Radionuclides and trace elements in fish collected upstream and downstream of Los Alamos national laboratory and the doses to humans from the consumption of muscle and bone

Abstract

The purpose of this study was to determine radionuclide and trace element concentrations in bottom‐feeding fish (catfish, carp, and suckers) collected from the confluences of some of the major canyons that cross Los Alamos National Laboratory (LANL) lands with the Rio Grande (RG) and the potential radiological doses from the ingestion of these fish. Samples of muscle and bone (and viscera in some cases) were analyzed for ³H, ⁹⁰Sr, ¹³⁷Cs, ^totU, ²³⁸Pu, ^239,240Pu, and ²⁴¹Am and Ag, As, Ba, Be, Cr, Cd, Cu, Hg, Ni, Pb, Sb, Se, and Tl. Most radionuclides, with the exception of ⁹⁰Sr, in the muscle plus bone portions of fish collected from LANL canyons/RG were not significantly (p<0.05) higher from fish collected upstream (San Ildefonso/background) of LANL. Strontium‐90 in fish muscle plus bone tissue significantly (p<0.05) increases in concentration starting from Los Alamos Canyon, the most upstream confluence (fish contained 3.4E‐02 pCi g^‐1 [126E‐02 Bq kg^‐1]), to Frijoles Canyon, the most downstream confluence (fish contained 14E‐02 pCi g^‐1 [518E‐02 Bq kg^‐1]). The differences in ⁹⁰Sr concentrations in fish collected downstream and upstream (background) of LANL, however, were very small. Based on the average concentrations (±2SD) of radionuclides in fish tissue from the four LANL confluences, the committed effective dose equivalent from the ingestion of 46 lb (21 kg) (maximum ingestion rate per person per year) of fish muscle plus bone, after the subtraction of background, was 0.1 ± 0.1 mrem y^‐1 (1.0 ± 1.0 μSv y^‐1), and was far below the International Commission on Radiological Protection (all pathway) permissible dose limit of 100 mrem y^‐1 (1000 μSv y^‐1). Of the trace elements that were found above the limits of detection (Ba, Cu, and Hg) in fish muscle collected from the confluences of canyons that cross LANL and the RG, none were in significantly higher (p<0.05) concentrations than in muscle of fish collected from background locations.     

Radionuclides in deer and elk from Los Alamos National Laboratory and the doses to humans from the ingestion of muscle and bone.

This paper summarizes radionuclide concentrations (3H, 90Sr, 137Cs, 238Pu, 239,240Pu, 241Am, and totU) in muscle and bone tissue of mule deer (Odocoileus hemionus) and Rocky Mountain elk (Cervus elaphus) collected from Los Alamos National Laboratory (LANL), Los Alamos, New Mexico, lands from 1991 through 1998. Also, the committed effective dose equivalent (CEDE) and the risk of excess cancer fatalities (RECF) to people who ingest muscle and bone from deer and elk collected from LANL lands were estimated. Most radionuclide concentrations in muscle and bone from individual deer (n = 11) and elk (n = 22) collected from LANL lands were either at less than detectable quantities (where the analytical result was smaller than two counting uncertainties) and/or within upper (95%) level background (BG) concentrations. As a group, most radionuclides in muscle and bone of deer and elk from LANL lands were not significantly higher (p < 0.10) than in similar tissues from deer (n = 3) and elk (n = 7) collected from BG locations. Also, elk that had been radio collared and tracked for two years and spent an average time of 50% of LANL lands were not significantly different in most radionuclides from road kill elk that have been collected as part of the environmental surveillance program. Overall, the upper (95%) level net CEDEs (the CEDE plus two sigma for each radioisotope minus background) at the most conservative ingestion rate (50 lbs of muscle and 13 lbs of bone) were as follows: deer muscle = 0.22 mrem y-1 (2.2 microSv y-1), deer bone = 3.8 mrem y-1 (38 microSv y-1), elk muscle = 0.12 mrem y-1 (1.2 microSv y-1), and elk bone = 1.7 mrem y-1 (17 microSv y-1). All CEDEs were far below the International Commission on Radiological Protection guideline of 100 mrem y-1 (1000 microSv y-1), and the highest muscle plus bone net CEDE corresponded to a RECF of 2E-06, which is far below the Environmental Protection Agency upper level guideline of 1E-04.     

Radionuclides in deer and elk from Los Alamos national laboratory and the doses to humans from the ingestion of muscle and bone

Abstract

This paper summarizes radionuclide concentrations (³H, ⁹⁰Sr, ¹³⁷Cs, ²³⁸Pu, ^239,240Pu, ²⁴¹Am, and ^totU) in muscle and bone tissue of mule deer (Odocoileus hemionus) and Rocky Mountain elk (Cervus elaphus) collected from Los Alamos National Laboratory (LANL), Los Alamos, New Mexico, lands from 1991 through 1998. Also, the committed effective dose equivalent (CEDE) and the risk of excess cancer fatalities (RECF) to people who ingest muscle and bone from deer and elk collected from LANL lands were estimated. Most radionuclide concentrations in muscle and bone from individual deer (n = 11) and elk (n = 22) collected from LANL lands were either at less than detectable quantities (where the analytical result was smaller than two counting uncertainties) and/or within upper (95%) level background (BG) concentrations. As a group, most radionuclides in muscle and bone of deer and elk from LANL lands were not significantly higher (p<0.10) than in similar tissues from deer (n = 3) and elk (n = 7) collected from BG locations. Also, elk that had been radio collared and tracked for two years and spent an average time of 50% on LANL lands were not significantly different in most radionuclides from road kill elk that have been collected as part of the environmental surveillance program. Overall, the upper (95%) level net CEDEs (the CEDE plus two sigma for each radioisotope minus background) at the most conservative ingestion rate (50 lbs of muscle and 13 lbs of bone) were as follows: deer muscle = 0.22 mrem y^‐1 (2.2 μSv y^‐1), deer bone = 3.8 mrem y^‐1 (38 μSv y^‐1), elk muscle = 0.12 mrem y^‐1 (1.2 μSv y^‐1), and elk bone = 1.7 mrem y^‐1 (17 μSv y^‐1). All CEDEs were far below the International Commission on Radiological Protection guideline of 100 mrem y^‐1 (1000 μSv y^‐1), and the highest muscle plus bone net CEDE corresponded to a RECF of 2E‐06, which is far below the Environmental Protection Agency upper level guideline of 1E‐04.     

Radionuclides in pinon pine (Pinus edulis) nuts from Los Alamos National Laboratory lands and the dose from consumption

One of the dominant tree species growing within and around the eastern portion of Los Alamos National Laboratory (LANL), Los Alamos, NM, lands is the pinon pine (Pinus edulis). Pinon pine is used for firewood, fence posts, and building materials and is a source of nuts for food--the seeds are consumed by a wide variety of animals and are also gathered by people in the area and eaten raw or roasted. This study investigated the (1) concentration of 3H, 137Cs, 90Sr, totU, 238Pu, 239,240Pu, and 241Am in soils (0- to 12-in. [31 cm] depth underneath the tree), pinon pine shoots (PPS), and pinon pine nuts (PPN) collected from LANL lands and regional background (BG) locations, (2) committed effective dose equivalent (CEDE) from the ingestion of nuts, and (3) soil to PPS to PPN concentration ratios (CRs). Most radionuclides, with the exception of 3H in soils, were not significantly higher (p < 0.10) in soils, PPS, and PPN collected from LANL as compared to BG locations, and concentrations of most radionuclides in PPN fromLANL have decreased over time. The maximum net CEDE (the CEDE plus two sigma minus BG) at the most conservative ingestion rate (10 lb [4.5 kg]) was 0.0018 mrem (0.018 microSv); this is far below the International Commission on Radiological Protection (all pathway) permissible dose limit of 100 mrem (1000 microSv). Soil-to-nut CRs for most radionuclides were within the range of default values in the literature for common fruits and vegetables.     

Exposure assessment for trace elements from consumption of marine fish in Southeast Asia

Concentrations of 20 trace elements were determined in muscle and liver of 34 species of marine fish collected from coastal areas of Cambodia, Indonesia, Malaysia and Thailand. Large regional difference was observed in the levels of trace elements in liver of one fish family (Carangidae): the highest mean concentration was observed in fish from the Malaysian coastal waters for V, Cr, Zn, Pb and Bi and those from the Java Sea side of Indonesia for Sn and Hg. To assess the health risk to the Southeast Asian populations from consumption of fish, intake rates of trace elements were estimated. Some marine fish showed Hg levels higher than the guideline values by U.S. Environmental Protection Agency and Joint FAO/WHO Expert Committee on Food Additives (JECFA). This suggests that consumption of these fish may be hazardous to the people.     

Residues in fish exposed to sublethal doses of endosulfan and fish collected from cotton growing area

A one step extraction and cleanup procedure for determining endosulfan in fish was investigated. Minced Fish was mixed with trisodium citrate, disodium hydrogen orthophosphate and sodium sulphate into a dry powdery mixture, which was eluted through silicic acid and alumina with a mixture of dichloromethane and hexane. The eluate was concentrated and chromatographed on GLC using an EC detector without further cleanup. Three species of fresh water fish exposed to 0.7-16 micrograms/litre-1 technical grade endosulfan in tanks for various periods of time were found to concentrate both alpha and beta endosulfan and metabolise them to sulfate, diol, ether and lactone. Fish collected from Gwydir River in the cotton growing area in summer (Dec. 1986-Feb. 1987) were found to contain endosulfan residues suggesting endosulfan is quite stable in the environment and can cause residues.     

Bioaccumulation of trace elements in pelagic fish from the Western Indian Ocean

Trace elements were analyzed in fish of commercial interest to determine their importance in marine systems of the Western Indian Ocean and their bioaccumulation patterns. The results are equivalent or lower than levels reported in ichthyofauna worldwide. Certain values of muscular Cd, Hg, Pb and Zn were, however, above thresholds for human consumption. Levels varied among tissues, species and fish length, but were seldom influenced by the nutritional condition of the fish, its gender and its reproductive status. Correlations between hepatic Hg and Se levels in Swordfish (r2=0.747) and Yellowfin Tunas (r2=0.226), and among metallothionein linking metals imply the existence of detoxification processes in these species. Level differences between fish from the Mozambique Channel and Reunion Island reflect differences of diets rather than differences of elemental availability in both environments.     

Butyltins in muscle and liver of fish collected from certain Asian and Oceanian countries

Concentrations of butyltin residues were determined in muscle tissue of fish collected from local markets and sea food shops in India, Bangladesh, Thailand, Indonesia, Vietnam, Taiwan, Australia, Papua New Guinea and the Solomon Islands. Contamination levels were determined in the Asia-Pacific region and human exposure was estimated. Similarly, corresponding liver samples of fish muscle collected in Australia, Papua New Guinea and the Solomon Islands were analyzed to obtain information on partitioning of butyltin compounds between muscle and liver tissues. Butyltin compounds were detected in most of the samples which suggested widespread contamination in Asia and Oceania. The concentrations of butyltin compounds were, on average, an order of magnitude higher in liver than in muscle. Residue concentration of Sigmabutyltin in liver was found to be correlated significantly (p < 0.02) with those in muscle. Intensive ship-scrapping activities, sewage disposal and antifouling paints are considered the major sources of butyltins in this region. Increased proportions of MBT over DBT and TBT in samples from most locations indicated degradation of TBT to MBT in fish tissues during storage at 4 degrees C in the dark over 1-2 years. The possibility that fish have been subject to increased exposure to MBT and that TBT degrades to MBT quite rapidly in tropical environments are also considered. Butyltin concentrations in fish from Asia and Oceania were lower than those reported for Japan, Canada and the USA. Although the number of samples analyzed from each country was small, it is tentatively suggested that intake of butyltins by humans via consumption of fish in these countries was < 25% of the tolerable daily intake of 250 ng kg bw(-1) day(-1). To our knowledge, this is the first study reporting on butyltin pollution in developing Asian countries.     

Historical deposition of mercury and selected trace elements to high-elevation National Parks in the Western U.S. inferred from lake-sediment cores

Atmospheric deposition of Hg and selected trace elements was reconstructed over the past 150 years using sediment cores collected from nine remote, high-elevation lakes in Rocky Mountain National Park in Colorado and Glacier National Park in Montana. Cores were age dated by ²¹⁰Pb, and sedimentation rates were determined using the constant rate of supply model. Hg concentrations in most of the cores began to increase around 1900, reaching a peak sometime after 1980. Other trace elements, particularly Pb and Cd, showed similar post-industrial increases in lake sediments, confirming that anthropogenic contaminants are reaching remote areas of the Rocky Mountains via atmospheric transport and deposition. Preindustrial (pre-1875) Hg fluxes in the sediment ranged from 5.7 to 42 μg m^?2 yr^?1 and modern (post-1985) fluxes ranged from 17.7 to 141 μg m^?2 yr^?1. The average ratio of modern to preindustrial fluxes was 3.2, which is similar to remote lakes elsewhere in North America. Estimates of net atmospheric deposition based on the cores were 3.1 μg m^?2 yr^?1 for preindustrial and 11.7 μg m^?2 yr^?1 for modern times. Current-day measurements of wet deposition range from 5.0 to 8.6 μg m^?2 yr^?1, which are lower than the modern sediment-based estimate of 11.7 μg m^?2 yr^?1, perhaps owing to inputs of dry-deposited Hg to the lakes.     

Levels of trace elements in green turtle eggs collected from Hong Kong: Evidence of risks due to selenium and nickel

Concentrations of 22 trace elements were determined in green turtle (Chelonia mydas) eggs collected from Hong Kong. Concentrations of selenium, lead and nickel in these eggs were generally higher than those reported in other studies. The predicted no effect concentrations (PNEC; ng/g wet weight) of Pb (1000), Se (340 and 6000 for the worst-case and best-case scenarios, respectively) and Ni (17) in the green turtle eggs were estimated. Hazard quotients (HQs) estimate that Se (HQs: 0.2-24.5) and Ni (HQs: 4.0-26.4) may pose some risks to the turtles. Our study also found that concentrations of Ag, Se, Zn, Hg and Pb in the shell of the turtle eggs were significantly correlated with levels in the whole egg contents (yolk+albumen). Once the precise relationships of specific elements are established, egg-shell concentrations may be used as a non-lethal, non-invasive, surrogate for predicting whole egg burden of certain contaminants in marine turtles.     

Contamination by arsenic and other trace elements in tube-well water and its risk assessment to humans in Hanoi, Vietnam

Concentrations of As and other trace elements and their association were examined in groundwater (n = 25) and human hair (n = 59) collected at Gia Lam District and Thanh Tri District, suburban areas of Hanoi, Vietnam, in September 2001. Concentrations of As in the groundwater ranged from <0.10 to 330 microg/l, with about 40% of these exceeding WHO drinking water guideline of 10 microg/l. Also, 76% and 12% of groundwater samples had higher concentrations of Mn and Ba than WHO drinking water guidelines, respectively. Arsenic concentrations in hair of residents in Gia Lam and Thanh Tri Districts (range 0.088-2.77 microg/g dry wt.) were lower than those in other As-contaminated areas of the world, but were higher than those of people in non-contaminated areas. Concentrations of As and Mn in hair of some individuals from the Gia Lam and Thanh Tri Districts exceeded the level associated with their toxicity and, therefore, a potential health risk of As and Mn is a concern for the people consuming the contaminated water in this area. Cumulative As exposure was estimated to be lower than the threshold levels at the present, which might explain the absence of manifestations of chronic As poisoning and arsenicosis in the residents of Gia Lam and Thanh Tri Districts. To our knowledge, this study revealed for the first time that the residents are exposed not only to As but also Mn and Ba from groundwater in the Red River Delta, Vietnam.     

Silver and other trace elements in a freshwater fish, Carasius auratus langsdorfii, from the Asakawa River in Tokyo, Japan

The concentrations of silver (Ag) in a typical freshwater fish in Japan, Carasius auratus langsdorfii, and some other species have been determined to examine the Ag-contamination of fish and to specify the Ag accumulating species and part. They were dissected roughly into four parts, and analyzed by an instrumental neutron activation analysis. It was found that Ag was accumulated in the samples from the Asakawa River, and that the Ag concentration in the entrails of C. auratus langsdorfi reached 12 microg g(-1). The analysis of a C. auratus langsdorfii, which was dissected into 13 individual organs, showed that the Ag was accumulated highly in the liver, followed by the gallbladder and kidney. The inter-species and inter-part distributions of other trace elements have also been studied.     

Radionuclides in pinon pine (Pinus edulis) nuts from los alamos national laboratory lands and the dose from consumption

Abstract

One of the dominant tree species growing within and around the eastern portion of Los Alamos National Laboratory (LANL), Los Alamos, NM, lands is the pinon pine (Pinus edulis). Pinon pine is used for firewood, fence posts, and building materials and is a source of nuts for food—the seeds are consumed by a wide variety of animals and are also gathered by people in the area and eaten raw or roasted. This study investigated the (1) concentration of ³H, ¹³⁷Cs, ⁹⁰Sr, ^totU, ²³⁸Pu, ^{239, 240}Pu, and²⁴¹ Am in soils (0‐ to 12‐in. [31 cm] depth underneath the tree), pinon pine shoots (PPS), and pinon pine nuts (PPN) collected from LANL lands and regional background (BG) locations, (2) committed effective dose equivalent (CEDE) from the ingestion of nuts, and (3) soil to PPS to PPN concentration ratios (CRs). Most radionuclides, with the exception of ³H in soils, were not significantly higher (p < 0.10) in soils, PPS, and PPN collected from LANL as compared to BG locations, and concentrations of most radionuclides in PPN from LANL have decreased over time. The maximum net CEDE (the CEDE plus two sigma minus BG) at the most conservative ingestion rate (10 lb [4.5 kg]) was 0.0018 mrem (0.018 μSv); this is far below the International Commission on Radiological Protection (all pathway) permissible dose limit of 100 mrem (1000 μSv). Soil‐to‐nut CRs for most radionuclides were within the range of default values in the literature for common fruits and vegetables.     

Concentrations of polychlorinated dibenzo-p-dioxins and furans in fish downstream from a Ky-5 manufacturing

Concentrations of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) were studied in seven fish species, burbot (Lota lota), pike (Esox lucius), perch (Perca fluviatilis), pikeperch (Stizopedion lucioperca), bream (Abramis brama), salmon (Salmo salar) and Baltic herring (Clupea harengus membras) in River Kymijoki and its estuary polluted by Ky-5 manufacturing. The fish were caught at 14 localities along the river and its estuary. The selected species represent different trophic levels and/or inhabit different environments. The concentrations of PCDD/Fs were low, in most samples below 1 pg g(-1) ITEQ (NATO/CCMS 1988) fresh weight (fw) in muscle, except salmon and Baltic herring. These two species graze at the open sea and consequently accumulate contaminants at a large area in the Baltic Sea. The lipid content in salmon and Baltic herring was an order of magnitude higher than in other species. PCDD/Fs in fish muscle showed only slightly elevated levels in the Kymijoki area and its estuary as compared to the levels in the same species in Finnish freshwaters and sea areas. The concentration of the main impurities of the fungicide Ky-5 was higher in the Kymijoki River downstream the Ky-5 manufacturing place compared to the up-stream locations. The PCDD/F concentrations in fish liver and spawn were 10-100 times higher than the concentration in muscle, because of the much higher lipid concentrations of these organes. Consequently, the tolerable daily intake values could be as much as 100 times smaller (M. Korhonen, M. Verta, T. Vartiainen, Organohalog. Comp. 32 (1997) 305-310; P. Mikkelson, J. Paasivirta, H. Kiviranta, Organohalog. Comp. 39 (1998) 59-62).     

Estimation of the atmospheric emissions of trace elements from anthropogenic sources in Europe

The total emissions of 15 elements from various anthropogenic sources in Europe are presented here. The data were obtained on the basis of trace element emission factors and statistical information on the consumption of ores, rocks and fuels and the production of various types of industrial goods. Available information on types of fuels, ores and rocks and differences in manufacturing techniques used in the European countries have been taken into account. Different types of dust removal installations and their effectiveness have also been considered, as well as import-export relations of fuels and ores between particular countries. The author assessed the spatial distributions of trace element emissions based on information on location of industrial areas in Europe and plant capacities.     

Use of mosses to study atmospheric deposition of trace elements: contributions from investigations in Norway

This paper presents essential features of biomonitoring work carried out in the author's laboratory during more than 25 years using various analytical techniques for the determination of over 50 elements. A substantial part of this work concerns large-scale deposition surveys in Norway using the moss Hylocomium splendens, where five nationwide surveys have been carried out since 1977. Considerable efforts have also been spent on intercalibration of different species of mosses and transformation of concentrations in moss to absolute deposition rates. Other significant activities include establishment of recommended values for moss reference samples, source apportionment of lead in mosses by stable isotope ratios and monitoring of local metal deposition around factories. Experience from this work has facilitated a critical evaluation of the contribution from sources other than atmospheric deposition to the elemental composition of the moss, as well as factors leading to depletion of elements in the moss. Recent work indicates that mosses may also be suitable for the monitoring of persistent halogenated organic pollutants and ¹³⁷Cs deposition.     

A preliminary risk assessment of trace elements accumulated in fish to the Indo-Pacific Humpback dolphin (Sousa chinensis) in the northwestern waters of Hong Kong

In order to assess the potential risks associated with consumption of contaminated prey items to the Indo-Pacific Humpback dolphin (Sousa chinensis), fish species (Collichthys lucida, Pseudosciaena crocea, Johnius sp., Thryssa sp., Mugil sp. and Trichiurus sp.) representing the main food items of the dolphin were collected from the northwestern waters of Hong Kong, including the Sha Chau and Lung Kwu Chau Marine Park, which form the main habitat of the dolphin in Hong Kong. Within these waters, there are several potential sources of pollution including significant inputs from the Pearl River catchment, several major sewage outfalls and a series of mud pits that receive contaminated dredged sediments. Concentrations of thirteen trace elements (Ag, As, Cd, Co, Cr, Cs, Cu, Hg, Mn, Ni, Se, V, and Zn) in the fish tissue were analyzed by inductively coupled plasma mass spectrometer (ICP-MS). An assessment of the risks of adverse effects on the dolphin due to consumption of tainted fish was undertaken using two toxic reference benchmarks, namely the reference dose (RfD) and toxicity reference value (TRV). The risk quotient (RQ) calculated for each element showed that the risks from consumption of fish were generally low and within safe limits. The risks associated with arsenic, cadmium and mercury were, however, elevated. The highest calculated RQ was associated with total arsenic; however, the majority of arsenic in marine organisms tends to be in the non-toxic organic form, and the actual risk to the dolphin due to this metalloid is likely to be lower.     

Distribution of metals and trace elements in adult and juvenile penguins from the Antarctic Peninsula area

The presence of metals in the Antarctic environment is principally a natural phenomenon caused by geochemical characteristics of the region, although some anthropogenic activities can increase these natural levels. Antarctic penguins present several of the characteristics of useful sentinels of pollution in Antarctica such as they are long-lived species situated at the top of food web. The concentrations of Al, Cr, Mn, Fe, Ni, Cu, Zn, As, Se, Cd, and Pb were determined by inductively coupled plasma–mass spectrometry in samples of liver, kidney, muscle, bone, feather, and stomach contents of gentoo, chinstrap, and Adélie penguin (12 adults, five juveniles) from carcasses of naturally dead individuals collected opportunistically in the Antarctic Peninsula area. The obtained results showed that accumulation and magnification of several elements can be occurring, so that Cd and Se reached levels potentially toxic in some specimens. The presence of human activities seems to be increasing the presence of toxic metals such as Mn, Cr, Ni, or Pb in penguins.     

Polychlorinated dibenzo-p-dioxins and dibenzofurans in commercial diphenyl ether herbicides,and in freshwater fish collected from the application area

This paper describes the analyses of polychlorinated dibenzodioxins, dibenzofurans, and related compounds in diphenyl ether herbicides, CNP, NIP, and X-52. The levels of tetra-, penta-CDDs, and tetra-CDFs were about 150, 30, and 15 ppm, respectively in CNP formulations. NIP and X-52 contained lower chlorine alalogs. Isomer distribution of PCDDs in CNP agreed with an estimate from the reaction of chlorophenols. Freshwater fish samples heavily contaminated with CNP in the application season also contained 0.2 ppb of 1,3,6,8-tetra-CDD.     

Exposure Assessment of methyl mercury from consumption of fish and seafood in Peninsular Malaysia

Environmental Science and Pollution Research - The concentration of meHg in freshwater fish and seafood was investigated, as well as the consumption patterns of fish and seafood by different...