利用加速器质谱仪进行快速~(129)I检测的方法研究

加速器质谱法是~(129)I最灵敏的检测方法。传统方法分析样品时通常需要复杂的化学制样流程,对样品中碘元素进行分离、富集和纯化,测试周期较长,成本高。在核应急分析等类型的应用研究中,需要对大批量样品中的~(129)I含量开展快速检测,针对此类应用需求特点,本研究尝试开发一种快速、流程简便并且成本低廉的~(129)I-AMS检测方法。以三种已知~(129)I水平的国际标准物质作为研究样品,将干燥和研磨均匀化的样品粉末直接与加入过本底碘的电热导体介质(Nb粉末)混合后压入靶座,实现快速制靶,进行加速器质谱测量,再结合制靶时称量的相关质量关系数据就能直接计算得出原始样品中的~(129)I活度。通过对测量数据与已知值进行比较分析验证了方法的可靠性,估算方法的探测下限可达0.15μBq?g~(-1)。     

Influence of releases of I-129 from reprocessing plants on the marine environment of the North Adriatic Sea

Compared to the pre-nuclear era, large amounts of ¹²⁹I have been released to the marine environment, especially as liquid and gaseous discharges from two European reprocessing plants located at Sellafield and La Hague. Their liquid discharges influence Northern Europe and most research was conducted in the area of the North Atlantic Ocean and the Baltic Sea. In this article data on ¹²⁹I content and ¹²⁹I/¹²⁷I ratios observed in the North Adriatic Sea, which is a rather enclosed basin of the Mediterranean Sea, are presented. To the best of our knowledge no data on ¹²⁹I in the Mediterranean Sea have previously been reported. As this area is isolated from direct liquid discharges, the main transport pathway is probably gaseous releases from reprocessing plants. Surface sea water, the marine alga Fucus virsoides, an iodine accumulator, and the Mediterranean mussel Mytilus galloprovincialis collected in 2009 and 2010, and marine sediment collected in 2005 and 2009 were analysed. The ¹²⁹I/¹²⁷I isotopic ratios observed were in the range from 0.8 to 3.0 × 10⁻⁰⁸ for seawater, from 0.06 to 0.35 × 10⁻⁰⁸ for marine sediment, from 0.05 to 0.10 × 10⁻⁰⁸ for F. virsoides and from 0.3 to 0.9 × 10⁻⁰⁸ for M. galloprovincialis.     

Validation of I ecological transfer models and thyroid dose assessments using Chernobyl fallout data from the Plavsk district, Russia

Within the project “Environmental Modelling for Radiation Safety” (EMRAS) organized by the IAEA in 2003 experimental data of ¹³¹I measurements following the Chernobyl accident in the Plavsk district of Tula region, Russia were used to validate the calculations of some radioecological transfer models. Nine models participated in the inter-comparison. Levels of ¹³⁷Cs soil contamination in all the settlements and ¹³¹I/¹³⁷Cs isotopic ratios in the depositions in some locations were used as the main input information. 370 measurements of ¹³¹I content in thyroid of townspeople and villagers, and 90 measurements of ¹³¹I concentration in milk were used for validation of the model predictions.A remarkable improvement in models performance comparing with previous inter-comparison exercise was demonstrated. Predictions of the various models were within a factor of three relative to the observations, discrepancies between the estimates of average doses to thyroid produced by most participant not exceeded a factor of ten.     

Level and origin of 129I and 137Cs in lichen samples (Cladonia alpestris) in central Sweden

Lichen is a symbiosis between algae and fungi. They have for decades been used as bioindicators for atmospheric deposition of heavy metals, organic compounds and radioactive elements. Especially the species Cladonia alpestris and Cladonia rangiferina are important for the food chain lichen-reindeer-man.The concentration of ¹²⁹I was determined in lichen samples (Cladonia alpestris) contaminated by fallout from atmospheric nuclear tests explosions and the Chernobyl accident. The samples were collected at Lake Rogen District (62.3°N, 12.4°E) in central Sweden in the periods 1961-1975 and 1987-1998, and analysed with accelerator mass spectrometry (AMS) at CNA (Seville) to study its distribution in different layers. Data on the ¹³⁷Cs activity measured previously were also included in this study. The ¹²⁹I concentration ranged from (0.95 ± 0.13) × 10⁸ at g⁻¹ in 1961 in the uppermost layer to (14.2 ± 0.5) × 10⁸ at g⁻¹ in 1987 in deepest layer. The ¹²⁹I/¹³⁷Cs atom ratio ranged between 0.12 and 0.27 for lichen samples collected in the period 1961-1975, indicating weapons tests fallout. For lichen samples collected between 1987 and 1998 the behaviour of ¹³⁷Cs concentrations reflected Chernobyl fallout. The concentrations of the two radionuclides followed each other quite well in the profile, reflecting the same origin for both.From the point of view of the spatial distribution in the lichen, it appears that ¹²⁹I was predominantly accumulated in the lowest layer, the opposite to ¹³⁷Cs for which the highest amounts were detected systematically in the topmost layer of lichen. This vertical distribution is important for radioecology because lichen is the initial link in the food chain lichen-reindeer-man, and reindeer only graze the upper parts of lichen carpets.     

Radioiodine and radiocesium in Thessaloniki, Northern Greece due to the Fukushima nuclear accident

Radioiodine (¹³¹I) in air and rainwater as high as 497 μBq m⁻³ and 0.7 Bq L⁻¹, respectively, as well as ¹³⁷Cs and ¹³⁴Cs in air as high as 145 μBq m⁻³ and 126 μBq m⁻³, respectively were recorded in Thessaloniki, Northern Greece (40°38′N, 22°58′E) from March 24, 2011 through April 09, 2011, after a nuclear accident occurred at Fukushima, Japan (37°45′N, 140°28′E) on March 11, 2011.     

Can we remove iodine-131 from tap water in Japan by boiling? - Experimental testing in response to the Fukushima Daiichi Nuclear Power Plant accident

Iodine-131 concentrations in tap water higher than 100 Bq L⁻¹ were reported by several local governments in Japan following the Fukushima Daiichi Nuclear Power Plant accident. Some individuals in the emergency-response community recommended the boiling of tap water to remove iodine-131. However, the tap water boiling tests in this study showed no iodine-131 loss from the tap water with either short-term boiling (1-10 min) or prolonged boiling (up to 30 min) resulting in up to 3-fold volume reductions. In this situation, boiling was shown to be not effective in removing iodine-131 from tap water; indeed even higher concentrations may result from the liquid-volume reduction accompanying this process.     

大气129I水平对超低129I含量地质样品分析中流程空白的影响

为了采用¹²⁹I进行地质定年研究,该类样品中的¹²⁹I/¹²⁷I原子比值通常低于10^-12,因此低的¹²⁹I流程空白是分析地质定年样品的前提条件之一。在全球范围内,大气中129I的水平呈现显著变化趋势,¹²⁹I/¹²⁷I原子比值范围在10^-10 到10^-6。然而,在样品制备过程中,是否大气中的¹²⁹I会影响流程空白尚未可知。本研究调查了三种常用的¹²⁹I分析方法,包括直接沉淀法、溶剂萃取法和管式燃烧法（分别以压缩空气和氧气作为载气）来比较流程空白中的¹²⁹I/¹²⁷I比值。研究结果表明：在最佳实验室条件下,流程空白均被控制在较低的水平,可用于分析各种环境和地质样品。另外,通过研究溶液的长时间储存,发现当0.4 mol???L^-1NaOH溶液储存一年以上时,¹²⁹I?/?¹²⁷I比值比新配制的NaOH溶液有所提高,但基本在实验室正常本底2×10^-13以内。采用压缩空气作为载气的管式燃烧法比氧气为载气时具有明显提高的¹²⁹I?/?³I比值。研究表明样品和试剂的储存,以及制样过程中与大气的交换程度均会影响流程空白中¹²⁹I的水平。因此在分析超低¹²⁹I含量的地质样品时,固体样品中碘的分离应采用低本底的分析方法（如以纯气体作为载体的管式燃烧法）,如有必要还可在低大气¹²⁹I水平的实验室进行实验。     

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.     

Measured elemental transfer factors for boreal hunter/gatherer scenarios: fish, game and berries

The environmental assessment of long-term nuclear waste management requires data to estimate food chain transfers for radionuclides in various environmental settings. For key elements such as iodine (I) and chlorine (Cl), there is a paucity of transfer factor data, particularly outside of agricultural food chains. This study dealt with transfers of I, Cl and 28 other elements to foods that would be typical of boreal hunter/gatherer lifestyles, as well as being common foods for modern recreational and subsistence hunters. Food/substrate concentration ratios (CRs) and related transfer factors for eight species of widely distributed fish, whitetail deer (Odocoileus virginianus), Canada geese (Branta canadensis) and wild blueberries (Vaccinium myrtilloides) were measured and compared to the literature. Limited data were obtained for caribou (Rangifer tarandus), elk (Cervus elaphus) and moose (Alces americanus). Freshwater sediment Kd values and CRs for a ubiquitous freshwater macrophyte were also obtained. The CRs for I in fish were 29 L kg⁻¹ in edible muscle (fillets) of large-bodied species and 85 L kg⁻¹ for whole, small-bodied fish. The log CRs for fish and macrophytes were correlated across elements. For several elements, the Kds for sediments in deep water were ∼4-fold higher than for littoral samples. The elemental transfers to wild animals for some elements were notably different than the literature indicates for domestic animals. It is argued that the transfer data obtained using indigenous elements from real environmental settings, as opposed to contaminant elements in experimental or impacted environments, are especially relevant to assessment of long-term impacts.     

Dose assessment for marine biota and humans from discharge of (131)I to the marine environment and uptake by algae in Sydney, Australia

Iodine-131 reaches the marine environment through its excretion to the sewer by nuclear medicine patients followed by discharge through coastal and deepwater outfalls. ¹³¹I has been detected in macroalgae, which bio-accumulate iodine, growing near the coastal outfall of Cronulla sewage treatment plant (STP) since 1995. During this study, ¹³¹I levels in liquid effluent and sludge from three Sydney STPs as well as in macroalgae (Ulva sp. and Ecklonia radiata) growing near their shoreline outfalls were measured. Concentration factors of 176 for Ulva sp. and 526 for E. radiata were derived. Radiation dose rates to marine biota from ¹³¹I discharged to coastal waters calculated using the ERICA dose assessment tool were below the ERICA screening level of 10 μGy/hr. Radiation dose rates to humans from immersion in seawater or consumption of Ulva sp. containing ¹³¹I were three and two orders of magnitude below the IAEA screening level of 10 μSv/year, respectively.