± 21.9 8.4 (0.04) 49.0 176 62.8 69.1 (B) (A) (B) (B) lead 36.7 ± 27.6 101 ± 50.6 22.5 ± 10.5 9.5 ± 3.7 5.2 (NS) 5.19 21.1 3.31 0.94 mercury 53.4 ± 9.91 26.5 ± 11.5 207 ± 26.1 329 ± 47.9 26.5 (<0.0001) 51.7 11.4 188 264 (B) (C) (A) (A) selenium 1910 ± 164 1310 ± 95.9 1700 ± 177 933 ± 71.4 24.3 (<0.0001) 1830 1290.0 1590 892 (A) (B) (A,B) (C)

n=9 n=4 n=2 n=12 EGG arsenic 79.4 ± 8.56 155 ± 41.8 72.1 ± 4.9 15.0 ± 3.36 20.1 (0.0002) 75.6 136 71.9 5.8 (A) (A) (A) (B) cadmium 17.3 ± 4.93 40.1 ± 9.63 11.5 ± 0.46 12.8 ± 1.1 8.3 (0.04) 10.9 36.5 11.5 12.4 (B) (A) (B) (B) chromium 16.4 ± 2.66 18.8 ± 0.97 20.9 ± 7.1 19.7 ± 3.72 0.7 (NS) 14.5 18.7 19.6 16.7 lead 0.08 ± 0 96.2 ± 20.4 65.2 ± 19.8 16.2 ± 7.88 18.1 (0.0004) 0.08 90.8 62.1 0.6 (B) (A) (A) (B) mercury 7.89 ± 2.81 8.25 ± 1.89 20.0 ± 1 64.3 ± 11.0 18.4 (0.0004) 6.01 7.57 20.0 53.3 (C) (C) (B) (A) selenium 1450 ± 263 1510 ± 188 1380 ± 120.04 769 ± 121 8.5 (0.05) 1240 1470 1370 686 (A) (A) (A) (A) Table 4. Correlation of size and contaminant levels in Dolly Varden from the Aleutians. Correlations are given for all islands combined (n=75), fish from Umnak and Adak combined (N=24) and fish from Amchitka (n=51). Correlations for muscle are above the diagonal and liver below. Given are Kendall tau correlations. Island arsenic cadmium chromium lead mercury selenium length weight

All arsenic ********* 0.2 (0.01) NS 0.2 (0.05) -0.3 (<0.0001) NS 0.3 (0.001) 0.2 (0.05) Umnak & Adak ********* NS NS NS NS NS NS 0.3 (0.05) Amchitka ********* NS -0.2 (0.05) NS NS NS NS NS

All cadmium 0.5 (<0.0001) ********* -0.2 (0.05) NS NS NS NS 0.2 (0.02) Umnak & Adak NS ********* NS NS NS NS NS NS Amchitka 0.3 (0.01) ********* -0.3 (0.02) NS NS 0.3 (0.02) NS 0.3 (0.002)

All chromium NS NS ********* 0.3 (0.0005) -0.2 (0.02) -0.2 (0.03) NS NS Umnak & Adak NS NS ********* 0.5 (0.002) -0.3 (0.04) NS 0.3 (0.03) NS Amchitka -0.3 (0.003) NS ********* NS NS NS NS -0.2 (0.02)

All lead NS NS NS ********* NS NS NS NS Umnak & Adak NS NS NS ********* NS NS NS NS Amchitka NS NS NS ********* NS NS -0.2 (0.04) NS

All mercury -0.4 (<0.0001) -0.4 (<0.0001) NS NS ********* NS NS NS Umnak & Adak 0.4 (0.03) 0.4 (0.02) NS NS ********* NS NS NS Amchitka NS -0.2 (0.03) NS NS ********* NS 0.3 (0.01) 0.3 (0.007)

All selenium 0.2 (0.02) 0.2 (0.005) -0.4 (<0.0001) NS NS ********* 0.3 (0.0001) 0.4 (<0.0001) Umnak & Adak NS NS NS NS NS ********* NS NS Amchitka 0.3 (0.002) 0.3 (0.001) -0.4 (<0.0001) NS NS ********* 0.4 (<0.0001) 0.5 (<0.0001)

All length 0.3 (<0.0001) 0.3 (0.0003) -0.2 (0.003) NS -0.2 (0.01)a 0.4 (<0.0001) ********* 0.7 (<0.0001) Umnak & Adak NS NS NS NS NS NS ********* 0.6 (<0.001) Amchitka 0.2 (0.05) NS -0.4 (<0.0001) NS NS 0.5 (<0.0001) ********* 0.8 (<0.0001)

All weight 0.3 (0.002) 0.2 (0.02) -0.3 (<0.0001) NS NS 0.5 (<0.0001) 0.7 (<0.0001) ********* Umnak & Adak NS NS NS NS NS NS 0.6 (0.0005) ********* Amchitka 0.3 (0.009) 0.2 (0.02) -0.4 (<0.0001) NS NS 0.5 (<0.0001) 0.8 (<0.0001) ********* 80 a. This negative correlation probably reflects trophic level differences between landlocked and sea run fish rather than differences in mercury levels due to fish length. Table 5. Correlation between tissues for contaminant levels in Dolly Varden from the Aleutians. Given are Kendall tau correlations. Muscle and Kidney and Liver and liver kidney egg egg kidney egg n=75 n=43 n=27 n=19 n=43 n=27 arsenic 0.5 (<0.0001) 0.4 (0.0007) 0.6 (<0.0001) 0.6 (0.0007) 0.5 (<0.0001) 0.6 (<0.0001)

cadmium 0.2 (0.05)NS NS NS 0.5 (<0.0001) 0.3 (0.02)

chromium 0.2 (0.004) NS NS NS NS NS

leadNSNS -0.4 (0.009) 0.5 (0.01) NS NS

mercury 0.6 (<0.0001) 0.7 (<0.0001) 0.7 (<0.0001) 0.8 (<0.0001) 0.8 (<0.0001) 0.8 (<0.0001)

selenium 0.5 (<0.0001)NS NS 0.3 (0.04) 0.4 (0.0008) 0.5 (0.0002) 81 Table 6. Contaminant levels in 4 organs (egg, kidney, liver, muscle) of Dolly Varden collected from the Aleutian Islands during the summer of 2004. (Given are ppb, wet weight). Egg Kidney Liver Muscle mean ± std. err mean ± std. err mean ± std. err mean ± std. err geometric mean geometric mean geometric mean geometric mean X2 (p) Metals n=27 n=43 n=75 n=75

arsenic 61.5 ± 11.4 199 ± 27.9 127 ± 29.7 69.3 ± 12.3 32.0 (<0.0001) 26.3 111 20.9 5.69 (B) (A) (B) (C)

cadmium 18.5 ± 2.86 200 ± 20.6 78.0 ± 9.45 2.07 ± 1.07 167.6 (<0.0001) 13.9 153 55.3 0.07 (C) (A) (B) (D)

chromium 18.6 ± 1.89 101 ± 20.9 151 ± 77.3 23.1 ± 3.52 72.1 (<0.0001) 16.4 68.9 41.1 3.47 (B) (A) (A) (C)

lead 26.3 ± 7.91 34.2 ± 12.1 19.4 ± 5.98 22.1 ± 4.84 (NS) 0.89 3.38 2.82 0.97

mercury 33.9 ± 7.24 169 ± 24.6 237 ± 23.8 114 ± 12.9 46.4 (<0.0001) 17.9 93.8 151 52.8 (C) (A) (A) (B)

selenium 1150 ± 123 1480 ± 93.9 1210 ± 67.9 349 ± 35.7 109.8 (<0.0001) 986 1360 1040 133

(A) (A) (A) (B) 82 83

Table 7. Gender differences in Metal levels (ppb, wet weight)(ng/g) of Dolly Varden. Given are arithmetic means ±SE (geometric means below) with Kruskal- Wallis Chi Square values and p values.

Male Female X2(p) n=35 n=32 standard length (cm) 30.8 ± 0.9 29.1 ± 0.9 1.6 (NS) weight (g) 402 ± 29.7 304 ± 33.2 7.5 (0.006)

MUSCLE arsenic 74.9 ± 21.6 63.7 ± 16.1 0.1 (NS) 5.83 3.99 cadmium 3.10 ± 2.20 1.16 ± 0.70 3.2 (NS) 0.12 0.04 chromium 19.1 ± 5.40 31.2 ± 5.50 6.9 ( 0.008) 1.50 11.0 lead 15.7 ± 7.30 28.2 ± 7.70 1.7 (NS) 0.45 1.41 mercury 126 ± 16.0 122 ± 23.6 0.6 (NS) 61.9 65.2 selenium 427 ± 56.1 307 ± 52.6 2.0 (NS) 184 97.7 LIVER arsenic 135 ± 53.7 133 ± 36.4 0.5 (NS) 18.9 23.4 cadmium 61.7 ± 6.80 94.3 ± 18.7 0.4 (NS) 52.1 60.4 chromium 199 ± 158 121 ± 64.1 1.2 (NS) 36.3 44.1 lead 13.2 ± 2.30 10.6 ± 2.90 1.6 (NS) 2.77 1.97 mercury 271 ± 30.8 233 ± 41.3 2.6 (NS) 194 135 selenium 1400 ± 93.7 1110 ± 98.4 7.7 (0.005) 1231 985 KIDNEY n=19 n=22 arsenic 210 ± 49.7 197.95 ± 34.3 0.1 (NS) 111 112 cadmium 155 ± 23.0 234 ± 27.67 5.3 (0.02) 120 202 chromium 75.3 ± 11.9 127.02 ± 39.0 0.1 (NS) 62.8 77.1 lead 30.2 ± 20.5 39.8 ± 16.0 1.2 (NS) 2.18 4.90 mercury 204 ± 34.3 150 ± 36.9 2.5 (NS) 132 75.9 selenium 1470 ± 141.98 1520 ± 137 0.0 (NS) 1330 1400 84

Table 8. Risk evaluation for human consumption of Dolly Varden from the Aleutians, based on the average metal level (converted to ug/g or ppm on wet weight basis). Assumptions include a "typical" 70 kg adult, consuming one 228 g (8 ounce) meal per day. Amchitka Intake/70 kg EPA chronic Hazard ELEMENT Mean One meal per day body wgt oral Rfd quotient (ug/g) ug/228 g ug/kg/day ug/kg/day Arsenica 0.012 2.74 0.04 0.3 0.13 Cadmium 0.002 0.46 0.01 10 0.00 Chromiumb 0.018 4.10 0.06 1500 0.00 Leadc 0.012 2.74 0.04 Mercury 0.157 35.80 0.51 0.1 5.11 Selenium 0.393 89.60 1.28 5 0.26

Umnak/Adak Intake/70 kg EPA chronic Hazard ELEMENT Mean One meal per day body wgt oral Rfd quotient (ug/g) ug/228 g ug/kg/day ug/kg/day Arsenica 0.191 43.55 0.62 0.3 2.07 Cadmium 0.002 0.46 0.01 10 0.00 Chromiumb 0.033 7.52 0.11 1500 0.00 Leadc 0.043 9.80 0.14 Mercury 0.024 5.47 0.08 0.1 0.78 Selenium 0.257 58.60 0.84 5 0.17 a. The RfD is for inorganic arsenic. Most of the arsenic in seafood is organic arsenic with low toxicity. b. Chromium in the form of Cr-III is an essential trace element and an allowable daily intake of 1500. The RfD of 0.3 mg/kg/day is set for Cr-VI. For the sake of this risk assessment, the chromium in fish is assumed to be hexavalent. c. Lead does not have an oral RfD. 85

Table 9. Percent of Dolly Varden muscle samples above regulatory action level for mercury. Island Umnak/Adak Amchitka

Sample size (n) 24 51

> 0.1 ppm 0 73

> 0.2 ppm (Canada's maximum level 0 26 for subsistence fisheries)

> 0.3 ppm (EPA freshwater criterion) 0 14

> 0.5 ppm (old FDA action level, 0 2 1969-1979; Health Canada’s current guideline)

> 1.0 ppm (current FDA action level) 0 0

Unalaska Umnak Anchorage Adak Amchitka Bering Sea Bering Pacific Ocean Russia (US) Alaska Figure the three 1. Map showing islands Dolly Vardenwhere collected. were

N 10 km Alaska Adak Isalnd Adak 1 km Kuluk Bay Clam Lagoon Harbor Sweeper Cove Sweeper Andrew Lake Town (Adak)Town Airport Adak Isalnd Sweeper Creek Figure 2. Map showing the location of Dolly Varden collection on Adak.

N Alaska Amchitka Constantine Constantine Harbor Long Shot he locations of Dolly Varden collection on Amchitka. Cannikin Lake Lake Cannikin Fox Lake Atomic Test Site Collection Location Milrow Cannikin Amchitka Island Island Amchitka 10 km Figure 3. Map showing t

N 20 km Alaska Alaska Umnak Umnak Isalnd Umnak of Dolly of Dolly Varden collection on Umnak 1 km Town (Nikolski) Town Umnak Umnak Lake Mueller Cove River Cove Umnak Isalnd Sheep Creek Figure 4. Map showing the location

Figure 5. Arsenic levels in Dolly Varden muscle by standard length.

500 H B Fox Lake 450 J Cannikin Lake F 400 F H Adak 350 F Umnak 300 HF 250 F H H F 200 H F H F 150 F F H F

Arsenic in Muscle (ppb) F 100 H FJF B F J J 50 B J FJ B B B JB J J B J J 0 B BB B JBBBBBBBBJBJBBBJBBJBB B J JJ J J 0 5 10 15 20 25 30 35 40 45 Standard Length (cm)

Figure 6. Cadmium levels in Dolly Varden muscle by standard length. 80 J B Fox Lake

70 J Cannikin Lake

H Adak 60 F Umnak 50

30 Cadmium (ppb) H 20

10 H H JF H B HJ JB FJ FJ 0 B BB BBBBBJBBBBBBJBBBBJBJBJJFBHF BFFFFJHHFJFJ JJFJ J 0 5 10 15 20 25 30 35 40 45 Standard Length (cm)

Figure 7. Chromium levels in Dolly Varden muscle by standard length. 140 B Fox Lake B 120 J Cannikin Lake H Adak B B 100 F Umnak F B 80 B F B F 60 H F F F BB Chromium (ppb) 40 F F B B H F B F F F F 20 B BJ H F B B FJ B J H J B BB B B J JJ J 0 H BB J B BBJHJBHBJJJB BJ J HJ JJJ 0 5 10 15 20 25 30 35 40 45

Standard Length (cm)

Figure 8. Lead levels in Dolly Varden muscle by standard length. 250 B Fox Lake F J Cannikin Lake 200 H Adak F Umnak B 150

100 F B F F F F F

Lead in Muscle (ppb) B F 50 B F F B J JJ B B B B B F B B F 0 H B JB BBBBBBJJJBBBJJHHHBJHBJJJBBH BFJ JJ HJ JFJ F 0 5 10 15 20 25 30 35 40 45

Standard Length (cm)

Figure 9. Mercury levels in Dolly Varden muscle by standard length. 600 B Fox Lake B 500 J Cannikin Lake H Adak 400 F Umnak B B B J 300 BB B B B JJ J 200 J B J BJ B JJ JJJ J B J B B BB J J Mercury in Muscle (ppb) BJ J F 100 B B B H B B H F B FH B BH HFFFF FF F F 0 H BB BBJ H F F H J 0 5 10 15 20 25 30 35 40 45

Standard Length (cm)

Figure 10. Selenium levels in Dolly Varden muscle by standard length. 1200 J B Fox Lake J J 1000 J Cannikin Lake J J H Adak J J 800 F Umnak J J J JJ J J J J J

600 F F B J J J F H 400 B F F H F J F F BBB F B H

Selenium in Muscle (ppb) B H B BFF 200 F F F B B F BB B BB B B HF H B F B B H 0 B BBBBB BF H 0 5 10 15 20 25 30 35 40 45

Standard Length (cm)