129I record of nuclear activities in marine sediment core from JiaozhouBay in China

Iodine-129 has been used as a powerful tool for environmental tracing of human nuclear activities. In this work, a sediment core collected from Jiaozhou Bay, the east coast of China, in 2002 was analyzed for 129I to investigate the influence of human nuclear activities in this region. Significantly enhanced 129I level was observed in upper 70&nbsp;cm of the sediment core, with peak values in the layer corresponding to 1957, 1964, 1974, 1986, and after 1990. The sources of 129I and corresponding transport processes in this region are discussed, including nuclear weapons testing at the Pacific Proving Grounds, global fallout from a large numbers of nuclear weapon tests in 1963, the climax of Chinese nuclear weapons testing in the early 1970s, the Chernobyl accident in 1986, and long-distance dispersion of European reprocessing derived 129I. The very well 129I records of different human nuclear activities in the sediment core illustrate the potential application of 129I in constraining ages and sedimentation rates of the recent sediment. The releases of 129I from the European nuclear fuel reprocessing plants at La Hague (France) and Sellafield (UK) were found to dominate the inventory of 129I in the Chinese sediments after 1990, not only the directly atmospheric releases of these reprocessing plants, but also re-emission of marine discharged 129I of these reprocessing plants in the highly contaminated European seas.</p

Progress on I-129 analysis and its application in environmental and geological researches

Iodine-129 is a naturally generated isotope, but anthropogenic releases are the dominated source of I-129 in the present environment. Among many measurement techniques, neutron activation analysis (NM) and accelerator mass spectrometry (AMS) are only methods used for measurement of I-129 in environmental level. Based on its source terms, chemical properties and environmental behaviors, I-129 can be applied for geological dating in a range of 2-80 Ma, investigation of formation and migration of hydrocarbon, circulation of ocean water, atmospheric process of iodine, as well as reconstruction of dispersion and migration of short-lived radioisotopes of iodine released from nuclear accidents. This article aims to summarize and critically compare the analytical techniques used for I-129 measurement and chemical methods for separation of iodine from various sample matrices, purification from the interferences, as well as preparation of suitable target for AMS measurement. The major applications in environmental and geological researches are reviewed, which mainly focus on the new progress and potential development in the future. The application of I-129 in the investigation of radioactive contamination from the Fukushima accident is discussed.</p

Uranium isotopes in carbonate aquifers of arid region setting

Groundwater in arid and semiarid regions is vital resource for many uses and therefore information about concentrations of uranium isotopes among other chemical parameters are necessary. In the study presented here, distribution of U-238 and U-235 in groundwater of four selected locations in the southern Arabian peninsula, namely at two locations within the United Arab Emirates (UAE) and two locations in Oman are discussed. The analyses of the uranium isotopes were performed using ICP-MS and the results indicated a range of concentrations for U-235 and (238) U at 3-39 ng L-1 (average: 18 ng L-1) and 429-5,293 ng L-1 (average: 2,508 ng L-1) respectively. These uranium concentrations are below the higher permissible WHO limit for drinking water and also comparable to averages found in groundwater from similar aquifers in Florida and Tunisia. Negative correlation between rainfall and uranium concentrations suggests that in lithologically comparable aquifers, climate may influence the concentration of uranium in subtropical to arid regions.</p

Comparison of sample preparation methods for reliable plutonium and neptunium urinalysis using automatic extraction chromatography

This paper describes improvement and comparison of analytical methods for simultaneous determination of trace-level plutonium and neptunium in urine samples by inductively coupled plasma mass spectrometry (ICP-MS). Four sample pre-concentration techniques, including calcium phosphate, iron hydroxide and manganese dioxide co-precipitation and evaporation were compared and the applicability of different techniques was discussed in order to evaluate and establish the optimal method for in vivo radioassay program. The analytical results indicate that the various sample pre-concentration approaches afford dissimilar method performances and care should be taken for specific experimental parameters for improving chemical yields. The best analytical performances in terms of turnaround time (6 h) and chemical yields for plutonium (88.7 +/- 11.6%) and neptunium (94.2 +/- 2.0%) were achieved by manganese dioxide co-precipitation. The need of drying ashing (&gt;= 7 h) for calcium phosphate co-precipitation and long-term aging (5 d) for iron hydroxide co-precipitation, respectively, rendered time-consuming analytical protocols. Despite the fact that evaporation is also somewhat time-consuming (1.5 d), it endows urinalysis methods with better reliability and repeatability compared with co-precipitation techniques. In view of the applicability of different pre-concentration techniques proposed previously in the literature, the main challenge behind relevant method development is pointed to be the release of plutonium and neptunium associated with organic compounds in real urine assays. In this work, different protocols for decomposing organic matter in urine were investigated, of which potassium persulfate (K2S2O8) treatment provided the highest chemical yield of neptunium in the iron hydroxide co-precipitation step, yet, the occurrence of sulfur compounds in the processed sample deteriorated the analytical performance of the ensuing extraction chromatographic separation with chemical yields of &lt;= 50%.</p

Determination of ultra-low level plutonium isotopes (Pu-239,(240)pu) in environmental samples with high uranium

In order to measure trace plutonium and its isotopes ratio (240Pu/239Pu) in environmental samples with a high uranium, an analytical method was developed using radiochemical separation for separation of plutonium from matrix and interfering elements including most of uranium and ICP-MS for measurement of plutonium isotopes. A novel measurement method was established for extensively removing the isobaric interference from uranium (238U1H and 238UH2+) and tailing of 238U, but significantly improving the measurement sensitivity of plutonium isotopes by employing NH3/He as collision/reaction cell gases and MS/MS system in the triple quadrupole ICP-MS instrument. The results show that removal efficiency of uranium interference was improved by more than 15 times, and the sensitivity of plutonium isotopes was increased by a factor of more than 3 compared to the conventional ICP-MS. The mechanism on the effective suppress of 238U interference for 239Pu measurement using NH3-He reaction gases was explored to be the formation of UNH+ and UNH2+ in the reactions of UH+ and U+ with NH3, while no reaction between NH3 and Pu+. The detection limits of this method were estimated to be 0.55 fg mL-1 for 239Pu, 0.09 fg mL&minus;1 for 240Pu. The analytical precision and accuracy of the method for Pu isotopes concentration and 240Pu/239Pu atomic ratio were evaluated by analysis of sediment reference materials (IAEA-385 and IAEA-412) with different levels of plutonium and uranium. The developed method were successfully applied to determine 239Pu and 240Pu concentrations and 240Pu/239Pu atomic ratios in soil samples collected in coastal areas of eastern China.</p

Tracing variability in the iodine isotopes and species along surfacewater transect from the North Sea to the Canary Islands

A complete transect of surface water samples from the North Sea to the Canary Islands was collected during a continuous period in 2010. The samples were analyzed for total 129I and 127I isotopes and their iodide and iodate species. The results indicate a large variability in the total 129I and its species along the transect, whereas less change and variation are observed for the total 127I and its species. Transport of 129I from the western English Channel via Biscay Bay is the main source of 129I in the northeastern Atlantic Ocean.</p

Analysis of low-level I-129 in brine using accelerator mass spectrometry

An improved solvent extraction procedure for iodine separation from brine samples has been applied at Xi&#39;an Accelerator Mass Spectrometry (AMS) center. Oil in the brine sample has to be removed to avoid appearance of the third phase during solvent extraction and to improve the chemical yield of iodine. The small amount of oil remained in the water phase was first removed by phase separation through settling down sufficiently based on their immiscibility, and then by filtration through a cellulose filter, on which oil was absorbed and removed. After oil removed, extraction recovery of iodine could achieve more than 90 %. The sodium bisulfite as an effective reductant should be added before acidification to avoid loss of iodine by formation of I-2 in sample via reaction of iodate and iodide at pH 1-2, and then pH was adjusted to 1-2 to reduce the iodate to iodide followed by oxidation of iodide to I-2 and solvent extraction to separate all inorganic iodine. As a pre-nuclear era sample, I-129/I-127 ratio in brine is normally more than two orders of magnitude lower than that in present surface environmental samples, so prevention of cross-contamination and memory effect in apparatus during processing procedure are very critical for obtaining reliable results, and monitoring the procedure blank is very important for analytical quality of I-129. The I-129/I-127 isotopic ratio in the brine samples and procedure blank of iodine reagents were measured to be (1.9-2.7) x 10(-13) and 2.08 x 10(-13), respectively, 3-4 orders of magnitudes lower than that in environmental samples in Xi&#39;an, and the result of procedure blank is in the same level as the previous experiments in past 3 years, indicating contamination is not observed in our method.</p

129I assessment reveals the impact of Fukushima incidenton Dapeng Peninsula, Shenzhen, China

In order to assess the radioactive impact of Fukushima Incident on the coastal environment of Dapeng Peninsula, Shenzhen, China, combining accelerator mass spectrometry with epithermal neutron activation analysis, we measured the 129I/127I ratios and 129I levels in surface seawater, oyster (Ostrea gigas) and kelp (Sargassum henslouianum). The results showed that the influence of Daya Bay Nuclear Power Base was ignorable to local environment, but the Fukushima Incident had caused significant increase of 129I levels in oyster (P&nbsp;&lt;&nbsp;0.001) and kelp (P&nbsp;&lt;&nbsp;0.05) from Dapeng Peninsula between Jun-2011 and Apr-2012. However, the 129I levels in oyster and kelp were far below the guideline given by Codex Alimentarius Commission and would not cause immediate harm to the health of local residents.</p

Level and source of 129I of environmental samples in Xi'an region, China

Iodine-129 is widely used as a tracer in various environmental practices such as monitoring of nuclear environmental safety, seawater exchange and transport, geochemical cycle of stable iodine and dating of geological events. The spatial distribution of (129)I concentration varies significantly on global scale because of anthropogenic input from nuclear activities coupled with scarcity of data on environmental (129)I variability in many parts of the world including Asia. Here we report new data on (129)I and (127)I concentrations in soil, vegetation, river water and precipitation collected from Xi&#39;an area, China. The results indicate values for environmental (129)I/(127)I ratios in the investigated area range from 1.1 x 10(-10) to 43.5 x 10(-10) with a mean of 20.6 x 10(-10), which is 1-3 orders of magnitude lower than the ratios observed in Europe, but comparable with those observed in the locations far from direct effect of point release sources and at similar latitude. The main source of (129)I in the investigated area is attributed to the global fallout of both atmospheric nuclear weapons testing and long distance dispersion of fuel reprocessing releases. (C) 2011 Elsevier B.V. All rights reserved.</p

Iodine-129 in Snow and Seawater in the Antarctic: Level and Source

Anthropogenic 129I has been released to the environment in different ways and chemical species by human nuclear activities since the 1940s. These sources provide ideal tools to trace the dispersion of volatile pollutants in the atmosphere. Snow and seawater samples collected in Bellingshausen, Amundsen, and Ross Seas in Antarctica in 2011 were analyzed for 129I and 127I, including organic forms; it was observed that 129I/127I atomic ratios in the Antarctic surface seawater ((6.1&minus;13) &times; 10&minus;12) are about 2 orders of magnitude lower than those in the Antarctic snow ((6.8&minus;9.5) &times; 10&minus;10), but 4&minus;6 times higher than the prenuclear level (1.5 &times; 10&minus;12), indicating a predominantly anthropogenic source of 129I in the Antarctic environment. The 129I level in snow in Antarctica is 2&minus;4 orders of magnitude lower than that in the Northern Hemisphere, but is not significantly higher than that observed in other sites in the Southern Hemisphere. This feature indicates that 129I in Antarctic snow mainly originates from atmospheric nuclear weapons testing from 1945 to 1980; resuspension and re-emission of the fallout 129I in the Southern Hemisphere maintains the 129I level in the Antarctic atmosphere. 129I directly released to the atmosphere and re-emitted marine discharged 129I from reprocessing plants in Europe might not significantly disperse to Antarctica.</p