127I and 129I species in the English Channel and its adjacent areas: Uncovering impact on the isotopes marine pathways.

Radioactive iodine-129 has been released from the La Hague nuclear fuel reprocessing facility (NRF) into the English Channel, but the distribution and transformation of the isotope species, and environmental consequences have not been fully characterized in the Channel. Here we present data on iodine isotopes (129I and 127I) species in surface water of the English Channel and the southern Celtic Sea. Compared to 127I species, the concentrations of 129I- and 129IO3- show more variations, but iodate is the major species for both 129I and 127I. Our data provide new information regarding iodide-iodate inter-conversion showing that water dilution and mixing are the main factors affecting the 127I and 129I species distribution in the Channel. Some reduction of iodate occurs within the English Channel and mainly in the west part because of biotic processes. The 129I species transformation is overall insignificant, especially in the eastern Channel, where a constant value of 129IO3-/129I is observed, which might characterize the La Hague wastewater signal. In the Celtic Sea, oxidation of iodide can be traced by 127I and 129I species. On a larger scale, 129I generally experienced an oxidation process in the Atlantic Ocean, while in the coast of shallow shelf seas, new produced 129I- can be identified, especially in the German Bight and the Baltic Sea. The data of 129I species in the English Channel can provide estimate of redox rates in a much broader marine areas if the transit time of 129I from La Hague is well-defined. Furthermore, estimate of inventories for 129I and its species in the Channel, and fluxes of 129I species from the English Channel to the North Sea add important information to the geochemical cycle of 129I.

Construction and Preclinical Evaluation of a 124/131I-Labeled Radiotracer for the Detection of Mesothelin-Overexpressing Cancer.

Mesothelin is a molecular biomarker of many types of solid cancers, which may represent a highly promising new target in the development of cancer-targeted diagnostic agents. A human anti-mesothelin antibody with a low molecular weight, ET210sc, was applied; this antibody has potent affinity and can penetrate tissue quickly and stably without causing immunoreactions. We developed a new 124/131I-labeled radiotracer of ET210sc. The 124/131I-labeled ET210sc radiotracer showed excellent radiochemical quality (with over 99% radiolabeling yield, 0.07 GBq/µmol specific activity) and remarkable stability in phosphate-buffered saline (>95% at 3 days). The radiotracer retained its potent affinity (dissociation constant, Kd = 0.101 nM). The radiotracer specifically bound to mesothelin-positive cells in vitro. Interestingly, the radiotracer exhibited significant positive-to-negative tumor uptake ratios (1.5:1) 3 days postinjection. The estimated absorbed doses of each organ (e.g., 0.704 mGy/MBq for the rectum; 0.341 mGy/MBq for the spleen) met the medical safety standards for further clinical applications. Our findings provide an initial proof of concept for the potential use of 124/131I-labeled ET210sc radiotracers to detect mesothelin-overexpressing cancer. 124I-ET210sc is proposed to be an ideal imaging agent for further clinical applications.

Iodine isotopes (129I and 127I) in the hydrosphere of Qinghai-Tibet region and South China Sea.

The radioactive isotope 129I, with a half-life of 1.57 × 107 years, is widely used as a tracer to assess nuclear safety, to track environmental and geological events and to figure out the details of the stable iodine geochemical cycle. This work investigated the 129I and 127I distribution in water samples collected from the terrestrial (rivers, lakes and springs) and marine water systems (estuary and sea) in China. The measured 129I concentrations of (1-51) × 106 atoms/L and 129I/127I ratios of (0.03-21) × 10-10 shows the variability of 129I level in the water systems. The local permafrost and seasonal frozen environment play a key role in groundwater recharge in the Qinghai-Tibet region, which is reflected in the 129I distribution in surface water. The depth distribution of 129I in the water column of the South China Sea reflects the effluence of different currents. The results also indicate that the hydrosphere of China contains one to three orders of magnitude less 129I compared to those reported in Europe. Despite the large distance, the European nuclear fuel reprocessing facilities represent the major source of 129I in the hydrosphere of China through atmospheric transport. The contribution of the Fukushima nuclear accident to 129I levels in the hydrosphere of China was negligible.

Iodine in Swiss milk depending on production (conventional versus organic) and on processing (raw versus UHT) and the contribution of milk to the human iodine supply.

The iodine content in milk depends on various factors, including the season, production system, and location of milk production. The aim of this study was 1) to obtain data on the iodine concentration of conventional and organically produced milk and according to seasons; 2) to compare these actual data with previous measurement data; 3) to study the influence of UHT treatment on the iodine content and 4) to estimate the contribution of organic and conventional milk to the consumer's iodine intake. A total of 110 samples of conventional and organic ultra-heat treated (UHT) whole milk were collected in the period between 1 May 2013 and 30 April 2014 from two large-scale companies, processing milk from two regions in Switzerland. The iodine concentration in organic milk (average 71 ±â€¯25 µg/l) was significantly lower than in conventional milk (average 111 ±â€¯26 µg/l) and varied between suppliers. Milk iodine concentration varied according to the month of collection in organic and conventionally produced milk, with lowest values between August and October (organic milk 42 µg/l; conventional milk 75 µg/l) and highest values in January (organic milk 99 µg/l; conventional milk 145 µg/l). Heat treatment did not influence iodine concentration. Since milk and dairy products are significant source of food-related iodine intake in Switzerland, consumers who prefer organic milk and dairy products are likely to have an inferior iodine status.

Stimulated thyroglobulin values above 5.6 ng/ml before radioactive iodine ablation treatment following levothyroxine withdrawal is associated with a 2.38-fold risk of relapse in Tg-ab negative subjects with differentiated thyroid cancer

Background. Serum thyroglobulin (Tg) is the key parameter used in the follow-up of subjects with differentiated thyroid cancer (DTC). Current guidelines advise its measurement to take place when Thyrotropin (TSH) levels are >30 µU/ml (stimulated Tg) and when TSH < 0.1 µU/ml (suppressed Tg). Although stimulated Tg levels <1 ng/ml have been shown to display excellent prognosis, relapses may occur despite low Tg levels. Recently, very low cut-off levels of stimulated Tg have been proposed for determining the recurrence risk in these subjects. In this study, we aimed to assess the association between ablative stimulated Tg obtained before radioactive iodine ablation therapy (RAI) (ASTg) and late stimulated Tg obtained 6-12 months after primary therapy (LSTg) in a group of subjects with DTC. We also aimed to establish a cut-off level of Tg for recurrence. Methods. We retrospectively analyzed 393 subjects with low or intermediate risk DTC diagnosed at our institution between January 2000 and December 2010 with a mean follow-up period of 64.4 months (range 14-192 months). All stimulated Tg levels were performed following levothyroxine withdrawal in this study. Results. Histopathological analysis indicated papillary carcinoma in 362 (92.1%) subjects and follicular carcinoma in 31 (7.9%) subjects. Three hundred and twenty-four (82.4%) of our cases were females, and 69 (17.6%) were males. Recurrence occurred in 82 (20.9%) of the subjects. Relapse was significantly more frequently observed in subjects with ASTg ≥ 2 ng/ml; and LSTg ≥ 2 ng/ml. (p = 0.004 and p < 0.001, respectively). In subjects negative for thyroglobulin antibodies (Tg-ab), an ASTg value ≥5.6 ng/ml was established to increase the risk of recurrence by 2.38-fold (p = 0.002), whereas an LSTg ≥ 0.285 ng/ml increased the risk of relapse by 3.087-fold (p < 0.001). Conclusion. As a result of this study, we determined that the optimum cut-off level for both ASTg and LSTg may be lower than those previously reported. Using such a lower cut-off may improve sensitivity for detecting relapse (AU)

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Iodine isotopes in precipitation: Four-year time series variations before and after 2011 Fukushima nuclear accident.

Rainwater samples were collected monthly from Fukushima, Japan, in 2012-2014 and analysed for (127)I and (129)I. These are combined with previously reported data to investigate atmospheric levels and behaviour of Fukushima-derived (129)I before and after the 2011 nuclear accident. In the new datasets, (127)I and (129)I concentrations between October 2012 and October 2014 varied from 0.5 to 10 µg/L and from 1.2 × 10(8) to 6.9 × 10(9) atoms/L respectively, resulting in (129)I/(127)I atomic ratio ranges from 3 × 10(-8) to 2 × 10(-7). The (127)I concentrations were in good agreement with those in the previous period from March 2011 to September 2012, whereas the (129)I concentrations and (129)I/(127)I ratios followed declining trends since the accident. Although (129)I concentrations in five samples during the period of 2013-2014 have approached the pre-accident levels, (129)I concentrations in most samples remained higher values in winter and spring-summer. The high (129)I levels in winter and spring-summer are most likely attributed to local resuspension of the Fukushima-derived radionuclide-bearing fine soil particles deposited on land surfaces, and re-emission through vegetation taking up (129)I from contaminated soil and water, respectively. Long-term declining rate suggests that contribution of the Fukushima-derived (129)I to the atmosphere would become less since 2014.

Concentrations of iodine isotopes ((129)I and (127)I) and their isotopic ratios in aerosol samples from Northern Germany.

New data about (129)I, (127)I concentrations and their isotopic ratios in aerosol samples from the trace survey station of the Physikalisch-Technische Bundesanstalt (PTB) in Braunschweig, Northern Germany, are presented and discussed in this paper. The investigated samples were collected on a weekly basis during the years 2011 to 2013. Iodine was extracted from aerosol filters using a strong basic solution and was separated from the matrix elements with chloroform and was analysed by accelerator mass spectrometry (AMS) for (129)I and by inductively coupled plasma mass spectrometry (ICP-MS) for (127)I. The concentrations of (127)I and (129)I in aerosol filters ranged from 0.31 to 3.71 ng m(-3) and from 0.06 to 0.75 fg m(-3), respectively. The results of (129)I/(127)I isotopic ratios were in the order 10(-8) to 10(-7). The (129)I originated directly from gaseous emissions and indirectly from liquid emissions (via sea spray) from the reprocessing plants in Sellafield and La Hague. In comparison with the results of (131)I after the Fukushima accident, no contribution of (129)I from this accident was detectable in Central Europe due to the high background originating from the (129)I releases of the European reprocessing plants. (129)I atmospheric activity concentrations were compared with those of an anthropogenic radionuclide ((85)Kr). We did not find any correlation between (129)I and (85)Kr, both having nuclear reprocessing plant as the main source.

Temporal variation of iodine concentration and speciation (127I and 129I) in wetland groundwater from the Savannah River Site, USA.

(129)I derived from a former radionuclide disposal basin located on the Savannah River Site (SRS) has concentrated in a wetland 600 m downstream. To evaluate temporal environmental influences on iodine speciation and mobility in this subtropical wetland environment, groundwater was collected over a three-year period (2010-2012) from a single location. Total (127)I and (129)I showed significant temporal variations, ranging from 68-196 nM for (127)I and <5-133 pCi/L for (129)I. These iodine isotopes were significantly correlated with groundwater acidity and nitrate, two parameters elevated within the contaminant plume. Additionally, (129)I levels were significantly correlated with those of (127)I, suggesting that biogeochemical controls on (127)I and (129)I are similar within the SRS aquifer/wetland system. Iodine speciation demonstrates temporal variations as well, reflecting effects from surface recharges followed by acidification of groundwater and subsequent formation of anaerobic conditions. Our results reveal a complex system where few single ancillary parameters changed in a systematic manner with iodine speciation. Instead, changes in groundwater chemistry and microbial activity, driven by surface hydrological events, interact to control iodine speciation and mobility. Future radiological risk models should consider the flux of (129)I in response to temporal changes in wetland hydrologic and chemical conditions.

Speciation of iodine isotopes inside and outside of a contaminant plume at the Savannah River Site.

A primary obstacle in understanding the fate and transport of the toxic radionuclide (129)I (a thyroid seeker) is an accurate method to distinguish it from the stable isotope, (127)I, and to quantify the various species at environmentally relevant concentrations (~10(-8) M). A pH-dependent solvent extraction and combustion method was paired with accelerator mass spectrometry (AMS) to measure ambient levels of (129)I/(127)I isotope ratios and iodine speciation (iodide (I(-)), iodate (IO3(-)), and organo-I (OI)) in aquatic systems. The method exhibited an overall uncertainty of 10% or less for I(-) and IO3(-), and less than 30% for OI species concentrations and enabled (129)I measurements as low as 0.001 Bq/L (1 Bq/L=10(-13) M). The method was used to analyze groundwater from the Savannah River Site (SRS), South Carolina, USA, along a pH, redox potential (Eh), and organic carbon gradient (8-60 µM DOC). The data confirmed that the (129)I/(127)I ratios and species distribution were strongly pH dependent and varied in a systematic manner from the strongly acidic source. While (129)I speciation in plume samples containing total I concentrations >1.7 Bq/L was similar whether measured by AMS or GC-MS ([I(-)]≫[IO3(-)]=[OI]), AMS enabled (129)I speciation measurements at much lower concentrations than what was possible with GC-MS. AMS analyses demonstrated that groundwater samples minimally impacted by the plume were still orders of magnitude higher than ambient (129)I concentrations typically found elsewhere in the USA groundwaters and rivers. This is likely due to past atmospheric releases of volatile (129)I species by SRS nuclear reprocessing facilities near the study site. Furthermore, the results confirmed the existence of (129)I not only as I(-), but also as OI and IO3(-) species.

Temporal variation of iodine isotopes in the North Sea.

Monitoring temporal variability of (129)I in the North Sea, a relatively large reservoir of radioactive discharges from the nuclear fuel reprocessing facilities, is vital for the environmental situation in the region. New information on concentration levels and distribution of (129)I and (127)I and their species forms (iodide and iodate) are gained here through sampling of surface water in 2010. The results show generally large spatial and temporal (compared to data from 2005) fluctuations of total (129)I and (127)I, and iodide and iodate. In samples south of 53°N, the level of (127)I(-) in 2010 was generally comparable or higher than in 2005. The results also show total (129)I concentrations comparable in the south, but 2-8 times lower in the north, to the analyses made in 2005. Different from total (129)I, the (129)I(-)/(129)IO3(-) values in the northern part were 2 times higher in 2010 than values observed in 2005. These variations in total (129)I and (127)I and their species are related to coastal water offshore propagation and surface currents that are linked to long-term and seasonal climatic changes over the North Atlantic and North Sea. Inventory estimation shows that >90% of (129)I resides in the Southern and German Bights, which also suggests negligible contribution from the Sellafield facility discharges when compared with that from the La Hague. Variability in discharge rate from La Hague may also affect the distribution patterns of (129)I in the North Sea on the monthly scale.

Iodine isotopes (127I and 129I) in aerosols at high altitude Alp stations.

Concentrations of gases and particulate matter have been proven to be affected by meteorological and geographical variables from urban locations to high mountain clean air sites. Following our previous research in Vienna, we summarize here new findings about concentration levels of iodine isotopes in aerosols collected at two Alpine meteorological stations, Sonnblick (Austria) and Zugspitze (Germany) during 2001. The present study mainly focuses on the effect of altitude on the anthropogenic concentration of (129)I and on the isotopic ratio (129)I/(127)I. Iodine was separated from matrix elements by using either an anion exchange method or solvent extraction, and was analyzed by ICP-MS and AMS. Over the altitude change from Vienna to Zugspitze and Sonnblick (202 m to 2962 m and 3106 m above sea level), stable iodine level decreased from an average of 0.94 ng m(-3) to 0.52 ng m(-3) and 0.62 ng m(-3), respectively. Similarly, (129)I concentrations at both Alpine stations were about 1 order of magnitude lower (10(4) atoms m(-3)) than values obtained for Vienna (10(5) atoms m(-3)) and reveal a strong vertical concentration gradient of (129)I. A high degree of variability is observed, which is due to wide variation in the origin of air masses. Furthermore, air trajectory analysis demonstrates the importance of large scale air transport mostly from southeast Europe for influencing Sonnblick whereas influence from northwest Europe is strong at Zugspitze. In contrast to (129)I, a higher concentration of (7)Be was found at higher altitude stations compared to Vienna which probably results from its production in the upper atmosphere.

Iodide and iodate (129I and 127I) in surface water of the Baltic Sea, Kattegat and Skagerrak.

Despite the common incorporation of iodine in the biological cycle and occurrence of huge contamination of the radioactive isotope (129)I in the Baltic Proper, Skagerrak and Kattegat, there is no data on chemical speciation of iodine in these waters. We here present first time data on iodine isotopes (129)I and (127)I species as iodide and iodate in surface seawater samples collected from 16 locations in August 2006 and 19 locations in April 2007 in the Baltic Proper, Skagerrak and Kattegat. After extensive separation methods, the isotopes concentrations were determined using accelerator mass spectrometry (AMS) technique for the (129)I and inductively coupled plasma mass spectroscopy (ICP-MS) for (127)I. High concentrations of both isotopes species were found in the Skagerrak-Kattegat basins, whereas the values in the Baltic Proper are low for both species. The ratios of (129)I(-)/(129)IO(3)(-) and (127)I(-)/(127)IO(3)(-) significantly increase from south to central Baltic Sea, and iodide (both isotopes) appears as the predominant inorganic iodine species along the Baltic Sea. The results show insignificant change in (129)I and (127)I speciation and suggest that reduction of iodate and oxidation of iodide in Skagerrak and Kattegat may be a slow process. Additionally, the positive correlation between salinity and iodide and iodate (both isotopes) may reflect effective control of Skagerrak water mass on iodine distribution in surface water of the Baltic Sea.

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.

Factors controlling mobility of 127I and 129I species in an acidic groundwater plume at the Savannah River Site.

In order to quantify changes in iodine speciation and to assess factors controlling the distribution and mobility of iodine at an iodine-129 ((129)I) contaminated site located at the U.S. Department of Energy's Savannah River Site (SRS), spatial distributions and transformation of (129)I and stable iodine ((127)I) species in groundwater were investigated along a gradient in redox potential (654 to 360 mV), organic carbon concentration (5 to 60 µmol L(-1)), and pH (pH 3.2 to 6.8). Total (129)I concentration in groundwater was 8.6±2.8 Bq L(-1) immediately downstream of a former waste seepage basin (well FSB-95DR), and decreased with distance from the seepage basin. (127)I concentration decreased similarly to that of (129)I. Elevated concentrations of (127)I or (129)I were not detected in groundwater collected from wells located outside of the mixed waste plume of this area. At FSB-95DR, the majority (55-86%) of iodine existed as iodide for both (127)I and (129)I. Then, as the iodide move down gradient, some of it transformed into iodate and organo-iodine. Considering that iodate has a higher K(d) value than iodide, we hypothesize that the production of iodate in groundwater resulted in the removal of iodine from the groundwater and consequently decreased concentrations of (127)I and (129)I in downstream areas. Significant amounts of organo-iodine species (30-82% of the total iodine) were also observed at upstream wells, including those outside the mixed waste plume. Concentrations of groundwater iodide decreased at a faster rate than organo-iodine along the transect from the seepage basin. We concluded that removal of iodine from the groundwater through the formation of high molecular weight organo-iodine species is complicated by the release of other more mobile organo-iodine species in the groundwater.

Iodine isotopes (129I and 127I) in the Baltic Proper, Kattegat, and Skagerrak basins.

Radioactive anthropogenic pollution has raised concerns about the present and future environmental status of the semienclosed Baltic Sea. We here study the distribution and inventory of the anthropogenic radioactive (129)I in water depth profiles collected from 16 sites in August 2006 and 19 sites in April 2007 in the Baltic Proper and related Kattegat and Skagerrak basins. The results reveal considerable differences of (129)I concentration in terms of spatial and temporal variability and expose relatively high concentrations in the deep waters. Variability in the concentration of (127)I, stable natural isotope of iodine, seems to follow changes in the seawater salinity, but in oxygen-poor bottom waters sediment diagenetic release may contribute to the concentration of both isotopes in the water body. Inventory estimates show that (129)I in August 2006 (24.2 ± 15.4 kg) is higher than that in April 2007 (14.4 ± 8.3 kg) within the southern and central Baltic Proper whereas almost a constant load occurs in the Kattegat Basin. Calculated model inventory shows correspondence to empirical data and provides a guideline for future environmental assessment on the impact of (129)I load in the studied region.

A novel approach for the simultaneous determination of iodide, iodate and organo-iodide for 127I and 129I in environmental samples using gas chromatography-mass spectrometry.

In aquatic environments, iodine mainly exists as iodide, iodate, and organic iodine. The high mobility of iodine in aquatic systems has led to (129)I contamination problems at sites where nuclear fuel has been reprocessed, such as the F-area of Savannah River Site. In order to assess the distribution of (129)I and stable (127)I in environmental systems, a sensitive and rapid method was developed which enables determination of isotopic ratios of speciated iodine. Iodide concentrations were quantified using gas chromatography-mass spectrometry (GC-MS) after derivatization to 4-iodo-N,N-dimethylaniline. Iodate concentrations were quantified by measuring the difference of iodide concentrations in the solution before and after reduction by Na(2)S(2)O(5). Total iodine, including inorganic and organic iodine, was determined after conversion to iodate by combustion at 900 °C. Organo-iodine was calculated as the difference between the total iodine and total inorganic iodine (iodide and iodate). The detection limits of iodide-127 and iodate-127 were 0.34 nM and 1.11 nM, respectively, whereas the detection limits for both iodide-129 and iodate-129 was 0.08 nM (i.e., 2pCi (129)I/L). This method was successfully applied to water samples from the contaminated Savannah River Site, South Carolina, and more pristine Galveston Bay, Texas.

MD-354 selectively antagonizes the antinociceptive effects of (-)nicotine in the mouse tail-flick assay.

RATIONALE: (-)Nicotine produces antinociceptive effects in rodents. meta-Chlorophenylguanidine (MD-354), an analgesia-enhancing agent, binds at 5-HT(3) and alpha(2)-adrenoceptors and potentiates the antinociceptive effects of an "inactive" dose of clonidine. The present study examined the actions of MD-354 on (-)nicotine-induced antinociception. MATERIALS AND METHODS: Mouse tail-flick and other assays were employed. RESULTS: In the tail-flick assay, (-)nicotine (ED(50) = 1.66 mg/kg) but not MD-354 produced dose-related antinociceptive effects. Administered in combination with (-)nicotine (2.5 mg/kg), MD-354 (AD(50) = 3.4 mg/kg) did not potentiate, but effectively antagonized the antinociceptive actions of (-)nicotine. In a mouse hot-plate assay, MD-354 failed to modify (-)nicotine responses. In combination with a locomotor activity-suppressing dose of (-)nicotine, MD-354 (up to 17 mg/kg) failed to antagonize (-)nicotine-induced hypolocomotion. In a rat drug discrimination paradigm using (-)nicotine as training drug, MD-354 produced saline-appropriate responding; in combination with the training dose of (-)nicotine, MD-354 failed to antagonize the nicotine cue. CONCLUSIONS: MD-354 selectively antagonizes the antinociceptive actions of (-)nicotine in the tail-flick, but not in the hot-plate assay, or either the motor effects, or discriminative stimulus effects of (-)nicotine. The most parsimonious explanation is that MD-354 might act as a negative allosteric modulator of alpha 7 nACh receptors, and radioligand binding and functional data are provided to support this conclusion.

Time series of 129I and 127I speciation in precipitation from Denmark.

Environmental 129I mainly released from reprocessing plants at La Hague (France) and Sellafield (U.K.) provides a unique atmospheric and environmental tracer. This study deals with 129I and 127I speciation in precipitation collected in Denmarkduring 2001-2006 that indicates many newfindings. The concentrations of total 129I in precipitation vary from 0.28 to 5.63 x 10(9) atoms 129I L(-1) with an average of (2.34 +/- 1.43) x 10(9) atoms 129I L(-1), and the annual deposition flux of 129I is (1.25 +/- 0.30) x 10(12) atoms m(-2). Increased 129I levels in precipitation and 129I/ 127I ratio are attributed to the releases of 129I from the reprocessing plants at La Hague and Sellafield. Iodide is the major specie of 129I, which accounts for 50-99% of total 129I. The concentrations of total 127I vary from 0.78 to 2.70 microg iodine L(-1) with an average of 1.63 +/- 0.47 microg iodine L(-1), and annual deposition flux of 0.95 +/- 0.26 mg m(-2). Unlike 129I, iodate is the major specie of 127I, which accounts for 43-93% of total 127I. The 291I/ l27I atomic ratios for total iodine vary from 5.04 to 76.5 x 10(-8) with an average of (30.1 +/- 16.8) x 10(-8). These values are 10 times lower for iodate with an average of (2.95 +/- 3.13) x 10(-8). Seasonal variations of 129I/127 ml values and 129I concentrations are associated with highs in spring and lows in summer-autumn periods. Re-emission of 129 from the surface water of the English Channel, Irish Sea, North Sea, and Norwegian Sea, especially from the European continental coast areas, is evidently the major source of 129I in the precipitation, while stable 127I in the precipitation has multiple sources, i.e., marine, as well as terrestrial emission. This work shows that data on speciation of iodine isotopes can provide thorough indications about the sources and geochemical cycle despite the complicated atmospheric chemistry of iodine.

Determination of (129)I and (127)I concentration in soil samples from the Chernobyl 30-km zone by AMS and ICP-MS.

A large amount of radioiodine isotopes (mainly (131)I, t(1/2) = 8 days) was released from the accident at Chernobyl Nuclear Power Plant (CNPP) in April-May 1986. An increase in childhood-thyroid cancer in the contaminated areas in Belarus, Russia and the Ukraine was demonstrated to be caused by radioiodine released at the time of the accident. However, there is a lack of quantitative data on the (131)I levels in the local environment (e.g. air, plant, soil). At this point, a long-lived iodine isotope, (129)I (t(1/2) = 15.7 million years), also released with a certain ratio to (131)I from CNPP, could be used for estimating the (131)I levels in the environment. In this paper we present analytical results of the (129)I concentrations and (129)I/(127)I atom ratios in soil samples collected from the CNPP exclusion zone (30-km zone), with the aim of assessing current contamination levels and distribution patterns. For the analysis of the iodine fraction in the investigated soil samples, the pyrohydrolysis method was utilized for separation of (127)I and (129)I nuclides, and subsequently their concentration was determined using inductively coupled plasma mass spectrometry (ICP-MS) and accelerator mass spectrometry (AMS), respectively. The concentration of (129)I and the (129)I/(127)I atom ratio in the surface soil samples in the 30 km-zone of CNPP ranged from 4.6 to 170 mBq/kg, and from 1.4 x 10(-6) to 13 x 10(-6), respectively. These values are significantly higher than those from global (129)I fallout, indicating that most of the measured (129)I was due to the deposition of the accident. Stable iodine concentrations in this area were found to be very low (below 1 ppm) for most of the samples, suggesting the environmental iodine levels in this area to be potentially low. The (129)I/(137)Cs activity ratio in surface and sub-surface soils was not so constant, i.e., in the range (7.3-20.2) x 10(-7). This might be due to the different behavior of deposition and/or migration of these nuclides in soil. These results suggest the obtained data of (129)I to be useful for the reconstruction of the (131)I deposition in the contaminated areas.

Subcellular imaging of RNA distribution and DNA replication in single mammalian cells with SIMS: the localization of heat shock induced RNA in relation to the distribution of intranuclear bound calcium.

The subcellular localization of RNA for understanding transcriptional activity by using RNA precursors, like 5-bromouridine (BrU), generally requires chemical fixation and staining of cells with monoclonal antibody for imaging BrU-containing RNA in individual cells. Although effective for RNA localization, the native chemical composition of diffusible ions and molecules is destroyed in this approach and one cannot study their spatial relationship with RNA localization sites in this sample type. This work presents a novel secondary ion mass spectrometry approach in cryogenically prepared cells, which allows the same cell imaging of RNA (and/or replicating DNA) distribution in relation to intracellular chemical composition. The heat shock treatment of HeLa cells was used as a model system because the transcription of heat shock genes is activated during heat shock while other transcriptional activities of the cell are suppressed. The HeLa cells were heat-shocked for 1 h at 42 degrees C in presence of 100 muM BrU and/or 100 microM IdU (5-iododeoxyuridine). Following the heat shock treatments, the cells were cryogenically prepared with our sandwich freeze-fracture method and freeze-dried prior to secondary ion mass spectrometry analysis. A CAMECA IMS 3f secondary ion mass spectrometry ion microscope (CAMECA, Paris, France) capable of producing elemental (isotopic) distributions with a spatial resolution of 500 nm was used in the study. Secondary ion mass spectrometry analysis of fractured freeze-dried HeLa cells revealed well-preserved intracellular (39)K and (23)Na concentrations in heat-shocked cells. Both DNA replication and RNA distribution (total RNA) were imaged directly in the same cell by secondary ion mass spectrometry imaging of masses (127)I (from IdU) and (81)Br (from BrU), respectively. Surprisingly, the nucleus of heat-shocked cells contained spatially resolved regions with elevated levels of bound calcium (approximately 0.75 mM total calcium instead of 0.50 mM total calcium in the nucleoplasm). These regions spatially correlated with depleted levels of BrU-RNA in (81)Br secondary ion mass spectrometry images. The remainder of intranuclear regions displayed the presence of BrU-RNA with heterogeneous distribution. These observations indicate that calcium in its bound form may play a fundamental role in processes such as transcription and/or processing and storage of RNA. The shape of intranuclear regions with elevated levels of bound calcium resembled the heat shock induced nuclear bodies in HeLa cells. The analysis of cryogenically prepared frozen freeze-dried cells provides an ideal sample type for further understanding of the role of bound calcium in transcription of genes under physiological and pathological conditions.