Yukun Fan

Iodine-129 in Seawater Offshore Fukushima: Distribution, Inorganic Speciation, Sources, and Budget

The Fukushima nuclear accident in March 2011 has released a large amount of radioactive pollutants to the environment. Of the pollutants, iodine-129 is a long-lived radionuclide and will remain in the environment for millions of years. This work first report levels and inorganic speciation of (129)I in seawater depth profiles collected offshore Fukushima in June 2011. Significantly elevated (129)I concentrations in surface water were observed with the highest (129)I/(127)I atomic ratio of 2.2 × 10(-9) in the surface seawater 40 km offshore Fukushima. Iodide was found as the dominant species of (129)I, while stable (127)I was mainly in iodate form, reflecting the fact that the major source of (129)I is the direct liquid discharges from the Fukushima NPP. The amount of (129)I directly discharged from the Fukushima Dai-ichi nuclear power plant to the sea was estimated to be 2.35 GBq, and about 1.09 GBq of (129)I released to the atmosphere from the accident was deposited in the sea offshore Fukushima. A total release of 8.06 GBq (or 1.2 kg) of (129)I from the Fukushima accident was estimated. These Fukushima-derived (129)I data provide necessary information for the investigation of water circulation and geochemical cycle of iodine in the northwestern Pacific Ocean in the future.

Determination of Ultralow Level 129I/127I in Natural Samples by Separation of Microgram Carrier Free Iodine and Accelerator Mass Spectrometry Detection

Separation of carrier free iodine from low iodine level samples and accurate measurement of ultralow level (129)I in micrograms of iodine target are essential but a bottleneck in geological dating of terrestrial system and tracer research using naturally produced (129)I. In this work, we present a carrier free method using coprecipitation of AgI with AgCl for preparing micrograms of iodine target, associated with combustion using a tube furnace for separating iodine from solid samples and anion exchange chromatography for preconcentrating iodine from a large volume of water. An accelerator mass spectrometry was used to measure ultralow level (129)I in micrograms of iodine target. The recovery of iodine in the entire separation procedure is higher than 80% and 65% for solid and water samples, respectively. One microgram iodine in the target (AgI-AgCl) can produce a stable (127)I signal for AMS measurement of (129)I/(127)I, and a detection limit of this method for (129)I is calculated to be 10(5) atoms. This will allow us to accurately determine (129)I in prenuclear geological samples of low iodine concentration with (129)I/(127)I of 10(-12), such as loess, soil, coral, rock, sediment, and groundwater. Some samples with low iodine content have been successfully analyzed, and the lowest value of the (129)I/(127)I ratio of 2 × 10(-11) was observed in 23.5 and 63.5 m loess samples collected in the Loess Plateau, China. The developed method sheds light on a wide application in earth science.

129)I record of nuclear activities in marine sediment core from Jiaozhou Bay 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 (129)I to investigate the influence of human nuclear activities in this region. Significantly enhanced (129)I level was observed in upper 70 cm of the sediment core, with peak values in the layer corresponding to 1957, 1964, 1974, 1986, and after 1990. The sources of (129)I 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 (129)I. The very well (129)I records of different human nuclear activities in the sediment core illustrate the potential application of (129)I in constraining ages and sedimentation rates of the recent sediment. The releases of (129)I from the European nuclear fuel reprocessing plants at La Hague (France) and Sellafield (UK) were found to dominate the inventory of (129)I in the Chinese sediments after 1990, not only the directly atmospheric releases of these reprocessing plants, but also re-emission of marine discharged (129)I of these reprocessing plants in the highly contaminated European seas.

Speciation analysis of 129I in seawater by carrier-free AgI-AgCl coprecipitation and accelerator mass spectrometric measurement.

A rapid and simple method was developed for speciation analysis of (129)I in seawater by selective coprecipitation of carrier-free iodide and accelerator mass spectrometry (AMS) measurement of (129)I. Iodide was separated from seawater and other species of iodine by coprecipitation of AgI with Ag2SO3, AgCl, and AgBr by addition of only 100 mg/L Ag(+) and 0.3 mmol/L NaHSO3 at pH 4.2-5.5. The separation efficiency of iodide was more than 95%, and crossover between (129)IO3(-) and (129)I(-) fractions is less than 3%. Iodate and total inorganic iodine were converted to iodide by use of NaHSO3 at pH 1-2 and then separated by the same method as for iodide. Ag2SO3 in the coprecipitate was removed by washing with 3 mol/L HNO3 and the excess AgCl and AgBr was removed by use of diluted NH3, and finally a 1-3 mg precipitate was obtained for AMS measurement of (129)I. The recovery of iodine species in the entire procedure is higher than 70%. Six seawater samples collected from the Norwegian Sea were analyzed by this method as well as a conventional anion-exchange chromatographic method; the results from the two methods show no significant difference (p = 0.05). Because only one separation step and fewer chemicals are involved in the procedure, this method is suitable for operation on board sampling vessels, as it avoids the transport of samples to the laboratory and storage for a longer time before analysis, therefore significantly improving the analytical capacity and reliability of speciation analysis of (129)I. This improvement can stimulate oceanographic tracer studies of (129)I.

Impact of North Korean nuclear weapons test on 3 September, 2017 on inland China traced by 14C and 129I

Environmental impact of North Korea nuclear weapons testing on 3 Sept, 2017, is of key concern. In order to investigate whether there is radioactive leakage and whether it can be transported to inland China, 14C and 129I are determined in aerosol samples collected in a Chinese inland city before and after the test. Aerosol Δ14C values before and after the test do not show any significant difference. In contrast, a four-fold increase of 129I/127I ratios was found after the test. The possible sources of 129I in these atmospheric samples and the impact of the North Korea nuclear test are discussed.

Authentication of Chinese vintage liquors using bomb-pulse (14)C.

The older a bottle of Chinese vintage liquor is, the higher the price it commands. Driven by the potential for higher profits, some newly-founded distilleries openly sell liquor whose storage ages are exaggerated. In China, the market for vintage liquor has become fraught with uncertainty and a pressing need has arisen to establish an effective method to authenticate the age of vintage liquors. A radiocarbon (14C) dating method is described here that can verify cellar-stored years of Chinese liquors distilled within the last fifty years. Two different flavored Chinese liquors produced in “the golden triangular region” in the Upper Yangtze River region in southwest China, with known cellar-stored years, were analyzed to benchmark the technique. Strong flavored liquors are found to be consistent with local atmospheric Δ14C values. A small offset of 2–3 years between predicted vintage years of soy-sauce flavored liquors and strong flavored liquors is found to be associated with the fermentation cycle of certain varieties. The technique can measure cellar-stored years of a wide range of liquors including those with fundamentally different aromas. This demonstrates the strength of our method in identifying suspect Chinese vintage liquors.

Rapid determination of 129I in large-volume water samples using rotary evaporation preconcentration and accelerator mass spectrometry measurement

A rapid method using rotary evaporation combined with accelerator mass spectrometry (AMS) measurement, was developed for the determination of 129I in large-volume water samples. The parameters including water bath temperature, pH, concentration volume and reducing reagent, were thoroughly optimized. The chemical yield of iodine under the optimal conditions is between 98.8 and 100.7%. Compared to the direct evaporation, the enrichment time can be shortened by five times. The measured 129I/127I ratios for the environmental water samples are in good agreement with those previously reported values, suggesting this method is accurate, robust and suitable for 129I determination in large water samples.

Measurement of 129I Level Around a Nuclear Power Plant by Accelerator Mass Spectrometer

129 I is a long-lived (15.7M year) radioisotope of iodine. It can be used as a tracer for monitoring nuclear proliferation and the 129 I/127 I ratio can be used to evaluate the radiation contamination level. Nowadays a great number of nuclear power plants will be built in China, but the data of 129 I concentration in environmental samples around nuclear power plants are limited. Accelerator Mass Spectrometer (AMS) whose detection limit is about 10−14 , is one of the best instruments for analyzing environmental samples. The methods of making 129 I target samples for AMS measurement from different type samples were studied, and the processing system for water and soil samples were established. Six surface seawater samples were collected at different distance away from a nuclear power plant in China. These samples were measured by Xi’an AMS. The ratios of 129 I/127 I in the seawater samples are between 0.829 × 10−10 and 9.451 × 10−10 , and the average value is about 3.518 × 10−10 . The ratios of 129 I/127 I in these samples are compared with other measurement results under different circumstances in other parts of the world. The results show that this nuclear power plant has not released superfluous 129 I into environment after several years’ operation. Since the AMS and sample processing system are established, we will do much work on nuclear technology application with 129 I tracer.© 2010 ASME