首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 46 毫秒
1.
Esaka F  Magara M  Suzuki D  Miyamoto Y  Lee CG  Kimura T 《Talanta》2010,83(2):569-573
Information on plutonium isotope ratios in individual particles is of great importance for nuclear safeguards, nuclear forensics and so on. Although secondary ion mass spectrometry (SIMS) is successfully utilized for the analysis of individual uranium particles, the isobaric interference of americium-241 to plutonium-241 makes difficult to obtain accurate isotope ratios in individual plutonium particles. In the present work, an analytical technique by a combination of chemical separation and inductively coupled plasma mass spectrometry (ICP-MS) is developed and applied to isotope ratio analysis of individual sub-micrometer plutonium particles. The ICP-MS results for individual plutonium particles prepared from a standard reference material (NBL SRM-947) indicate that the use of a desolvation system for sample introduction improves the precision of isotope ratios. In addition, the accuracy of the 241Pu/239Pu isotope ratio is much improved, owing to the chemical separation of plutonium and americium. In conclusion, the performance of the proposed ICP-MS technique is sufficient for the analysis of individual plutonium particles.  相似文献   

2.
We have developed an analytical method for detection of239Pu in aqueous samples at concentrations as low as 10–10M. This nuclear counting technique utilizes the uranium L X-rays, which follow the alpha-decay of plutonium. Because L X-rays are specific for the element and not for the individual isotope, the isotopic composition of the plutonium sample must be known. The counting efficiency in the 11–23 keV range is determined from a plutonium standard, and the concentration of the sample is then calculated from the L X-ray count and the isotopic composition. The total L X-ray count is corrected for possible contributions from other radionuclides present as impurities by measuring the low-energy gamma-spectrum for each contaminant to establish specific photon/X-ray ratios. The ratios are important when241Pu and242Pu are measured, because the respective decay chain members produce non-U L X-rays. This new method can replace the use of labor-intensive radiochemical separation techniques and elaborate activation methods for analysis of239Pu in aqueous samples. It is also applicable for assaying plutonium in liquid wastes that pose possible hazards to the environment.  相似文献   

3.
A gamma-spectrometric method using an intrinsic high resolution germanium detector has been developed for the determination of isotope ratios of plutonium from samples in solution form. The method is based on the assay of low energy gamma-rays of238Pu,239Pu,240Pu and241Pu and does not require the use of branching intensities or the knowledge of detection efficiencies for different gamma rays. Since low energy gamma-rays are used, the effect of241Am has also been studied. It is found that results are not affected up to 0.5 wt% of241Am in plutonium samples. An accuracy of 3% is achievable in the determination of240Pu/239Pu and241Pu/239Pu atom ratios as demonstrated by carrying out measurements on isotopic standards of plutonium.  相似文献   

4.
The origin and release date of environmental plutonium have been assessed by the measurement of plutonium and americium isotopic composition. The applicability and sensitivity of different plutonium isotope ratios, 240Pu/239Pu and 241Pu/239Pu measured by inductively coupled plasma sector field mass spectrometry and 238Pu/239Pu analysed by alpha spectrometry, have been evaluated for origin determination in several types of environmental samples. With use of mixing models the contribution of different sources (e.g. global fallout or Chernobyl) can be calculated. By the measurement of the 241Am/241Pu isotope ratio, the release date (i.e. formation of 241Pu by irradiation) can be estimated in environmental samples, which is an important parameter to distinguish recent plutonium release from previous (e.g. Chernobyl) emissions.  相似文献   

5.
In order to know the distribution of plutonium derived from the Nagasaki atomic bomb, soil samples were measured to determine the 240Pu/239Pu isotope ratio of and concentrations of 239+240Pu and 137Cs. The 239+240Pu concentrations in soils, except for Nishiyama area, were close to the average concentration of soil collected in Japan. In soils collected at the Nishiyama area and at the eastern area of Nagasaki Prefecture and at part of northern area in Kumamoto Prefecture, the 240Pu/239Pu ratios were lower than the global fallout values. This suggests that plutonium from the atomic bomb was deposited in the eastern area from the hypocenter reaching up to 100 km eastwards.  相似文献   

6.
There continue to be reports in the literature that suggest a difference in the behavior of239+240Pu and238Pu in some aquatic environments. Plutonium isotopes have been measured in marine samples collected over 3 decades from Enewetak atoll, one of the sites in the Marshall Islands used by the United States between 1946 and 1958 to test nuclear devices. The plutonium isotopes originated from a variety of complex sources and could possibly coexist in this environment as different physical-chemical species. However results indicate little difference in the mobility and biological availability of239+240Pu and238Pu.  相似文献   

7.
A method is described for the determination of plutonium concentration in the presence of a bulk of other impurities by isotope dilution mass spectrometry /IDMS/ using239Pu as a spike. The method involves the addition of239Pu spike / 90 atom%/ to samples with239Pu / 70 atom%/ and vice versa. After ensuring chemical exchange between the sample and the spike isotopes, plutonium is purified by conventional anion exchange procedure in 7M HNO3 medium.239Pu/240Pu atom ratio in the purified spiked sample is determined with high precision /better than 0.1%/ using a thermal ionization mass spectrometer. Concentration of plutonium in the sample is calculated from the changes in239Pu/240Pu atom ratio in the spiked mixture. Results obtained on different plutonium samples using239Pu as a spike are compared with those obtained by the use of242Pu spike. Precision and accuracy comparable to those achieved by using242Pu are demonstrated. The method provides an alternative in the event of non-availability of enriched242Pu or244Pu required in IDMS of plutonium and at the same time, offers certain advantages over the use of242Pu or244Pu spike.  相似文献   

8.
Analysis of plutonium isotopes by Semiconductor Alpha Spectrometry (SAS), ICP-sector field mass spectrometry (ICP-MS) and Accelerator Mass Spectrometry (AMS) was carried out in seawater samples collected from the Northeast Atlantic Ocean (nuclear waste dumping sites) and Northwest Pacific Ocean. No particularly elevated levels of the atom ratios of 240Pu/239Pu compared to global fallout ratio (0.18) were found in the Northeast Atlantic Ocean seawater samples. The higher levels of atom ratios of 240Pu/239Pu were found in the Northwest Pacific Ocean. This is mainly due to contribution from the local fallout from nuclear weapon tests carried out at the Pacific Proving Grounds at the Marshall Islands.  相似文献   

9.
Plutonium isotopes were measured by alpha-spectrometry and ICP-MS in sediment samples from two European lakes: Blelham Tarn in U.K. and Stechlin lake in Germany. The ICP-MS measurements were made after alpha-spectrometry counting of the planchets. The planchets were prepared by traditional electrodeposition method after radiochemical extraction, separation and purification of the Pu fraction. A short radiochemical separation using plutonium selective resin, between the two spectrometry measures, is presented. The results show that these two complementary methods are in good agreement, the plutonium activity concentrations are the same. Alpha-spectrometry allows the 238Pu determination and ICP-MS individual measurement of 239Pu and 240Pu. 238Pu/239+240Pu and 240Pu/239Pu ratios are calculated to determine the plutonium contamination source. With the results of these two techniques, it could be demonstrate that the plutonium is of global fallout origin.  相似文献   

10.
IAEA reference materials (radionuclides in the marine environment) collected in areas affected by nuclear reprocessing plants and nuclear weapons tests have been analysed by semiconductor alpha-spectrometry (SAS), liquid scintillation spectrometry (LSS) and mass spectrometric techniques (high resolution ICP-MS and AMS) with the aim of developing analytical procedures and to study the geochemical behavior of plutonium in the marine environment. The Pu results obtained by SAS, ICP-MS and AMS were in reasonably good agreement (R 2 = 0.99). The mean atom ratios of 240Pu/239Pu in IAEA reference materials, IAEA-134, 135 and 381 were (0.212±0.010), (0.211±0.004) and (0.242±0.004), respectively. IAEA-384 (Fangataufa Lagoon Sediment) gave a 240Pu/239Pu mean atom ratio of 0.051±0.001. The results of 241Pu obtained by ICP-MS and LSS also show reasonable agreement (R 2 = 0.91). Pu isotopic signatures were useful in tracing Pu origin and in interpreting biogeochemical processes involving Pu in the marine environment.  相似文献   

11.
A modified radiometric method for the determination of plutonium in irradiated nuclear fuel is described. The analysis consists of total plutonium alpha-activity, activity ratio238Pu:(239Pu+240Pu) and burnup determination. The error of plutonium determination is practically identical with that of a classical radiometric method. The method suggested is suitable for large sample series of the same type of irradiated nuclear fuel.  相似文献   

12.
Summary Studies on the environmental behavior of plutonium in the marine environment require an analytical method with high sensitivity and capability to provide the isotopic composition of Pu in marine samples. In this work, as part of our on-going project on Pu environmental behavior in the Pacific Ocean, a sector field ICP-MS method combined with an off-line anion-exchange chromatography system was optimized for the determination of Pu and its atomic ratio of 240Pu/239Pu in sediment core samples. Using a conical concentric nebulizer and 150-second counting time, we were able to lower the detection limit of Pu down to 0.35 fg. The mass discrimination effect was evaluated using a mixed Pu isotope standard solution with certified a 240Pu/239Pu isotope ratio (NBS-947). The overall performance of the analytical method was validated by the determination of Pu and its isotope composition in an ocean sediment reference material (IAEA-368). Both the 239+240Pu activity and 240Pu/239Pu atomic ratio were found to be in good agreement with the certified and/or literature values. As an important application, we employed the analytical method to investigate the vertical profiles of 239+240Pu activity and 240Pu/239Pu atomic ratio in sediment cores in the Sea of Okhotsk and the NW Pacific. It was found that the Bikini close-in fallout Pu could be transported as far as the Sea of Okhotsk. The results provided evidence to support our hypothesis on the oceanic current transportation of Bikini close-in fallout Pu in the NW Pacific and its marginal seas.  相似文献   

13.
In nuclear safeguards, precise and accurate isotopic analyses are needed for two major elements from the nuclear fuel cycle: uranium and plutonium. This can be achieved by Isotope Dilution Mass Spectrometry (IDMS), which is one of the most reliable analytical techniques for the determination of plutonium amount content to a high level of accuracy. In order to achieve reliable isotope measurements isotopic reference materials with certified amount of plutonium and isotopic composition are required. At the Institute for Reference Materials and Measurements (IRMM) various plutonium spike reference materials for isotopes 239Pu, 240Pu, 242Pu and 244Pu are available. This enabled the setup of an inter-calibration campaign inter-linking selected plutonium spikes on a metrological basis applying state-of-the-art measurement procedures. The aim of this campaign is threefold: firstly to perform measurements on selected plutonium spike isotopic reference materials for quality control purposes, secondly to verify the amount content and the isotopic composition of the recently produced IRMM-1027m large sized dried (LSD) spikes and thirdly to demonstrate IRMM’s measurement capabilities for plutonium analysis via external quality tools. The obtained results using various spike isotopic reference materials will be presented and discussed in this paper. The measurement uncertainties of the IDMS results were calculated according to the guide to the expression of uncertainty in measurement (GUM).  相似文献   

14.
Uranium (U) and plutonium (Pu) isotopes in coral soils, contaminated by nuclear weapons testing in the northern Marshall Islands, were isolated by ion-exchange chromatography and analyzed by mass spectrometry. The soil samples were spiked with 233U and 242Pu tracers, dissolved in minerals acids, and U and Pu isotopes isolated and purified on commercially available ion-exchange columns. The ion-exchange technique employed a TEVA® column coupled to a UTEVA® column. U and Pu isotope fractions were then further isolated using separate elution schemes, and the purified fractions containing U and Pu isotopes analyzed sequentially using multi-collector inductively coupled plasma mass spectrometer (MCICP-MS). High precision measurements of 234U/235U, 238U/235U, 236U/235U, and 240Pu/239Pu in soil samples were attained using the described methodology and instrumentation, and provide a basis for conducting more detailed assessments of the behavior and transfer of uranium and plutonium in the environment.  相似文献   

15.
The Standard Reference Material 4351 from the National Institute of Standards and Technology is acknowledged to be inhomogeneous. The value of a single analysis for239Pu+240Pu could lie within a wide range, but the accuracy of the analysis can be corroborated by comparing the corresponding238Pu/239Pu+240Pu or240Pu/239Pu values with the relationships between these ratios and the total plutonium concentration.  相似文献   

16.
A reverse isotope dilution alpha spectrometric /R-IDAS/ method using239Pu as a spike is described for the determination of plutonium concentration in high burn-up fuel samples wth238Pu/(239Pu+240Pu) alpha activity ratio >0.5, without resorting to any purification from241Am and a bulk of other impurities. It involves the addition of a pre-clibrated spike solution to a known aliquot of the plutonium sample solution followed by source preparation using TEG as a spreading agent. The results obtained on a number of plutonium samples containing 20–80% of241Am /alpha activity wise/ using this method are compared with those achieved by R-IDAS using purification with TTA, with respect to precision and accuracy. Precision and accuracy of 0.5% are demonstrated. This method eliminates the need of any separation and purification of plutonium from241Am and a bulk of other impurities like uranium.  相似文献   

17.
In the paper the results of 241Pu activity concentration determination in the biggest Polish rivers are presented. The analysis of more than 100 river water samples showed the Vistula and the Odra as well as three Pomeranian Rivers are important sources of 241Pu in the southern Baltic Sea. There were differences in 241Pu activities depending on season and sampling site and the plutonium contamination came mainly from the global atmospheric fallout as well as the Chernobyl accident, which is confirmed by plutonium activity ratios of 241Pu/239+240Pu and 238Pu/239+240Pu.  相似文献   

18.
Among the transuranic elements present in the environment, plutonium isotopes are mainly attached to particles, and therefore they present a great interest for the study and modelling of particle transport in the marine environment. Except in the close vicinity of industrial sources, plutonium concentration in marine sediments is very low (from 10−4 ng kg−1 for 241Pu to 10 ng kg−1 for 239Pu), and therefore the measurement of 238Pu, 239Pu, 240Pu, 241Pu and 242Pu in sediments at such concentration level requires the use of very sensitive techniques. Moreover, sediment matrix contains huge amounts of mineral species, uranium and organic substances that must be removed before the determination of plutonium isotopes. Hence, an efficient sample preparation step is necessary prior to analysis. Within this work, a chemical procedure for the extraction, purification and pre-concentration of plutonium from marine sediments prior to sector-field inductively coupled plasma mass spectrometry (SF-ICP-MS) analysis has been optimized. The analytical method developed yields a pre-concentrated solution of plutonium from which 238U and 241Am have been removed, and which is suitable for the direct and simultaneous measurement of 239Pu, 240Pu, 241Pu and 242Pu by SF-ICP-MS.  相似文献   

19.
Correlations have been established between %Eff 240Pu and various plutonium isotopes formed in thermal reactors. Based on these correlations, a method has been developed for the estimation of isotopic composition of plutonium obtained from thermal reactors. The method is simple, fast, non-destructive and finds application for the verification of plutonium isotopic composition in the finished products of known plutonium content. The method could be applied in the nuclear fuel fabrication to verify and confirm the fissile content (239Pu+241Pu) specification. It has also been shown that in principle, similar correlations could be established for Pu obtained from different thermal reactor fuels with reactor specific fitting parameters.  相似文献   

20.
Half-life of241Pu is of great importance in nuclear technology. In view of large variation in the values (13–15 y) reported till 1974 in literature, efforts have been made in different laboratories to determine this half-life with high precision and accuracy. In our laboratory, it has been determined by different methods which may be classified in two categories, viz. (1) parent decay method, and (2) daughter growth method. In the parent decay method, change in isotope ratios241Pu/239Pu,241Pu/240Pu and241Pu/242Pu was studied periodically by a thermal ionization mass spectrometer. Single as well as double ratio method was used to calculate the half-life. In the daughter growth method, the half-life was obtained in four independent ways. These were (1) alpha spectrometry taking239Pu and242Pu separately as reference isotopes and studying periodically the increase in alpha activity ratio, (2) alpha proportional counting for observing periodically the change in total alpha activity, (3) isotope dilution alpha spectrometry using243Am as a spike, (4) isotope dilution mass spectrometry using243Am as a spike. In all these methods, synthetic mixtures were prepared for achieving high precision and accuracy in different measurements. Based on the results obtained in this laboratory and the values reported by other laboratories, a half-life value of 14.4±0.1 y is recommended. The paper reviews the past history, puts forth the present status, highlights the current trends for studying the effect of chemical composition of plutonium on the half-life of241Pu and presents the future requirements for achieving higher accuracy in the half-life of241Pu.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号