Anthropocene 129I Record in the Yellow Sea Sediments and Its Indication for River-Delivered Radioactive Pollution to Marginal Seas.

As the number of coastal nuclear facilities rapidly increases and the wastewater from the Fukushima Nuclear Plant has been discharged into the Pacific Ocean, the nuclear environmental safety of China's marginal seas is gaining increased attention along with the heightened potential risk of nuclear accidents. However, insufficient work limits our understanding of the impact of human nuclear activities on the Yellow Sea (YS) and the assessment of their environmental process. This study first reports the 129I and 127I records of posthuman nuclear activities in the two YS sediments. Source identification of anthropogenic 129I reveals that, in addition to the gaseous 129I release and re-emission of oceanic 129I discharged from the European Nuclear Fuel Reprocessing Plants (NFRPs), the Chinese nuclear weapons testing fallout along with the global fallout is an additional 129I input for the continental shelf of the YS. The 129I/127I atomic ratios in the North YS (NYS) sediment are significantly higher than those in the other adjacent coastal areas, attributed to the significant riverine input of particulate 129I by the Yellow River. Furthermore, we found a remarkable 129I latitudinal disparity in the sediments than those in the seawaters in the various China seas, revealing that sediments in China's marginal seas already received a huge anthropogenic 129I from terrigenous sources via rivers and thus became a significant sink of anthropogenic 129I. This study broadens an insight into the potential impacts of terrigenous anthropogenic pollution on the Chinese coastal marine radioactive ecosystem.

Isotopic Evidence Unveils Fossil Fuels Contribution to Atmospheric Iodine.

Iodine is a crucial nutrient for public health, and its presence in the terrestrial atmosphere is a key factor in determining the prevalence of iodine deficiency disorders. While oceanic iodine emissions decrease at lower sea surface temperatures, the primary contributors to atmospheric iodine can vary from oceanic sources in the summer to other sources in winter. However, the specific sources and their respective contributions have remained unexplored. Fortunately, the atomic ratio of 129I to 127I significantly differs between nuclear activity and fossil fuels like coal and petroleum, which formed millions to billions of years ago. This distinction makes 129I a valuable tool for identifying iodine sources. In our study, we analyzed iodine isotopes and incorporated additional indicators such as element content in PM2.5 samples. Our findings reveal, for the first time, that in winter inland areas, fuel oil, alongside coal combustion, is a significant source of atmospheric iodine. This research enhances our comprehension of the impact of human activities on iodine levels in the environment. This understanding is crucial not only for addressing iodine deficiency-related health concerns but also for comprehending stratospheric ozone depletion, a phenomenon closely associated with atmospheric iodine.

Concentrations of iodine-129 in livestock, agricultural, and fishery products around spent nuclear fuel reprocessing plant in Rokkasho, Japan, during and after its test operation.

Concentrations of iodine-129 (129I) and atomic ratios of 129I/127I in livestock (grass and milk), agricultural (cabbage, Japanese radish, and rice), and fishery (flatfish and brown alga) products collected from locations around the first Japanese commercial spent nuclear fuel reprocessing plant in Rokkasho were measured from 2006 to 2016. The actual spent nuclear fuel rods were cut and processed to test the functioning of the plant that discharged controlled amounts of 129I to the atmosphere and coastal seawater during the period from 2006 to 2008 (the "cutting period"). Statistically significant increases in 129I concentration and 129I/127I ratio were observed during the cutting period in livestock products and flatfish. On the other hand, these parameters were statistically comparable during and after the cutting period in the other products. The radiation dose through the ingestion of the maximum 129I concentrations, measured in the different products, was estimated to be in the nanoSievert per year level. This value is much smaller than 1 mSv yr-1, which is the permissible authentic radiation dose for the general public. The 129I levels in the samples, especially in milk and flatfish, are discussed in context of the 129I discharge history from the plant.

Radioiodine Biogeochemistry and Prevalence in Groundwater.

129I is commonly either the top or among the top risk drivers, along with 99Tc, at radiological waste disposal sites and contaminated groundwater sites where nuclear material fabrication or reprocessing has occurred. The risk stems largely from 129I having a high toxicity, a high bioaccumulation factor (90% of all the body's iodine concentrates in the thyroid), a high inventory at source terms (due to its high fission yield), an extremely long half-life (16M years), and rapid mobility in the subsurface environment. Another important reason that 129I is a key risk driver is that there is uncertainty regarding its biogeochemical fate and transport in the environment. We typically can define 129I mass balance and flux at sites, but cannot predict accurately its response to changes in the environment. As a consequence of some of these characteristics, 129I has a very low drinking water standard, which is set at 1 pCi/L, the lowest of all radionuclides in the Federal Register. Recently, significant advancements have been made in detecting iodine species at ambient groundwater concentrations, defining the nature of the organic matter and iodine bond, and quantifying the role of naturally occurring sediment microbes to promote iodine oxidation and reduction. These recent studies have led to a more mechanistic understanding of radioiodine biogeochemistry. The objective of this review is to describe these advances and to provide a state of the science of radioiodine biogeochemistry relevant to its fate and transport in the terrestrial environment and provide information useful for making decisions regarding the stewardship and remediation of 129I contaminated sites. As part of this review, knowledge gaps were identified that would significantly advance the goals of basic and applied research programs for accelerating 129I environmental remediation and reducing uncertainty associated with disposal of 129I waste. Together the information gained from addressing these knowledge gaps will not alter the observation that 129I is primarily mobile, but it will likely permit demonstration that the entire 129I pool in the source term is not moving at the same rate and some may be tightly bound to the sediment, thereby smearing the modeled 129I peak and reducing maximum calculated risk.

Records of the riverine discharge of 129I in riverbank sediment after the Fukushima accident.

Although 129I discharge from watersheds is fundamental for assessing long-term radiation effects on aquatic ecosystems, 129I originating from the Fukushima nuclear accident is yet be evaluated. This study investigated the transport behavior of 129I by riverbank surveys conducted from 2013 to 2015 in a watershed where the 129I/137Cs activity ratio is low in the mountainous area and high in the plain as of 2011. Until 2015, the 129I/137Cs activity ratio of the levee crown in the studied watershed was similar to that of the surrounding area in 2011. However, the 129I/137Cs ratios of the surface riverbank sediments were all low, indicating that radionuclides transported from the mountainous area were deposited on the riverbank in the plain. The vertical distribution of the 129I/137Cs ratio in the riverbank sediments indicated that some 129I and 137Cs deposited during the accident remained in the lower layers, but most were eroded immediately after the accident. Based on the 129I/137Cs ratios of sediments deposited on the riverbank, which remained constant until 2015 after the accident, the amount of 129I discharged to the ocean was determined from the previously evaluated 137Cs discharge. It was calculated that 1.8 × 105 Bq and 1.2 × 107 Bq of 129I were discharged with sediment from the studied watershed and the contaminated river watersheds (Abukuma River and Fukushima coastal rivers, including the study river), respectively. This amount of 129I was 0.3% of the 129I released from the Fukushima Dai-ichi Nuclear Power Plant into the ocean immediately after the accident. Furthermore, a comparison of the 129I/137Cs ratio showed that the continuous 129I and 137Cs discharge from the river contribute little to their amount in the seafloor sediments along the Fukushima coast.

Sources of highly regional 129I in soils in northeast China.

The transport and deposition pathways of anthropogenic radionuclides at the global scale, particularly volatile 129I, remain somewhat elusive due to a dearth of comprehensive investigations. To gain a better understanding of the transport dynamics and deposition mechanism of anthropogenic 129I in the terrestrial environment, one hundred surface soil samples collected from northeast China were analyzed for 129I and 127I concentrations in this study. Our findings reveal that 129I/127I atomic ratios in the mid-eastern Inner Mongolia (MIM) were approximately an order of magnitude higher than the rest of the investigated area. This is, besides the global fallout and the long-range transport of 129I released from the European nuclear reprocessing plants via westerly winds, possibly attributed to the dust with high 129I levels from the East Asian arid regions. In addition to the significant dust-induced 129I input, the unique meteorological conditions and topographical features in the MIM synergistically contribute to the pronounced accumulation and deposition of 129I in this region. This study will provide novel insights into the transport and deposition mechanism of anthropogenic radionuclides, which is significant for the assessment of anthropogenic nuclear activities on the environment in the future.

Reconstructing atmospheric 129I deposition over 170 years with the varved sediment in the Sihailongwan Maar Lake, northeast China.

Long-term deposition of atmospheric radioactive iodine-129 (129I) is important for assessing the impact of human nuclear activities (HNAs), but still not well understood in East Asia. In this study, we quantitatively reconstructed the deposition history of airborne 129I using varved sediment from Sihailongwan Maar Lake (SHLW) in northeast China. Our results revealed significant increases in 129I concentrations and 129I/127I atomic ratios since the 1950s, indicating the influence of HNAs on the environment and marking the onset of the Anthropocene. The variation of 129I in the investigated site can be primarily attributed to the global fallout of ANWT as well as nuclear fuel reprocessing in Europe, Russia and the USA. Notably, neither the Chernobyl nor the Fukushima nuclear accidents have had any discernable impact on the SHLW Lake. Over the past 170 years (1846-2021), the reconstructed fluxes indicate a rapid increase in 129I deposition from the early 1950s until the 1970s followed by dramatic changes thereafter. The measured 129I fluxes range between (1.26-349) × 109 atoms m-2 yr-1 in the SHLW Lake, which are consistent with similar latitude zones across East Asia, but differ significantly from those observed in high-elevation glaciers within the Northern Hemisphere due to prevailing atmospheric circulation patterns. The total 129I inventory was calculated to be 11.9 × 1012 atoms m-2, with natural and anthropogenic 129I accounting for 2.86 % and 97.1 %, respectively, suggesting an overwhelming artificial contribution. The reconstructed fluxes and inventory of atmospheric 129I deposition quantitatively distinguish the natural and artificial contributions, and provide a novel insight into the historical environmental impact of HNAs in East Asia and the characteristics of the Anthropocene.

129I in the SE-Dome ice core, Greenland: A new candidate golden spike for the Anthropocene.

The Anthropocene is a proposed geological epoch that will mark the time when humans have irreversibly affected the Earth. One of the primary requirements to formally establish this is a Global Boundary Stratotype Section and Point or "golden spike" - a record of a planetary signal marking the new epoch's beginning. The leading candidates for the Anthropocene's golden spike are the fallout peaks of 14C (T1/2 = 5730 y) and 239Pu (T1/2 = 24,110 y) from nuclear weapons testing in the 1960s. However, these radionuclides' half-lives may not be long enough for their signals to be observable in the far future and are, thus, not durable. In this regard, here we show the 129I time series record (1957-2007) of the SE-Dome ice core, Greenland. We find that 129I in SE-Dome records almost the entire history of the nuclear age in excellent detail at a time resolution of about four months. More specifically, 129I in SE-Dome reflects signals from nuclear weapons testing in 1958, 1961, and 1962, the Chernobyl Accident in 1986, and various signals from nuclear fuel reprocessing within the same year or a year after. The quantitative relationships between 129I in SE-Dome and these human nuclear activities were established using a numerical model. Similar signals are observed in other records from various environments worldwide, such as sediments, tree rings, and corals. This global ubiquity and synchronicity are comparable to those of the 14C and 239Pu bomb signals, but the much longer half-life of 129I (T1/2 = 15.7 My) makes it a more durable golden spike. For these reasons, the 129I record of the SE-Dome ice core can be considered an excellent candidate for the Anthropocene golden spike.

129I in rainwater across Argentina.

Concentrations of 127I and 129I in rainwater samples from several stations across Argentina (latitudes between 25° S and 55° S) were measured and analyzed for the assessment of distribution patterns and potential sources of 129I in the Southern Hemisphere. Measured 129I levels, clearly above those explainable by natural background and atmospheric nuclear weapons tests, can be understood by the injection into the Southern Hemisphere of 129I that had been discharged from nuclear fuel reprocessing plants in the Northern Hemisphere.

Large seasonal fluctuations of groundwater radioiodine speciation and concentrations in a riparian wetland in South Carolina.

Recent studies evaluating multiple years of groundwater radioiodine (129I) concentration in a riparian wetland located in South Carolina, USA identified strong seasonal concentration fluctuations, such that summer concentrations were much greater than winter concentrations. These fluctuations were observed only in the wetlands but not in the upland portion of the plume and only with 129I, and not with other contaminants of anthropogenic origin: nitrate/nitrite, strontium-90, technecium-99, tritium, or uranium. This unexplained observation was hypothesized to be the result of strongly coupled processes involving hydrology, water temperature, microbiology, and chemistry. To test this hypothesis, an extensive historical groundwater database was evaluated, and additional measurements of total iodine and iodine speciation were made from recently collected samples. During the summer, the water table decreased by as much as 0.7 m, surface water temperature increased by as much as 15 °C, and total iodine concentrations were consistently greater (up to 680%) than the following winter months. Most of the additional iodine observed in the summer could be attributed to proportional gains in organo-iodine, and not iodide or iodate. Furthermore, 129I concentrations were observed to be two-orders-of-magnitude greater at the bottom of the upland aquifer than at the top. A coupled hydrological and biogeochemical conceptual model is proposed to tie these observations together. First, as the surface water temperature increased during the summer, microbial activity was enhanced, which in turn stimulated the formation of mobile organo-I. Hydrological processes were also likely involved in the observed iodine seasonal changes: (1) as the water table decreased in summer, the remaining upland water entering the wetland was comprised of a greater proportion of water containing elevated iodine concentrations from the low depths, and (2) water flow paths in summer changed such that the wells intercepted more of the contaminant plume and less of the diluting rainwater (due to evapotranspiration) and streamwater (as the lower levels promote a predominantly recharging system). These results underscore the importance of coupled processes influencing contaminant concentrations, and the need to assess seasonal contaminant variations to optimize long-term monitoring programs of wetlands.

Mathematical simulation of the Pacific Proving Grounds 129I/127I nuclear bomb peaks in coral cores from the Philippines.

One recent way of reconstructing the historical impact of aboveground nuclear weapons testing (ANWT) in places lacking historical data is by measuring 129I in natural archives such as coral cores. However, discussions arising from 129I in corals remain qualitative or semi-quantitative, which do not maximize the potential information derivable from the data. In this study, we construct a mathematical model that simulates the 129I bomb peaks from the Pacific Proving Grounds (PPG) tests, as observed in available coral core data from the east (Baler) and west (Parola) sides of the Philippines. Results show that the model can determine the expected increase in 129I/127I ratio in the Philippines per megaton of ANWT detonated in the PPG; confirm time lags for each major transport pathway from the PPG to the Philippines, indicating when to expect the radioactivity spike after detonation; and determine the most significant transport pathway from the PPG to each coral location. This work increases the application and significance of 129I/127I coral core data by deriving quantitative information about the magnitude, timing, and transport pathways of radioactivity from the ANWT site to the coral location. In the future, the model can be expanded to simulate other 129I sources besides ANWT.

Mass-spectrometric determination of iodine-129 using O2-CO2 mixed-gas reaction in inductively coupled plasma tandem quadrupole mass spectrometry.

This paper presents a mass-spectrometric method for determining the radionuclide iodine-129 (129I) from the significant amount of interference in inductively coupled plasma tandem quadrupole mass spectrometry (ICP-MS/MS) using a dynamic reaction cell passing a mixture gas of O2 and CO2. Thus far, mass spectrometry analysis of trace amounts of 129I has been hampered by the presence of xenon-129 (129Xe) and the formation of polyatomic ions from excess amounts of stable isotope 127I. In this study, flowing a mixture gas of O2 and CO2 into the dynamic reaction cell (Q2) successfully removed both 129Xe interference and polyatomic interference (127IH2) in the analysis of 129I in ICP-MS/MS. The resulting ratio of (background noise of m/z 129)/127I was 4.6 × 10-10 ± 3.3 × 10-10, which enables the analysis of 10 mBq/L of 129I in the presence of 100 mg/L of stable 127I without chemical separation. The detection limit of this method was 0.73 mBq/L (= 0.11 ng/L) with an APEX-Q sample inlet desolvation device. For demonstration purposes, spike and recovery analysis of rainwater was performed, and good agreement between the spiked and recovered amounts was achieved.

A radioecological model with moisture-dependent Kd: Application to 129I and 79Se natural release to a grassland.

A radioecological model previously developed to simulate chlorine cycling in a Scots pine forest was modified to examine the effect of soil hydrochemical conditions on the fate of 129I and 79Se released to a grassland through natural discharge of contaminated groundwater. To this end, the constant solid-liquid distribution coefficient (Kd) in the original model was replaced by a parametric equation to estimate 129I and 79Se Kd values from soil saturation - as a proxy for soil redox potential - and a set of Kd values determined experimentally under oxic and anoxic conditions. Additionally, the multi-compartment Scots pine tree module was replaced by a two-compartment module to represent 129I and 79Se cycling in grass. Simulations undertaken with the model indicated a considerable effect of soil redox conditions on 129I and 79Se accumulation in the soil column, especially in the saturated subsoil above the water table. The constant Kd overestimated 129I accumulation in the soil in relation to the parametric Kd. In contrast, the constant Kd underestimated 79Se accumulation in the soil. These results have implications for radiological impact assessments, specifically regarding the degree of conservatism in the Kd used in the assessment. In respect of bioavailability to grass, the simulated soil-to-plant transfer factors of 129I and 79Se compared favourably with values reported in the literature for similar soils and plant species, giving confidence in the model performance. The model presented here is a step forward in radioecological modelling as it includes the key processes that drive radionuclide transfers in soil-plant systems and the effect of soil redox conditions on sorption. The model can be readily extended to other cultivated lands and release scenarios to predict radionuclide transfer up the food chain.

Records of iodine isotopes (129I, 127I) in the Barkol peat bog from northwest China and their sources, transport and preservation.

The research on geochemical behaviors of iodine is significant for deep understanding of the source and distribution of iodine on the earth. However, as one of the most important sources, the ocean emissions and relative transport pathways of iodine, as well as the preservation after deposition are still not well known, especially in the arid areas of central Asia. A peat sediment core collected nearby Barkol Lake from northwest China was analyzed for iodine isotopes (127I and 129I). The observed high 127I concentration in the top 2 cm indicated a significant accumulation of iodine in the surface oxic conditions due to the continuous sources of incompletely decomposed organic matter. Dissociation of iodine into pore waters occurred once the anoxic conditions established beneath the surface by a serial reduction reaction during the degradation of organic matter. The temporal variation of anthropogenic 129I in the peat sediment recorded its sources and transport pathways. Besides the global fallout 129I during late 1950s and early 1960s, the significantly increased air releases from the European nuclear fuel reprocessing plants during 1975-1997 and the increased marine discharges since 1990s contributed the major portion of 129I in the peat core. The major transport pathway of 129I from the Europe was through Westerlies following the re-emission of the marine discharged 129I to the atmosphere, indicating a clearly ocean emitted iodine in the concerned central Asia.

A historical record of the impact of nuclear activities based on 129I in coral cores in Baler, Philippines: An update.

In a previous study in 2016, we presented how 129I in coral cores from the east (Baler) and west (Parola) sides of the Philippines recorded the impacts of human nuclear activities, including nuclear weapons testing, nuclear fuel reprocessing, and nuclear accidents. However, the 2016 Baler dataset only had a two-year time resolution and a crude age model based on growth band counting. Here we present a new 2020 Baler 129I/127I atomic ratio dataset that features at least annual time resolution and a more accurate age model constructed using 3D X-ray Computed Tomography. Results show that the bomb peaks in Baler primarily came from the Pacific Proving Grounds or PPG with a time lag of about 1.8 years (or more specifically, between 1.3 and 2.4 years). Moreover, a review of the Parola dataset shows that PPG signals may have been transported to Parola in the West Philippine Sea via two pathways: the northward and southward bifurcations of the North Equatorial Current, reaching Parola about 4.5 and 8.5 years after detonation, respectively. Moreover, a prominent peak in the year 2014.7 in Baler possibly came from the 2011 Fukushima Accident, transported by the Kuroshio Recirculation Gyre and the North Pacific Mode Waters with a 3.5-year time lag. This study contributes to the understanding of the impact and transport of human-made radionuclides to the Philippines and the relevant oceanographic processes in the Western Equatorial Pacific region.

Tracing the upwelling process in the northern Benguela upwelling system (nBUS) by 129I.

New data on the presence of 129I in seawater in the Southern Hemisphere measured by Accelerator Mass Spectrometry (AMS) is presented. The samples were collected in 2014 along the Namibian coast during a cruise organised by the National Marine Information and Research Centre (NatMIRC), the national laboratories of the Ministry of Fisheries and Marine Resources (MFMR) in Namibia, and the IAEA Environment Laboratories (IAEA NAEL) in Monaco. The Benguela upwelling system is known as one of the most important marine upwelling regions in the world. Strong winds induce an offshore transport of surface seawater which is substituted by cool subsurface water inshore. As this water is nutrient-rich, which leads to high primary productivity, the Benguela upwelling system has a very important role as a fishing production area. The 129I concentrations in samples were between (0.66 ± 0.14) × 107 and (1.45 ± 0.30) × 107 atoms/kg. The highest 129I concentrations were found in the offshore surface samples. Deep-sea and inshore samples contained lower 129I concentrations, possibly as an effect of the upwelling process. A comparison with previously published studies suggests that the presence of 129I in the northern Benguela upwelling system (nBUS), is mainly due to the impact of nuclear weapons global fallout, without any evident impact of nuclear fuel reprocessing.

Evaluation of radioiodine (129I) dissolution from sediment of a brackish lake beside a spent nuclear fuel reprocessing plant in Japan.

Dissolution fluxes of stable (127I) and radioactive (129I) isotopes of iodine from a brackish lake sediment beside a spent nuclear fuel reprocessing plant in Japan were evaluated through two kinds of experiments: incubation using a sediment core sample for 24 h, and observation of 127I and 129I concentrations in sedimentary pore water. For 127I, the dissolution flux evaluated in the incubation experiment was comparable with that obtained from the vertical gradient of 127I concentration in pore water in the observation experiment. This suggests that degradation of organic matter in the surface sediment is an important source of dissolved 127I found in the water. For 129I, the dissolution flux estimated in the incubation experiment showed negative values, indicating the transfer of 129I to the sediment from the overlying water (i.e., absorption). Moreover, the flux evaluated from the observation experiment was positive. This result suggests that degradation of organic matter in the surface sediment is scarcely important to the supply of 129I from the sediment to the water in the studied lake. The dissolution flux of 129I estimated in the observation experiment was smaller than the absorption flux of 129I in the incubation experiment. This potentially indicates that the dissolution of sedimentary 129I does not significantly change 129I concentrations in the water and sediment of the lake. This hypothesis was consistent with previous research conducted for the studied lake.

Short-term metabolism of biologically incorporated 125I ingested by olive flounder (Paralichthys olivaceus).

Iodine-129 with a long half-time of 1.6 × 107 y was discharged into the Pacific Ocean during the final safety tests of the first commercial nuclear fuel reprocessing plant in Japan, at Rokkasho, Aomori Prefecture. Olive flounder (Paralichthys olivaceus) is an important fishery along this coast. It is necessary to determine whether 129I accumulates in this species to assess the possible public acceptance. We developed a short-term metabolism model of 125I in the flounder using retention data for 1-6 days after the olive flounder had ingested a freshwater fish species, medaka (Oryzias latipes), that had been labeled with 125I by keeping them in water containing 125I for 7 days. A single compartment model constructed from whole-body retention data for 125I in the olive flounder, excluding the gastrointestinal tract and its contents, revealed a biological half-time of 2.9 days for 125I. When the gill and other tissues were separated to individual compartments, the biological half-time in the gill was three times longer than that in the other tissue, though the half-time in the gill is not statistically significant. The distribution of 125I among various tissues in the flounder 6 days after the ingestion of labeled medaka once a day for 6 days differed from that of stable I, suggesting that the biological half-time is longer in certain tissues. Further study is necessary to elucidate the metabolism of radioiodine in the flounder.

In situ reductive dissolution to remove Iodine-129 from aquifer sediments.

The use of an aqueous reductant (Na-dithionite) with pH buffer (K-carbonate, pH 12) was evaluated in this laboratory study as a potential remedial approach for removing Fe oxide associated iodine and enhancing pump-and-treat extraction from iodine-contaminated sediments in the unconfined aquifer in the 200 West Area of the Hanford Site. X-ray fluorescence data of untreated sediment indicated that iodine was largely associated with Fe (i.e., potentially incorporated into Fe oxides), but XANES data was inconclusive as to valence state. During groundwater leaching, aqueous and adsorbed iodine was quickly released, then additional iodine was slowly released potentially from slow dissolution of one or more surface phases. The Na-dithionite treatment removed greater iodine mass (2.9x) at a faster rate (1-4 orders of magnitude) compared to leaching with groundwater alone. Iron extractions for untreated and treated sediments showed a decrease in Fe(III)-oxides, which likely released iodine to aqueous solution. Solid phase inorganic carbon and aqueous Ca and Mg analysis further confirmed that significant calcite dissolution did not occur in these experiments meaning these phases did not release significant iodine. Although it was expected that, after treatment, 127I concentrations would eventually be lower than untreated sediments, continued, elevated iodine concentrations for treated samples over 750 h were observed for leaching experiments. Stop flow events during 1-D column leaching suggested that some iodide precipitated within the first few pore volumes. Further, batch extraction experiments compared iodine-129/127 removal and showed that iodine-129 was more readily removed than iodine-127 suggesting that the two are present in different phases due to their different origins. Although significantly greater iodine is removed with treatment, the long-term leaching needs to be investigated further as it may limit dithionite treatment at the field scale.

129I in a sediment core offshore Fukushima: Distribution, source and its implication.

129I released from the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident has been observed in the atmospheric, terrestrial and oceanic environments, and it also entered the marine sediments via dispersion by sea water movement and deposition around Japan. However, there have been few studies of marine sediment cores in contrast to the large number of studies on seawater. In this work, a sediment core collected near FDNPP was analyzed for 129I. It is observed that the 129I/127I atomic ratios in this sediment core are comparable to those in the seawater and sediments collected from offshore Fukushima after the accident, but 2 orders of magnitude higher than those in seawater in this region before the accident, suggesting the significant amount of 129I has been transferred and incorporated to the offshore shallow sediments. The difference in environmental behavior between 129I and 137Cs is discussed based on their depth distributions in the sediment core in comparison with the grain size distribution of sediments. The peak concentrations of iodine isotopes were found in a relatively deeper layer than radiocesium. Radiocesium follows the distribution of fine grains in the sediment core, implying its high association to fine grains.