RESUMO
This study established specialized radiation dose models to evaluate the internal radiation doses derived from 137Cs and 134Cs in fishes in the port of the Fukushima Daiichi Nuclear Power Plant from 2012 to 2023. By August 2018, the activities of 134Cs and 137Cs in fishes decreased at the T1/2 of 176 d and 191 d, respectively. The corresponding mass concentrations were far lower than 1 mg/kg and the chemical toxicity can be negligible. Regarding radiotoxicity, 18,000 Bq/kgfresh weight of 134Cs and 137Cs in grouper Sebastes schlegelii produced 276 µGy/h of radiation dose, which was below the no-effect-dose-rate benchmarks (400 µGy/h). 740,000 Bq/kgfresh weight of 134Cs and 137Cs in greenling Hexagrammos otakii produced 12,600 µGy/h of radiation dose, which was much higher than 400 µGy/h, indicating the possibility of radiation effects. If a person eats these two reported fishes, the resulting committed effective doses for humans are 7.7 µSv and 6.31 mSv, respectively.
Assuntos
Radioisótopos de Césio , Peixes , Acidente Nuclear de Fukushima , Centrais Nucleares , Monitoramento de Radiação , Poluentes Radioativos da Água , Animais , Radioisótopos de Césio/análise , Poluentes Radioativos da Água/análise , Japão , Doses de RadiaçãoRESUMO
Based on the monitoring data of 137Cs and 90Sr in Tian Bay in 2005-2023, the impacts of the operation of Tianwan Nuclear Power Plant on the marine ecosystem were assessed. The 137Cs and 90Sr activity concentrations in the seawater and sediment varied within the background ranges. The radiation dose rates derived from 137Cs and 90Sr for the marine organisms ranged from 2.4 × 10-5 to 2.2 × 10-4 nGy/h, it was far below the most conservative screening dose rate (10 µGy/h). The committed effective dose for humans was 0.070-0.094 µSv, 1/1500th of the world's mean annual effective dose (0.12 mSv) from ingesting food containing uranium and thorium series nuclides. Radiation risk assessment showed no radiation risk for the long-term discharge of nuclear wastes in the future. Overall, the long-term normal operation of TNPPs has almost no radiation impact on the adjacent marine ecosystem.
Assuntos
Organismos Aquáticos , Radioisótopos de Césio , Ecossistema , Centrais Nucleares , Monitoramento de Radiação , Água do Mar , Poluentes Radioativos da Água , Poluentes Radioativos da Água/análise , Radioisótopos de Césio/análise , Água do Mar/química , China , Sedimentos Geológicos/química , Medição de RiscoRESUMO
The Fukushima Daiichi Nuclear Power Plant (FDNPP) has generated quantities of polluted water since the accident in 2011 triggered by the massive earthquake. In order to understand the FDNPP accident comprehensively and to provide a basic reference for predicting the transport of the treated nuclear contaminated water in the Northwest Pacific further, the distributions of 137Cs and 134Cs in the seawater as deep as 2000 m were determined in the subtropical region in May 2013. The results suggested that the radiocesium from FDNPP still existed in May 2013. But no FDNPP-derived radiocesium was found below 1000 m layer. The FDNPP accident contributed 0.46 PBq of 137Cs to the upper 500 m of water column, which was â¼1.6 times of the background amount of 137Cs (0.28 PBq). The maximum activities of 137Cs and 134Cs were 7.88 Bq/m3 and 3.40 Bq/m3, respectively. It is mainly because of the Subtropical Mode Water (STMW) that carried 137Cs and 134Cs to the subtropical region along the subsurface isopycnals (25.0-25.6 δθ). As time went on, more FDNPP-derived radiocesiums were transported to the subtropical region and to the subsurface layer by the STMW than ever. The cyclonic mesoscale eddy further promoted more radiocesiums downward transport and deeper penetration on the basis of the subduction of STMW. However, the formation of the vertical stratification and the presence of the low salinity water mass (at the depth of â¼500-â¼700 m) restrained the penetration of the radiocesium into deeper and interior ocean and thus the FDNPP-derived 137Cs and 134Cs in the subtropical area mainly distributed in the upper 500 m layer.
Assuntos
Acidente Nuclear de Fukushima , Monitoramento de Radiação , Poluentes Radioativos da Água , Oceano Pacífico , Poluentes Radioativos da Água/análise , Monitoramento de Radiação/métodos , Água do Mar , Radioisótopos de Césio/análise , Água , JapãoRESUMO
Based on the monitoring data of Daya Bay in 2011-2017, the impact of long-term operation of nuclear power plants (NPPs) on the marine ecosystem was accessed. 137Cs and 90Sr in seawater and sediment of Daya Bay decreased with time. The environmental half-lives of 137Cs and 90Sr in seawater, 137Cs in sediment were 7.1 a, 11.7 a and 13.9 a, respectively. The total dose rates of the marine organisms ranged from 230.5 to 853.9 nGy/h, lower than the ERICA screening benchmark (10 µGy/h). 210Po, 226Ra and 232Th were the main dose contributors. 137Cs and 90Sr contributed to ~0.01 %-~0.06 % of the total radiation. 137Cs contributed to <0.6 of the committed effective dose for humans. There were almost no radiation effects on the marine ecosystem of Daya Bay from NPPs before 2017. In the future, there will be no radiation risk for the long-term discharge of low-level radioactive waste to Daya Bay.
Assuntos
Ecossistema , Centrais Nucleares , Humanos , Baías , China , Monitoramento AmbientalRESUMO
The source and vertical distribution of 137Cs,239+240Pu and 241Am activity concentrations in a soil core from Hunan Province, China were investigated. The maximum 137Cs and 239+240Pu activity concentrations were 15.45 ± 0.76 mBq/g and 0.819 ± 0.066 mBq/g, respectively. While the maximum 241Am activity concentration in samples obtained from the core was 0.341 ± 0.019 mBq/g. The 240Pu/239Pu atom ratio and the 137Cs/239+240Pu activity ratio were 0.183 ± 0.011 and 19.5 ± 1.8, respectively, and both were consistent with the characteristic value of global fallout. The integrated 241Am/239+240Pu activity ratio for global fallout was also re-estimated. The measured 241Am/239+240Pu activity ratio (average 0.43 ± 0.07) in the samples was very close to the estimated value (0.45), which suggested their 241Am also came from the global fallout. Regarding the vertical distribution of 137Cs, 239+240Pu and 241Am in these red soil samples, all these radionuclides had higher concentrations in upper layers of several centimeters of soil while they had slightly lower concentrations in lower soil layers down to 30 cm. Vertical distributions of 137Cs/239+240Pu and 241Am/239+240Pu activity ratios indicated the migration velocity was Am ≈ Pu > Cs. The intrinsic chemical properties of the radionuclides as well as soil type and properties (acidic, nutrient-deficient and low in organic matter and cation exchange capacity) might be reasons for the differences in their migration behaviors.
Assuntos
Plutônio , Monitoramento de Radiação , Poluentes Radioativos do Solo , Amerício , Radioisótopos de Césio/análise , China , Plutônio/análise , Solo , Poluentes Radioativos do Solo/análiseRESUMO
Mangrove forests are valuable intertidal ecosystems that provide coastline protection, biodiversity maintenance, and carbon sequestration. However, their survival is under severe threat from rapidly rising sea levels. In this study, we aimed to investigate the changes in the area of the Dongzhaigang mangrove in China since the 1950s and causes of these changes using literature and remote sensing data. The impact of historical and future sea level rise (SLR) on the mangroves was analyzed using remote sensing data and climate model data under the low, intermediate, and very high greenhouse gas emission scenarios (Representative Concentration Pathways (RCPs) 2.6, 4.5, and 8.5). The area of the mangrove forests decreased from 3416 to 1711 hm2 during 1956-1988 and remained constant at 1711 hm2 after the 1990s, owing to anthropogenic disturbances such as reclamation and aquaculture before the 1980s and the protection of nature reserve establishment after the 1990s, respectively. Under RCPs 4.5 and 8.5, SLR is expected to cause > 26% of the mangroves to disappear by 2100, whereas under RCP 2.6, only 17% of the mangroves will likely be lost. Biological measures such as reestablishment of ponds as mangrove forests, afforestation, and biological embankment for sediment trapping in coastal wetlands are recommended to enhance the resilience of mangroves to SLR.
Assuntos
Ecossistema , Elevação do Nível do Mar , Sequestro de Carbono , China , Áreas AlagadasRESUMO
To understand the possible influence of the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident on the deep sea, as well as the geochemical behavior and transport of radionuclides, 134Cs, 137Cs, 239, 240Pu, 241Pu, and 237Np were measured in the abyssal sediments of the Northwest Pacific (NWP) and Central Equatorial Pacific (CEP) Ocean. Data on the characteristics of these sediments obtained after the FDNPP accident are extremely rare, especially in the NWP subtropical gyre (NPSG) region. FDNPP-derived radio-Cs (134Cs, 137Cs) arrived at the open sea floor of the NWP before 2018 but was only found in the Kuroshio-Oyashio Extension (KOE) region. No FDNPP-derived Pu was detected in the abyssal sediments of the NWP or CEP. Pu in the NWP mainly originated from global fallout and the Pacific Proving Ground (PPG) close-in fallout, except for at station WP1 (39°N in the KOE region), where an abnormal but non-FDNPP-derived Pu signal was detected. Pu in the eastern CEP sediment was less affected by the PPG close-in fallout from the Marshall Islands and was mainly derived from global fallout, with some close-in fallout from the Johnston Atoll test. The KOE region was the area most affected by PPG close-in fallout Pu via Kuroshio transport, while the lowest inventories of 239+240Pu and 237Np were found in the NPSG region due to its oligotrophic environment. The 237Np originated from the same source as Pu, and the latitudinal pattern of 237Np was consistent with that of Pu. Station SS (in the marginal sea of the NWP) contained high 237Np/239Pu atom ratios in the deeper layers of sediment and had a 237Np depth profile opposite that of the 239+240Pu profile, compared to other stations; these differences are mainly attributed to differences in the behaviors of 237Np and 239Pu.
Assuntos
Acidente Nuclear de Fukushima , Plutônio , Monitoramento de Radiação , Poluentes Radioativos da Água , Radioisótopos de Césio/análise , Japão , Plutônio/análise , Poluentes Radioativos da Água/análiseRESUMO
To understand the transport of Fukushima Dai-ichi Nuclear Power Plant Accident (FDNPPA)-derived nuclear contaminated water, which will be discharged into the Pacific Ocean in the future, the distributions of 134Cs and 137Cs in seawater in the public areas east of Japan in winter 2011 were reported in this study. The ranges of 134Cs and 137Cs activities were Assuntos
Acidente Nuclear de Fukushima
, Monitoramento de Radiação
, Poluentes Radioativos da Água
, Radioisótopos de Césio/análise
, Japão
, Centrais Nucleares
, Oceano Pacífico
, Poluentes Radioativos da Água/análise
RESUMO
To investigate the potential long-term impact of the Fukushima Dai-ichi Nuclear Power Plant Accident (FDNPPA) on the South China Sea (SCS) and the East China Sea (ECS), radiocesium isotopes 134Cs and 137Cs in seawater from 2011 to 2015 were measured. The highest activities of 134Cs and 137Cs in seawater were 0.73 Bq/m3 and 3.34 Bq/m3, respectively. The results demonstrated that FDNPPA-derived radiocesium intruded into the Northeast SCS and the ECS in 2013 and reached a maximum in 2014. The intrusion occurred within the upper 100 m and contributed ≤72.5% of the total 137Cs in the seawater of the SCS and ECS. The formation, subduction, and transport of subtropical mode water (STMW)/central mode water (CMW) trapped FDNPPA-derived radiocesium in the ocean interior and transported it southwestward from the high-latitude open ocean to the low-latitude western boundary area. Then, the FDNPPA-derived radiocesium entered the Northeast SCS and the ECS by the intrusion of the subsurface high-salinity water of the Kuroshio Current into the Northeast SCS and the ECS.
Assuntos
Acidente Nuclear de Fukushima , Monitoramento de Radiação , Poluentes Radioativos da Água , Radioisótopos de Césio/análise , China , Japão , Monitoramento de Radiação/métodos , Água do Mar , Poluentes Radioativos da Água/análiseRESUMO
The Japanese government approved a plan to discharge Fukushima Daiichi Nuclear Power Plant Accident contaminated water (FDNPPACW) into the Pacific Ocean. It immediately caused a new wave of global concern and anxiety. To assess this matter, this work briefly reviewed the dispersion of FDNPPA-derived radionuclides in the Pacific Ocean in the past and the resulting impacts on marine biota. Combining the drafted plan of discharging FDNPPACW and the public's concerns, 5 points, including (1) the detailed plan of discharging FDNPPACW, (2) the isotopes left in the advanced liquid processing system (ALPS)-treated water and their amounts, (3) the stability of the Kuroshio Extension, (4) the fates and transports of the main radionuclides (left in the ALPS-treated water) in North Pacific seawater, (5) and bioaccumulations and the ecological half-lives of the main radionuclides (left in the ALPS-treated water) in marine biota in the North Pacific, remain to be known to understand the impacts of discharging FDNPPACW into the Pacific Ocean.
Assuntos
Acidente Nuclear de Fukushima , Monitoramento de Radiação , Poluentes Radioativos da Água , Radioisótopos de Césio/análise , Japão , Centrais Nucleares , Oceano Pacífico , Água , Poluentes Radioativos da Água/análiseRESUMO
The Fukushima Dai-ichi Nuclear Power Plant Accident (FDNPPA) derived 134Cs, 137Cs and 110mAg in blue sharks captured in the Northwest Pacific during 2011-2018 were assessed for the first time in the aspects of radioactive contamination, temporal variation, maternal-to-fetus transfer, tissue distribution and radiation dose, to demonstrate the impacts of the FDNPPA on blue sharks. The contribution of the FDNPPA derived radiocesium in blue sharks (>52%) was estimated based on 134Cs/137Csactivity ratios. The effective and ecological half-lives of the FDNPPA derived 134Cs (270 d, 410 d), and 137Cs (430 d, 450 d) were calculated. These contaminations decreased with time and returned to the level before the FDNPPA during the period of Sep. 2017-Sep. 2018.134Cs and 137Cs tended to distribute in muscles, while 110mAg mainly distribute in their guts. 134Cs and 137Cs were also transferred to fetuses and the activities were up to ~30% of the maternal activities. Dose assessment demonstrated that the highest FDNPPA derived dose rate in blue sharks (~0.42 nGy/h) was far below the ERICA ecosystem screening benchmark of 10 µGy/h and the committed effective dose in humans from ingesting blue shark meat (0.06-0.90 µSv) was far less than that from annual consumption of food and water. It was far from causing radiation harm to blue sharks and humans, suggesting that the impacts of the FDNPPA on blue sharks were not significant.
Assuntos
Acidente Nuclear de Fukushima , Monitoramento de Radiação , Tubarões , Poluentes Radioativos da Água , Animais , Radioisótopos de Césio/análise , Ecossistema , Humanos , Japão , Centrais Nucleares , Poluentes Radioativos da Água/análiseRESUMO
Ten sets of experiments with different settling times were conducted to investigate the effect of settling time on the adsorption of 137Cs in seawater onto ammonium phosphomolybdate (AMP). The weight yields of AMP and 137Cs yields in all groups were generally higher than 90%. The average weight yields of AMP in each group varied from 91.8 ± 0.5 to 95.9 ± 0.6% (1 SD), and the average 137Cs yields in each group varied from 88.3 ± 3.0 to 97.8 ± 3.7% (1 SD). The results showed that equilibrium between Cs and AMP is established immediately after the addition of stable Cs carrier and AMP, implying that the solution could be filtered immediately after the coprecipitation forms. IAEA seawater proficiency test exercises also confirmed that the AMP precipitate does not need to be treated statically in the case of 2 g AMP and 3.7 mg Cs carrier in a seawater sample solution. The modified AMP preconcentration method simultaneously meets the requirements of routine and nuclear emergency monitoring of 137Cs in seawater.
Assuntos
Compostos de Amônio , Monofosfato de Adenosina , Adsorção , Radioisótopos de Césio , Molibdênio , Ácidos FosfóricosRESUMO
More than 9 years since the Fukushima Dai-ichi Nuclear Power Plant Accident (FDNPPA), the impact of FDNPPA on marine biota is being revealed. In this work, the evolution of FDNPPA derived 134Cs, 137Cs and 110mAg in dolphin fishes (Coryphaena hippurus) in the Northwest Pacific from Dec. 2011 to Sept. 2018 were studied. Bioconcentration factors (BCF) of radiocesium (29-69 with the average of 48) in dolphin fishes were calculated. The background level of 137Cs in dolphin fishes (<0.14 Bq/kgfresh weight) before FDNPPA was estimated. The radioactive levels of these three radionuclides in dolphin fishes decreased with time. Among them, 134Cs and 110mAg decreased at the half-lives of 158 days and 54 days at the population level, respectively. After May 2014, 134Cs and 110mAg cannot be detected and the activity of 137Cs returned to the background level before FDNPPA. Radiation dose assessment demonstrated that it was far from causing radiation harm to dolphin fishes in the open ocean of Northwest Pacific and humans who ingested them.
Assuntos
Peixes/metabolismo , Acidente Nuclear de Fukushima , Monitoramento de Radiação , Poluentes Radioativos da Água/metabolismo , Animais , Radioisótopos de Césio , Humanos , Japão , Centrais Nucleares , Radioatividade , Poluentes Radioativos da Água/análiseRESUMO
Following nine years since the Fukushima Dai-ichi Nuclear Power Plant Acciden (FDNPPA), it might be the time to draw a much clearer conclusion for the impact of FDNPPA on marine biota. In this work, the evolution of the FDNPPA derived 134Cs, 137Cs and 110mAg in the neon flying squids in the Northwest Pacific from 2011 to 2018 were studied. The background level of 137Cs in neon flying squids (<0.10 Bq/kgfresh weight with the average of 0.017 Bq/kgfresh weight) before FDNPPA were estimated. The radioactive levels of 134Cs, 137Cs and 110mAg in neon flying squids decreased with time. 134Cs and 110mAg decreased at the half-lives of 7.6 months and 5.7 months at the population level, respectively. After May 2014, 134Cs and 110mAg cannot be detected and 137Cs activities returned to the background level before FDNPPA. BCFs of cesium isotopes (3.7-17.7 with the average of 10.8) and 110mAg (â¼7 × 104) for neon flying squids were estimated. The amount of 110mAg released into the Northwest Pacific (â¼20-â¼26 TBq) were firstly calculated using a 134Cs/110mAgactivity ratio method. Radiation dose assessment demonstrated that it was far from causing radiation harm to neon flying squids in the open ocean of Northwest Pacific and humans who ingested these neon flying squids.
Assuntos
Acidente Nuclear de Fukushima , Monitoramento de Radiação , Poluentes Radioativos da Água/análise , Animais , Radioisótopos de Césio/análise , Decapodiformes , Humanos , Japão , Neônio , Centrais NuclearesRESUMO
The marine environment is complex, and it is desirable to have measurements for seawater samples collected at the early stage after the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident to determine the impact of Fukushima-derived radionuclides on this environment. Here Pu isotopes in seawater collected 33-163â¯km from the FDNPP site at the very early stage after the accident were determined (May 2011, within two months after the accident). The distribution and temporal variation of 239Pu and 240Pu were studied. The results indicated that both 239+240Pu activity concentrations (from 0.81⯱â¯0.16 to 11.18⯱â¯1.28 mBq/m3) and 240Pu/239Pu atom ratios (from 0.216⯱â¯0.032 to 0.308⯱â¯0.036) in these seawater samples were within the corresponding background ranges before the accident, and this suggested that Fukushima-derived Pu isotopes, if any, were in too limited amount to be distinguished from the background level in the seawater. The analysis of Pu isotopic composition indicated that the major sources of Pu in the seawater after the accident were still global fallout and the Pacific Proving Ground close-in fallout. The contribution analysis showed that the contributions of the Pacific Proving Ground close-in fallout in the water column of the study area ranged from 26% to 77% with the average being 48%.
Assuntos
Acidente Nuclear de Fukushima , Plutônio/análise , Monitoramento de Radiação , Radioisótopos/análise , Água do Mar/análise , Poluentes Radioativos da Água/análise , JapãoRESUMO
In order to assess the impact of the Fukushima derived Pu isotopes on seawater, a new analytical method to rapidly determine Pu isotopes in seawater by SF-ICP-MS including Fe(OH)2 primary co-precipitation, CaF2/LaF3 secondary co-precipitation and TEVA+UTEVA+DGA extraction chromatographic separation was established. High concentration efficiency (~100%) and high U decontamination factor (~107) were achieved. The plutonium chemical recoveries were 74-88% with the mean of 83 ± 5%. The precisions for both 240Pu/239Pu atom ratios and 239+240Pu activity concentrations were less than 5% when 15 L of seawater samples with the typical 239+240Pu activity of the Northwest Pacific were measured. It just needs 12 hours to determine plutonium using this new method. The limit of detection (LOD) for 239Pu and 240Pu were both 0.08 fg/mL, corresponding to 0.01 mBq/m3 for 239Pu and 0.05 mBq/m3 for 240Pu when a 15 L volume of seawater was measured. This method was applied to determine the seawater samples collected 446-1316 km off the FDNPP accident site in the Northwest Pacific in July of 2013. The obtained 239+240Pu activity concentrations of 1.21-2.19 mBq/m3 and the 240Pu/239Pu atom ratios of 0.198-0.322 suggested that there was no significant Pu contamination from the accident to the Northwest Pacific.
Assuntos
Técnicas de Química Analítica/métodos , Isótopos/química , Plutônio/química , Água do Mar/análise , Poluentes Radioativos da Água/química , Fluoretos/química , Acidente Nuclear de Fukushima , Lantânio/química , Limite de Detecção , Monitoramento de Radiação/métodosRESUMO
A rapid method with enhanced 238U decontamination was developed for ultra-trace Pu analysis in small-volume urine bioassays. This method consists of acid digestion, co-precipitation, extraction chromatography and sector-field inductively coupled plasma mass spectrometry (SF-ICP-MS) measurement. Parameters that may influence the analytical performance were studied systematically. This method achieved a high 238U decontamination factor (3.8â¯×â¯106) and the 242Pu recovery was stable for 20â¯mL and 100â¯mL urine bioassays with an average value of 72.7⯱â¯5.5%. The limits of detection for 239Pu, 240Pu and 241Pu by the method were 0.016â¯fgâ¯mL-1, 0.016â¯fgâ¯mL-1 and 0.019â¯fgâ¯mL-1 for 20â¯mL urine samples and 0.003â¯fgâ¯mL-1, 0.002â¯fgâ¯mL-1 and 0.003â¯fgâ¯mL-1 for 100â¯mL urine samples, respectively. Considering the small volume of urine employed in this study, the absolute detection limits of the method were comparable or even better than those measured with thermal ionization mass spectrometry and accelerator mass spectrometry. All procedures for 20â¯mL and 100â¯mL urine bioassays were completed in 9.5â¯h and 11â¯h, respectively, and analysis of 10 samples could be finished within one day. With the considerably low detection limits of Pu isotopes and high sample throughput, this method would be a promising tool for the quick response to radiological emergencies and for rapid screening of unexpected occupational exposures of workers involved in the future FDNPP reactor decommissioning operations.
Assuntos
Espectrometria de Massas , Plutônio/urina , Bioensaio , Humanos , Espectrometria de Massas/métodosRESUMO
This study investigated the radioactive impacts on 10 nekton species in the Northwest Pacific more than one year after the Fukushima Nuclear Accident (FNA) from the two perspectives of contamination and harm. Squids were especially used for the spatial and temporal comparisons to demonstrate the impacts from the FNA. The radiation doses to nekton species and humans were assessed to link this radioactivity contamination to possible harm. The total dose rates to nektons were lower than the ERICA ecosystem screening benchmark of 10µGy/h. Further dose-contribution analysis showed that the internal doses from the naturally occurring nuclide 210Po were the main dose contributor. The dose rates from 134Cs, 137Cs, 90Sr and 110mAg were approximately three or four orders of magnitude lower than those from naturally occurring radionuclides. The 210Po-derived dose was also the main contributor of the total human dose from immersion in the seawater and the ingestion of nekton species. The human doses from anthropogenic radionuclides were ~ 100 to ~ 10,000 times lower than the doses from naturally occurring radionuclides. A morbidity assessment was performed based on the Linear No Threshold assumptions of exposure and showed 7 additional cancer cases per 100,000,000 similarly exposed people. Taken together, there is no need for concern regarding the radioactive harm in the open ocean area of the Northwest Pacific.
Assuntos
Organismos Aquáticos/efeitos da radiação , Acidente Nuclear de Fukushima , Monitoramento de Radiação/métodos , Radioisótopos/análise , Água do Mar/química , Poluentes Radioativos da Água/análise , Animais , Organismos Aquáticos/química , Decapodiformes/efeitos da radiação , Relação Dose-Resposta à Radiação , Peixes , Humanos , Doses de RadiaçãoRESUMO
Plutonium is extensively studied in radioecology (e.g., soil to plant transfer and radiological assessment) and geochemistry (e.g., sediment dating). Here, we reported a new chemical separation method for rapid determination of Pu in soil and sediment samples, based on the following investigations: extraction behaviors of interfering elements (IEs, for inductively coupled plasma mass spectrometry (ICPMS) measurement) on TEVA resin; decontamination of U using TEVA, UTEVA, and DGA resins; and the impact of coprecipitation on Pu determination. The developed method consists of four steps: HNO3 leaching for Pu release; CaF2/LaF3 coprecipitation for the removal of major metals and U; the proposed TEVA + UTEVA + DGA procedure for the removal of U, Pb, Bi, Tl, Hg, Hf, Pt, and Dy; and ICPMS measurement. The accuracy of this method in determining 239+240Pu activity and 240Pu/239Pu and 241Pu/239Pu isotopic ratios was validated by analyzing five standard reference materials (soil, fresh water sediment, and ocean sediment). This method is characterized by its stable and high Pu recovery (90-97% for soil; 92-98% for sediment) and high decontamination factor of U (1.6 × 107), which is the highest reported for soil and sediment samples. In addition, the short analytical time of 12 h and the method detection limits, which are the lowest yet reported in literature, of 0.56 µBq g-1 (0.24 fg g-1) for 239Pu, 1.2 µBq g-1 (0.14 fg g-1) for 240Pu, and 0.34 mBq g-1 (0.09 fg g-1) for 241Pu (calculated on the basis of a 1 g soil sample) allow the rapid determination of ultratrace level Pu in soil and sediment samples.