低水平放射性废水中钚的分析方法研究进展

钚是重要的核燃料,也是一种极毒的放射性核素,在核燃料循环和放射性废物处置过程中占有重要地位.近些年来,钚在自然水体中的含量、分布引起人们的关注.科研工作者针对低水平放射性废水,核设施周围自然水体,核试验、核事故情况下可能污染的自然水体等,建立了一些钚的分析方法.作者在对这些方法进行了比较的基础上,提出了一种在盐酸体系中用TEVA树脂负压微色谱柱液闪法将水溶液中钚与其他锕系元素及金属离子分离并测量的新方法.该方法有望在日常和应急监测中的得到应用.     

Americium,plutonium and uranium contamination and speciation in well waters,streams and atomic lakes in the Sarzhal region of the Semipalatinsk Nuclear Test Site,Kazakhstan

New data are reported on the concentrations, isotopic composition and speciation of americium, plutonium and uranium in surface and ground waters in the Sarzhal region of the Semipalatinsk Test Site, and an adjacent area including the settlement of Sarzhal. The data relate to filtered water and suspended particulate from (a) streams originating in the Degelen Mountains, (b) the Tel′kem 1 and Tel′kem 2 atomic craters, and (c) wells on farms located within the study area and at Sarzhal. The measurements show that ²⁴¹Am, ^239,240Pu and ²³⁸U concentrations in well waters within the study area are in the range 0.04–87 mBq dm⁻³, 0.7–99 mBq dm⁻³, and 74–213 mBq dm⁻³, respectively, and for ²⁴¹Am and ^239,240Pu are elevated above the levels expected solely on the basis of global fallout. Concentrations in streams sourced in the Degelen Mountains are similar, while concentrations in the two water-filled atomic craters are somewhat higher. Suspended particulate concentrations in well waters vary considerably, though median values are very low, at 0.01 mBq dm⁻³, 0.08 mBq dm⁻³ and 0.32 mBq dm⁻³ for ²⁴¹Am, ^239,240Pu and ²³⁸U, respectively. The ²³⁵U/²³⁸U isotopic ratio in almost all well and stream waters is slightly elevated above the ‘best estimate’ value for natural uranium worldwide, suggesting that some of the uranium in these waters is of test-site provenance. Redox analysis shows that on average most of the plutonium present in the microfiltered fraction of these waters is in a chemically reduced form (mean 69%; 95% confidence interval 53–85%). In the case of the atomic craters, the proportion is even higher. As expected, all of the americium present appears to be in a reduced form. Calculations suggest that annual committed effective doses to individual adults arising from the daily ingestion of these well waters are in the range 11–42 μSv (mean 21 μSv). Presently, the ground water feeding these wells would not appear to be contaminated with radioactivity from past underground testing in the Degelen Mountains or from the Tel′kem explosions.     

Radioactive Isotopes of Strontium, Caesium and Plutonium in Sediments of the Northern Adriatic Sea

Sediment samples of different strata (0-3 and 12-15 cm) were collected between 1990 and 1992 during seasonal cruises in the Northern Adriatic Sea. A complete mapping of the Sr-90, Cs-137, Pu-238 and Pu-239(240) concentrations was obtained for samples covering a wide area, stretching from the Gulf of Trieste towards the Ancona shoreline. Sr-90 concentrations varied between 1.5 and 6.5 Bq kg^-1 dw, Cs-137 was in the range 0.9-38.9 Bq kg^-1 dw, Pu-239(240) in the range 0.08-1.5 Bq kg^-1 dw and Pu-238 around 0.03 Bq kg^-1 dw. Special reference was also put on the comparison between the off-shore environment and data obtained from samples collected inside the Po river delta. in spite of the major accumulation of Cs-137 inside the estuarine environment, higher concentrations of strontium and plutonium isotopes were detected in the offshore environment.     

Speciation and the bioavailability of actinide elements

A good understanding of the quantitative uptake of actinide elements from foodstuffs, across the mucosal cell membranes of the gastrointestinal tract, into man is of great importance in setting intake limits and in assessing radiation doses to critical organs.

In the past, such knowledge has been gained from the extrapolation of animal models to man. Whilst this strategy has proved useful in a number of cases, it is, unfortunately, phenomenological and the results prone to perturbation from factors such as the fasting state of the animal and the initial chemical form of the actinide.

The application of computer simulation models which can calculate the chemical speciation of an element in a variety of foodstuffs under conditions pertinent to the gastrointestinal tract offers a non‐invasive and general method for predicting the uptake of exogenous elements, like the actinides.

This paper reviews the current state of chemical speciation analysis with respect to bioavailability highlighting areas requiring further consideration, presenting results amplifying the issues raised and showing that computer simulation has a rôle to play in predicting quantitative uptake of the actinides.     

土壤和沉积物中钚同位素组成的质谱分析方法

钚-238是一种半衰期较长的人为放射性核素,其含量极低,准确分析其同位素组成依赖于高效率的分离富集技术及高灵敏度的检测技术。本文综述了电感耦合等离子、电子加速、热电离和共振电离四种质谱分析方法在土壤和沉积物中钚同位素分析方面的应用现状,从技术原理、应用和成本等方面对比分析了各种分离和纯化方法、质谱检测方法的优势与不足,为钚同位素的地球化学应用及我国核能应用过程环境影响评估提供技术支持。     

Pu在处置库地下水中的种态模拟及影响特征

采用PHREEQC对Pu在西南某低放废物处置库、甘肃北山高放处置库五一检测井和三号井地下水中的种态及影响进行对比分析,并探讨了pH、pE和离子浓度对Pu在地下水溶液中的影响分布。结果表明:Pu在地下水中主要以Ⅳ价的Pu(OH)_4和Pu(OH)_3~+为主,其次有少量Ⅴ价的PuO_2~+存在。pE和pH对Pu在地下水中的种态存在影响较大,强酸环境中溶液主要以Pu(Ⅲ)存在,中性及碱性环境中,溶液主要以Pu(Ⅳ)存在。离子浓度对Pu在地下水中的种态有一定影响,主要原因是CO_3~(2-)和SO_4~(2-)易与Pu结合形成新的络合物。因此,放射性废物处置库选址与安全评价工作等需要充分考虑周边地下水溶液的离子浓度、pH和pE等影响因素。     

Some characteristics of plutonium distribution in the atmospheric air and plants in the zone surrounding the Mayak Production Association

The results of long-term studies on plutonium distribution in the atmospheric air and plants in the area surrounding the Mayak Production Association in the years 1976–1995 are summarized. Data are presented on the changes in plutonium concentration in the air overtime at some points located in the survey zone and the impact zone of the industrial enterprise as compared to those in the control region. In addition, data on the changes in air plutonium concentration depending on the season and direction of wind are presented; the ratios between plutonium concentrations in the air and the fallout are analyzed.Translated from Ekologiya, No. 1, 2005, pp. 20–25.Original Russian Text Copyright © 2005 by Chudin, Shcherbakova, Maslovskii, Kocheva, Iovlev, Denisenko, Demin, Mamin, Chebotina.     

Vertical Distribution and Inventories of 239,240Pu in Deep Sea Sediments of the Mediterranean Sea (Algerian Basin, Ionian Sea)

Deep-sea sediments collected in two areas of the Mediterranean Sea having different sedimentological characteristics have been analyzed to determine present concentrations and inventories of ^239,240Pu and to study the main mechanisms controlling them. Plutonium distribution in the deepest part of a submarine canyon (Taranto Valley, Ionian Sea) is compared to that obtained in an abyssal plain (north Algerian Plain). in the latter case, sedimentation is mainly due to the sinking of biogenic particles, while in the former lateral transport of terrigenous material along the slope of the canyon can significantly contribute to sediment accumulation on the bottom.

^239,240Pu surface concentration in the canyon ranged from 0.2 to 1 Bq kg^-1 (dry weight) and this was lower in the abyssal plain. in this area, plutonium was detectable only in the first 4 cm, while in the canyon it was present down to 11-15 cm. ^239,240Pu inventories are 3 Bq m^-2 in the plain and 45-60 Bq m^-2 in the canyon, indicating considerable input of terrigenous material towards the final part of the Taranto Valley.     

中国几个地区土壤中239,240Pu、241Am和137Cs等放射性核素的测定

分别从北京、太原、石家庄和济南地区采集了深度为0-5和5-20cm的土壤样品,进行了~(239,240)Pu、~(241)Am、~(137)Cs、~(40)K以及天然铀、钍系放射性核素的测定.估计了样品中放射性核素的水平和分布.结果表明,~(239,240)Pu、~(241)Am和~(137)Cs 的平均累积沉降量分别为24+13、10±5和1230±700MBq/km~2.~(239,240)Pu/~(137)Cs活度比为0.016—0.026(平均值0.020±0.004),~(214)Am/~(239,240)Pu活度比为0.35—0.49(平均值0.43±0.05).还讨论了这些核素与土壤中“过剩”~(210)Pb之间的关系.     

Geochemical Associations of Sellafield-Derived Radionuclides in Saltmarsh Deposits of the Solway Firth

This paper describes a study of the geochemical associations of Sellafield waste radionuclides in saltmarsh sediments from south-west s]Scotland. The contaminant radionuclides are transported to this environment in association with particulate material and ¹³⁷Cs was found to be predominantly (80-98%) non-extractable. In the case of ^239+240Pu there was a redistribution from the oxalate extractable oxide fraction to the pyrophosphate extractable organic fraction as a consequence of on-shore transfer of contaminated sediment. The relatively aggressive nature of the chemical extractants required to remove the radionuclides from the sediments suggests that they were in a form which was unlikely to result in their being released into the aquatic environment or taken up by plants. Plutonium had a greater potential mobility or bioavailability than Cs. Values of K^D for the desorption of ¹³⁷Cs from the sediment by freshwater, groundwater and seawater were all approximately 10⁵ L kg^-1, confirming its immobility in this environment. The desorption K_D values for stable ¹³³Cs were all approximately 10⁶ L kg^-1, so the stable Cs did not have a significant influence on the radiocaesium in this sediment.