Fukushima fallout in Northwest German environmental media

Traces of short- and long-lived fallout isotopes (¹³¹I, ¹³⁴Cs and ¹³⁷Cs) were found in environmental samples collected in Northwest Germany (rain water, river sediment, soil, grass and cow milk) from March to May 2011, following the radioactivity releases after the nuclear accident in Fukushima, Japan. The measured concentrations are consistent with reported concentrations in air, amount of rainfall and expected values applying simple radioecological models. The [¹³⁴Cs]/[¹³⁷Cs] ratio reported for air (about 1) allows for discrimination between “recent” and “old” ¹³⁷Cs. Expected ¹³⁶Cs values fell below the detection limits of the instrumentation, despite large sample masses and long counting times.     

Study of environmental burden of lead in children using teeth as bioindicator

The south region of Sao Paulo city hosts the Guarapiranga dam, responsible for water supply to 25% of the city population. Their surroundings have been subject to intense and irregular occupation by people from very low socioeconomics classes. Measurements undertaken on sediment and particulate materials in the dam revealed concentrations of lead, copper, zinc and cadmium above internationally accepted limits. Epidemiological and toxicological studies undertaken by the World Health Organization in individuals exhibiting lead concentrations in blood, near or below the maximum recommended (10 µg dl^? 1), surprisingly revealed that toxic effects are more intense in individuals belonging to low socioeconomics classes. Motivated by these facts, we aimed at the investigation of chronic incorporation of lead, as well as the use of our BIOKINETICS code, which is based on an accepted ICRP biokinetics model for lead, in order to extrapolate the results from teeth to other organs. The focus of our data taking was children from poor families, living in a small, restrict and allegedly contaminated area in São Paulo city. Thus, a total of 74 human teeth were collected. The average concentration of lead in teeth of children 5 to 10 years old was determined by means of a high-resolution inductively coupled plasma mass spectrometer (ICP-MS). For standardization of the measurements, an animal bone certified material (H-Animal Bone), from the International Atomic Energy Agency, was analyzed. The amount of lead in children living in the surroundings of the dam, was approximately 40% higher than those from the control region, and the average lead concentration was equal to 1.3 μg g^? 1 approximately. Grouping the results in terms of gender, tooth type and condition, it was concluded that a carious molar of boys is a much more efficient contamination pathway for lead, resulting in concentrations 70% higher than in the control region. We also inferred the average concentrations of lead in other organs of these children, by making use of our BIOKINETIC code.     

Dynamic model for radionuclide uptake in lichen

Samples of atmospheric particulate material and terrestrial plants, including lichens, were collected in New Brunswick, Canada between 1980 and 1983 and analyzed for a wide range of artificial and naturally-occuring radionuclides, including fission products (¹⁴¹Ce, ¹⁴⁴Ce, ¹⁰³Ru, ¹⁰⁶Ru, ⁹⁵Zr and ¹³⁷Cs) derived from the 16 October 1980 Chinese nuclear test. Activity ratios of some of the short-lived fission products in air particulates and lichens are in reasonable agreement with those predicted from fission product yields for nuclear weapons tests, indicating that only minor fractionation occurred for these radionuclides during their transport through air particulate and lichen environmental phases. The ⁷Be inventories measured in a suite of lichen (Cladonia rangiferina) samples were used to calibrate each lichen plant for its collection efficiency for atmospheric particulates and fallout radioactivity.A lichen model has been developed to predict lichen inventories of radioactivity for different lichen growth functions and bio-elimination rates. Assuming that lichen growth results in a linear increase in surface area with time, the experimental results yield biological residence times of 1–2 years for ²¹⁰Pb and Pu and 5–8 years for ¹³⁷Cs. The more efficient retention of ¹³⁷Cs is probably due to its physiological uptake in lichen plants as a proxy for potassium, as evidenced by an observed, inverse relationship between ¹³⁷Cs and ⁴⁰K activities in lichen.     

Heavy metals in sediments from Makupa and Port-Reitz Creek systems: Kenyan Coast

Copper, zinc, lead and cadmium heavy metals were determined in sediments from the Kenyan Coast. Sediment samples were obtained from Makupa and Port Reitz Creek systems. The samples were digested using concentrated hydrochloric acid and the metal content determined using Atomic Absorption Spectrophotometer (AAS). The method of analysis was evaluated using Soil-7 certified reference material (International Atomic Energy Agency, IAEA). For comparison, sediment samples were also analysed using Energy Dispersive X-ray fluorescence technique and results obtained show good agreement. Higher metal concentrations were obtained in Makupa Creek sediments (Cu, 102+/-46.0; Zn, 1017+/-840; Pb, 103+/-35.8; Cd, 51.0+/-14.3) as compared to Port Reitz Creek system (Cu, 21.6+/-7.1; Zn, 57.1+/-17.9; Pb, 26.2+/-11.6; Cd, 1.38+/-0.7). There was significant (p=0.05) variation in the elemental concentrations between and within sites. Industrial activities and a nearby municipal dumpsite were associated with the higher elemental concentrations particularly in Makupa Creek.     

Indoor and outdoor Radon concentration measurements in Sivas, Turkey, in comparison with geological setting

Indoor and soil gas Radon (²²²Rn) concentration measurements were accomplished in two stages in Sivas, a central eastern city in Turkey. In the first stage, CR-39 passive nuclear track detectors supplied by the Turkish Atomic Energy Authority (TAEA) were placed in the selected houses throughout Sivas centrum in two seasons; summer and winter. Before the setup of detectors, a detailed questionnaire form was distributed to the inhabitants of selected houses to investigate construction parameters and properties of the houses, and living conditions of inhabitants. Detectors were collected back two months later and analysed at TAEA laboratories to obtain indoor ²²²Rn gas concentration values. In the second stage, soil gas ²²²Rn measurements were performed using an alphameter near the selected houses for the indoor measurements. Although ²²²Rn concentrations in Sivas were quite low in relation with the allowable limits, they are higher than the average of Turkey. Indoor and soil gas ²²²Rn concentration distribution maps were prepared seperately and these maps were applied onto the surface geological map. In this way, both surveys were correlated with the each other and they were interpreted in comparison with the answers of questionnaire and the geological setting of the Sivas centrum and the vicinity.     

Sediment budgets and source determinations using fallout Cesium-137 in a semiarid rangeland watershed,Arizona, USA

Analysis of soil redistribution and sediment sources in semiarid and arid watersheds provides information for implementing management practices to improve rangeland conditions and reduce sediment loads to streams. The purpose of this research was to develop sediment budgets and identify potential sediment sources using ¹³⁷Cs and other soil properties in a series of small semiarid subwatersheds on the USDA ARS Walnut Gulch Experimental Watershed near Tombstone, Arizona, USA. Soils were sampled in a grid pattern on two small subwatersheds and along transects associated with soils and geomorphology on six larger subwatersheds. Soil samples were analyzed for ¹³⁷Cs and selected physical and chemical properties (i.e., bulk density, rocks, particle size, soil organic carbon). Suspended sediment samples collected at measuring flume sites on the Walnut Gulch Experimental Watershed were also analyzed for these properties. Soil redistribution measured using ¹³⁷Cs inventories for a small shrub-dominated subwatershed and a small grass-dominated subwatershed found eroding areas in these subwatersheds were losing −5.6 and −3.2 t ha⁻¹ yr⁻¹, respectively; however, a sediment budget for each of these subwatersheds, including depositional areas, found net soil loss to be −4.3 t ha⁻¹ yr⁻¹ from the shrub-dominated subwatershed and −0.1 t ha⁻¹ yr⁻¹ from the grass-dominated subwatershed. Generally, the suspended sediment collected at the flumes of the six other subwatersheds was enriched in silt and clay. Using a mixing model to determine sediment source indicated that shrub-dominated subwatersheds were contributing most of the suspended sediment that was measured at the outlet flume of the Walnut Gulch Experimental Watershed. The two methodologies (sediment budgets and sediment source analyses) indicate that shrub-dominated systems provide more suspended sediment to the stream systems. The sediment budget studies also suggest that sediment yields measured at the outlet of a watershed may be a poor indicator of actual soil redistribution rates within these semiarid watersheds. Management of these semiarid rangelands must consider techniques that will protect grass-dominated areas from shrub invasion to improve rangeland conditions.     

Cs, Pu concentrations and the Pu/Pu atom ratio in a sediment core from the sub-aqueous delta of Yangtze River estuary

A sediment core collected from the sub-aqueous delta of the Yangtze River estuary was subjected to analyses of ¹³⁷Cs and plutonium (Pu) isotopes. The ¹³⁷Cs was measured using γ-spectrometry at the laboratories at the Nanjing University and Pu isotopes were determined with Accelerator Mass Spectrometry (AMS), measurements made at the Australian National University. The results show considerable structure in the depth concentration profiles of the ¹³⁷Cs and ^239+240Pu. The shape of the vertical ¹³⁷Cs distribution in the sediment core was similar to that of the Pu. The maximum ¹³⁷Cs and ^239+240Pu concentrations were 16.21 ± 0.95 mBq/g and 0.716 ± 0.030 mBq/g, respectively, and appear at same depth. The average ²⁴⁰Pu/²³⁹Pu atom ratio was 0.238 ± 0.007 in the sediment core, slightly higher than the average global fallout value. The changes in the ²⁴⁰Pu/²³⁹Pu atom ratios in the sediment core indicate the presence of at least two different Pu sources, i.e., global fallout and another source, most likely close-in fallout from the Pacific Proving Grounds (PPG) in the Marshall Islands, and suggest the possibility that Pu isotopes are useful as a geochronological tool for coastal sediment studies. The ¹³⁷Cs and ^239+240Pu inventories were estimated to be 7100 ± 1200 Bq/m² and 407 ± 27 Bq/m², respectively. Approximately 40% of the ^239+240Pu inventory originated from the PPG close-in fallout and about 50% has derived from land-origin global fallout transported to the estuary by the river. This study confirms that AMS is a useful tool to measure ²⁴⁰Pu/²³⁹Pu atom ratio and can provide valuable information on sedimentary processes in the coastal environment.     

A study of radionuclides, metals and stable lead isotope ratios in sediments and soils in the vicinity of natural U-mineralisation areas in the Northern Territory

Australian guidelines recommend that tailings materials from uranium (U) mining and milling be contained without any detrimental impact on the environment for at least 1000 years. Natural analogue sites are being investigated to determine if they can provide data on the rates of natural erosion processes which occur over these timescales, for input into predictive geomorphic computer models. This paper presents radionuclide, metal and stable lead (Pb) isotope data from sediment cores and surface soils in the vicinity of two mineralised areas in the Alligator Rivers Region.Surface scrapes from the natural Anomaly #2, south of the Ranger mineral lease, exhibit radiogenic ²⁰⁶Pb/²⁰⁷Pb and ²⁰⁸Pb/²⁰⁷Pb ratios, and elevated U and metal concentrations typical for a near surface U anomaly. In contrast, samples taken from the Koongarra mineral lease (KML) show radionuclide activity and metal concentrations similar to natural areas elsewhere in the Alligator Rivers Region and Pb isotope ratios are closer to present day average crustal ratios (PDAC), as the orebodies at KML are covered by surficial sand. A sediment core collected from Anbangbang Billabong, downstream of KML, exhibits small variations in Pb isotope ratios that indicate that approximately 1% of the upper sediments in the sediment core may be derived from material originating from the U anomaly at Koongarra.     

Determination of total content and isotopic compositions of plutonium and uranium in environmental samples for safeguards purposes by ICP-QMS

The aim of this work was to determine the concentrations and isotopic compositions of plutonium and uranium in environmental samples for safeguards purposes. An analytical method was developed with a plutonium and uranium separation procedure based on extraction chromatography (using 2 mL TEVA and UTEVA columns) and detection with a quadrupole ICP-MS applying an ultra-sonic nebulizer coupled with a membrane desolvation system. Starting from blank swipes, the background equivalent concentration (BEC) was 8 fg for ²³⁹Pu and 1 ng ²³⁸U. The method was successfully applied to certified reference materials as well as to round robin samples obtained in the framework of the inter-laboratory exercise program, promoted by the Brazilian–Argentine Agency for Accounting and Control of Nuclear Materials (ABACC), together with the US Department of Energy (USDOE). After the introduction of an additional ion-exchange separation step, the methodology was applied to the IAEA-384 sediment reference sample with precise and accurate total plutonium and uranium, ²⁴⁰Pu/²³⁹Pu, ²⁴¹Pu/²³⁹Pu, ²³⁴U/²³⁸U and ²³⁵U/²³⁸U atomic ratio results.     

Carbon-14, tree rings,and urban air pollution

Differences in natural ¹⁴C content of rings from trees from urban and rural locations have been compared on a year by year basis. The differences as a fraction of the urban tree's radioactivity reflect the local excess ¹⁴C-free carbon dioxide from fossil fuel combustion in the urban environment. New York City, Boston, and Washington, D.C., show different degrees of excess carbon dioxide. New York City averages about 6% excess carbon dioxide between 1950 and 1970. From this is infered an average carbon monoxide concentration during this period of 5 ppm.     

Beryllium-7 atmospheric deposition and sediment inventories in the Neponset River estuary,Massachusetts, USA

Measured monthly atmospheric depositional fluxes of cosmogenically produced ⁷Be ranged from 1 to 67 mBq/cm² in Boston, Massachusetts between September 2000 and August 2007. These fluxes exhibited seasonality and supported a decay-corrected ⁷Be atmospheric depositional running inventory that ranged from 36 to 144 mBq/cm². Annual ⁷Be deposition exhibited an increasing trend that may reflect a general decrease in solar activity and a general increase in precipitation over the 7-year sampling period. To investigate short-term sediment dynamics and accumulation patterns in the Neponset River estuary, we collected six sediment cores in July 2006 and measured ⁷Be sediment inventories ranging from 48 to 546 mBq/cm² Comparisons of these sediment inventories with the ⁷Be running inventory from atmospheric deposition (101 mBq/cm²) at the time of core collection indicated a large degree of spatial heterogeneity in sediment accumulation patterns and its potential use as a tool for assessing the impacts of environmental restoration activities in estuarine environments.     

Spatial distribution of U isotopes in sea-water sediments, Red Sea, Egypt

Isotopes of uranium in the sea-water sediments collected from two different areas (El Hamraween harbour and Ras El Behar) on the Egyptian coast of the red sea have been studied using radiochemical separation procedures and alpha-particle spectrometry. Activity concentrations of ²³⁸U, ²³⁵U, ²³⁴U were calculated. The activities observed indicated enhanced radioactivity levels in sea-water sediments of El Hamraween harbour area due to the activities of phosphate shipment operation. Secular equilibrium between ²³⁴U and ²³⁸U was found in the analyzed samples. The average activity ratio of ²³⁵U/²³⁸U was close to the value 0.046 for uranium in nature.     

Fallout distribution in Padua and Northeast Italy after the chernobyl nuclear reactor accident

The radioactive cloud from the Chernobyl nuclear reactor accident arrived in northeast Italy on 30 April 1986. Ground-level air activities detected in Padua reached maximum values of 28·6, 19·2, 3·3, 1·7 and 7·5 Bq m⁻³ for ¹³¹I, ¹³²Te(¹³²I), ¹³⁷Cs and ¹⁰³Ru, respectively, on 1 May; about 10 days later, the activities had fallen to less than 1% of peak values. Considerations of cloud homogeneity are reported.The distribution of fallout radionuclides in Padua was evaluated on the basis of radioactivity detected on natural surfaces. The average committed dose equivalent to the thyroid for adult people in Padua through ¹³¹I inhalation was estimated at 0·37 mSv. Soil activity was monitored daily in samples collected in Padua during the first weeks of May 1986. Fallout deposition over northeast Italy was measured on 75 surface soil samples collected during June 1986 and long-lived radionuclide distribution maps were derived.     

Plutonium isotopes concentration in seawater and bottom sediment off the Pacific coast of Aomori sea area during 1991-2005

A radioactivity survey was launched in 1991 to determine the background levels of ^239+240Pu in the marine environment off a commercial spent nuclear fuel reprocessing plant before full operation of the facility. Particular attention was focused on the ²⁴⁰Pu/²³⁹Pu atom ratio in seawater and bottom sediment to identify the origins of Pu isotopes. The concentration of ^239+240Pu was almost uniform in surface water, decreasing slowly over time. Conversely, the ^239+240Pu concentration varied markedly in the bottom water and was dependent upon the sampling point, with higher concentrations of ^239+240Pu observed in the bottom water sample at sampling points having greater depth. The ²⁴⁰Pu/²³⁹Pu atom ratio in the seawater and sediment samples was higher than that of global fallout Pu, and comparable with the data in the other sea area around Japan which has likely been affected by close-in fallout Pu originating from the Pacific Proving Grounds. The ²⁴⁰Pu/²³⁹Pu atom ratio in bottom sediment samples decreased with sea depth. The land-originated Pu is not considered as the reason of the increasing ^239+240Pu concentration and also decreasing the ²⁴⁰Pu/²³⁹Pu atom ratio with sea depth, and further study is required to clarify it.     

Bioaccumulation and lack of oxidative stress response in the ragworm H. diversicolor following exposure to Ra in sediment

The main effluent from oil and gas production, produced water, from some platforms in the North Sea contains elevated concentrations of ²²⁶Ra. The aim of this study was to investigate whether ²²⁶Ra in sediment would accumulate in and affect sediment-dwelling organisms. In addition, we wanted to determine if the bioavailability would be modulated by the presence of a scale inhibitor which is used during oil and gas production. Hediste diversicolor was therefore exposed to different levels of ²²⁶Ra (30–6600 Bq kg⁻¹) in combination with scale inhibitor in the sediments in a flow through system. The levels of radioactivity in the exposures were close to levels that can be measured in proximity to oil/gas production facilities. ²²⁶Ra spiked to natural sediment partitioned into pore water and accumulated in the sediment-dwelling polychaete following a four-week exposure period. The results suggest that ²²⁶Ra did not bind strongly to sediment (low sediment:water partitioning coefficient), but it was not shown to bioaccumulate in any great extent (bioaccumulation factors of 0.019–0.022). Exposure of H. diversicolor in sediments with up to 6600 Bq kg⁻¹²²⁶Ra had no measurable effect on the total oxyradical scavenging capacity of the organisms compared to control. So although they accumulated the alpha-emitter, the treatments did not appear to cause oxidative stress in polychaete tissues.     

Transport and distribution of artificial gamma-emitting radionuclides in the River Yenisei and its sediment

Discharges from the Krasnoyarsk Mining and Chemical Industrial Complex (KMCIC) near Krasnoyarsk resulted in radioactive contamination of sediments of the River Yenisei. Between 1999 and 2006, 16 sediment cores were collected at different positions 15-1500 km downstream from the discharge point. The concentration of artificial gamma-emitting radionuclides (¹³⁷Cs, ⁶⁰Co, ¹⁵²Eu, and ²⁴¹Am) was determined with the objective to analyze the migration processes leading to the transport of these radionuclides along the river and to their vertical distribution within the sediment. In cores taken in the vicinity of the reactors, the average activity concentration of ¹³⁷Cs, ¹⁵²Eu, and ⁶⁰Co was about 1000 Bq kg⁻¹, and the activity concentration of ²⁴¹Am was about 20 Bq kg⁻¹. Contamination levels of artificial radionuclides were decreasing with increasing distance downstream the KMCIC: The fastest decrease of average activity by a factor of 10 over a distance of 300 km was observed for ²⁴¹Am, whereas for ¹³⁷Cs this decrease occurred over a distance of 1100 km. Sequential extraction experiments revealed that in all depths and at all distances the studied radionuclides were tightly bound to the sediment.To investigate the mechanisms of transport of the ¹³⁷Cs and ⁶⁰Co contamination, mathematical models have been used to describe the contamination in the river water and within the sediments.     

Dependence of dose loads on bone surfaces of murine rodents on the level of 90Sr accumulation in the skeleton

The relationship between ⁹⁰Sr accumulation in the skeleton after single injection and the resulting dose load on bone surfaces was studied in laboratory mice. Radiation doses were measured by a thermoluminescent method. A positive correlation was revealed between the surface dose rate on the skull and mandible and ⁹⁰Sr specific radioactivity in these bones. The possibility to calculate ⁹⁰Sr incorporation into the bone tissue from dosimetric data was evaluated as an analytical approach allowing preservation of the bone material for subsequent studies. Conversion coefficients relating surface doses to ⁹⁰Sr specific radioactivity in bones were calculated. However, their values have to be specifically defined for cases of chronic ⁹⁰Sr input and with regard to bone anatomy and species-specific and ecological features of test animals.     

Determination of radionuclide levels in rainwater using ion exchange resin and γ-spectrometry

The evaluation of radioactivity accidentally released into the atmosphere involves determining the radioactivity levels of rainwater samples. Rainwater scavenges atmospheric airborne radioactivity in such a way that surface contamination can be deduced from rainfall rate and rainwater radioactivity content. For this purpose, rainwater is usually collected in large surface collectors and then measured by γ-spectrometry after such treatments as evaporation or iron hydroxide precipitation. We found that collectors can be adapted to accept large surface (diameter 47 mm) cartridges containing a strongly acidic resin (Dowex AG 88) which is able to quantitatively extract radioactivity from rainwater, even during heavy rainfall. The resin can then be measured by γ-spectrometry. The detection limit is 0.1 Bq per sample of resin (80 g) for ¹³⁷Cs. Natural ⁷Be and ²¹⁰Pb can also be measured and the activity ratio of both radionuclides is comparable with those obtained through iron hydroxide precipitation and air filter measurements. Occasionally ²²Na has also been measured above the detection limit. A comparison between the evaporation method and the resin method demonstrated that 2/3 of ⁷Be can be lost during the evaporation process. The resin method is simple and highly efficient at extracting radioactivity. Because of these great advantages, we anticipate it could replace former rainwater determination methods. Moreover, it does not necessitate the transportation of large rainwater volumes to the laboratory.     

Partition of iodine (¹²⁹I and ¹²⁷I) isotopes in soils and marine sediments

Natural organic matter, such as humic and fulvic acids and humin, plays a key role in determining the fate and mobility of radioiodine in soil and sediments. The radioisotope ¹²⁹I is continuously produced and released from nuclear fuel reprocessing plants, and as a biophilic element, its environmental mobility is strongly linked to organic matter.Due to its long half-life (15.7 million years), ¹²⁹I builds up in the environment and can be traced since the beginning of the nuclear era in reservoirs such as soils and marine sediments. Nevertheless, partition of the isotope between the different types of organic matter in soil and sediment is rarely explored. Here we present a sequential extraction of ¹²⁹I and ¹²⁷I chemical forms encountered in a Danish soil, a soil reference material (IAEA-375), an anoxic marine sediment from Southern Norway and an oxic sediment from the Barents Sea. The different forms of iodine are related to water soluble, exchangeable, carbonates, oxides as well as iodine bound to humic acid, fulvic acid and to humin and minerals. This is the first study to identify ¹²⁹I in humic and fulvic acid and humin. The results show that 30-56% of the total ¹²⁷I and 42-60% of the total ¹²⁹I are associated with organic matter in soil and sediment samples. At a soil/sediment pH below 5.0-5.5, ¹²⁷I and ¹²⁹I in the organic fraction associate primarily with the humic acid while at soil/sediment pH > 6 ¹²⁹I was mostly found to be bound to fulvic acid. Anoxic conditions seem to increase the mobility and availability of iodine compared to oxic, while subaerial conditions (soils) reduces the availability of water soluble fraction compared to subaqueous (marine) conditions.     

Perfluoroalkyl substances and extractable organic fluorine in surface sediments and cores from Lake Ontario

Fourteen perfluoroalkyl substances (PFASs) including short-chain perfluorocarboxylates (PFCAs, C4–C6) and perfluoroalkane sulfonates (PFSAs, C4 and C6) were measured in surface sediment samples from 26 stations collected in 2008 and sediment core samples from three stations (Niagara, Mississauga, and Rochester basins) collected in 2006 in Lake Ontario. Perfluorooctanesulfonate (PFOS), perfluorooctanoate (PFOA), perfluorononanoate (PFNA), perfluorodecanoate (PFDA), and perfluoroundecanoate (PFUnDA) were detected in all 26 surface sediment samples, whereas perfluorohexane sulfonate (PFHxS), perfluorooctane sulfonamide (FOSA), perfluorododecanoate (PFDoDA) and perfluorobutanoate (PFBA) were detected in over 70% of the surface sediment samples. PFOS was detected in all of the sediment core samples (range: 0.492–30.1 ng g^− 1 d.w.) over the period 1952–2005. The C8 to C11 PFCAs, FOSA, and PFBA increased in early 1970s. An overall increasing trend in sediment PFAS concentrations/fluxes from older to more recently deposited sediments was evident in the three sediment cores. The known PFCAs and PFSAs accounted for 2–44% of the anionic fraction of the extractable organic fluorine in surface sediment, suggesting that a large proportion of fluorine in this fraction remained unknown. Sediment core samples collected from Niagara basin showed an increase in unidentified organic fluorine in recent years (1995–2006). These results suggest that the use and manufacture of fluorinated organic compounds other than known PFCAs and PFSAs has diversified and increased.