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放射性钚和铯在湖泊中的时空分布特性及近期沉积年代学应用
其他题名Spatial and Temporal Distribution of Plutonium and Radio-cesium in Lake Sediments and Their Application for Recent Chronology
廖海清
2008-05-04
学位授予单位中国科学院地球化学研究所
学位授予地点地球化学研究所
学位名称博士
关键词钚同位素 137cs 240pu/239pu同位素比 239+240pu/137cs活度比 湖泊沉积物 等离子质普法 中国核试验 计年
摘要短半衰期的137Cs具有高放射毒性,而半衰期较长的Pu的化学毒性极强,它们在环境中富集,进而在食物链中迁移,将直接威胁人类健康,国内在Pu和137Cs的分析方法、环境剂量以及湖泊地质等方面已展开了一些研究,但仍处于起步阶段,内容不够系统全面。湖泊和水库是生活饮用水或农用灌溉水源地,与人类生活息息相关,因此研究湖泊中人为放射性核素的污染状况、来源及归宿显得尤为重要;而且湖泊沉积物作为湖泊中大多污染物的最终归宿地,能够有效地保存湖泊区域的污染历史,研究湖泊沉积物有助于认清湖泊污染历史、探明污染机理,为污染现状评价、水质调查及治理提供可靠的基础依据,钚和铯的特殊性质可为环境科学等方面的研究提供关键的沉积年代学基础数据。 本研究在全国范围内选取具有代表性的不同区域分布、湖泊类型、人为扰动状况的湖泊为研究对象,应用基于γ谱的137Cs分析方法和本文建立的针对淡水湖泊沉积物的Pu同位素分析方法,研究了人为放射性核素Pu和137Cs在全国范围内的分布特征、近源传输及在湖泊中的沉积与迁移机理,并探讨了239+240Pu计年方法的有效性。通过上述研究,得到了如下主要结论: 1、建立了基于阴离子交换树脂分离的Pu同位素ICP-SF-MS分析方法,采用AG1-X8树脂分离Pu与杂质元素以及AG MP-1M纯化Pu同位素。高的仪器灵敏度、良好的U去除效率、足够的Pu同位素化学回收率表明该方法能够有效地检测湖泊沉积物样品中的痕量239Pu和240Pu。此外,纯化Pu同位素时,采用HBr洗脱Pu同位素以排除PbCl+对Pu同位素的干扰,因此该方法除了适应239Pu、240Pu分离分析之外,还可为后期分析浓度更低的241Pu提供技术保证。 2、通过分析沉积物岩芯中的239+240Pu沉积通量和137Cs沉积通量、240Pu/239Pu同位素平均比、239+240Pu/137Cs活度平均比及Pu、137Cs在沉积物岩芯中的剖面分布特征发现博斯腾湖有中国核试验基地的人为放射性核素污染,其表现形式为核爆试验产生的可溶性气溶胶颗粒和热核颗粒沉降后再悬浮造成的偶然性污染和源自罗布泊的地表径流引起的普遍性污染。博斯腾湖的Pu同位素结果表明平流层沉降的中国核试验的核碎片的240Pu/239Pu同位素原始比值可能为0.18左右,非常接近全球大气沉降值。苏干湖和双塔水库有源自中国核试验的可溶性气溶胶颗粒经大气沉降后再悬浮造成的人为放射性核素污染,苏干湖中大约有40%左右的137Cs以及27%左右的239+240Pu源自中国核试验,双塔水库中源自中国核试验的239+240Pu和137Cs所占的比例分别为27.1%和30.6%。 3、单一的239+240Pu和137Cs蓄积峰不能完全解析出沉积速率较慢的青海湖是否有源自在罗布泊进行的中国核武器爆炸试验的污染,但1963年全球大气沉降高峰下端的低240Pu/239Pu同位素比值表明青海湖可能有源自始建于1957年的中国原子城的地表径流泄漏或地下渗透泄漏的人为放射性核素污染。 4、西南地区的湖泊中,云南程海部分137Cs可能源于长距离迁移的中国核试验,但明确中国核试验对西南地区的影响还需要中国核试验源Pu和137Cs长距离迁移的信息,如青藏高原湖泊和西川盆地湖泊沉积物中人为放射性核素来源。其它湖泊中人为放射性核素的污染均源于全球大气沉降。 5、火山成因封闭式玛珥湖,在没有人为扰动的条件下,137Cs和239+240Pu主要以微弱的分子扩散迁移,迁移速率不明显,能较好地保持沉积历史;对人为活动比较频繁的浅水湖泊而言,人为活动、强风等恶劣气候以及上层水体和底层水体的交互对流等因素引起的沉积物再悬浮作用加剧了239+240Pu和137Cs主要以分子扩散迁移作用,造成水体寄宿时间短的浅水湖泊中239+240Pu和137Cs的不同步损失,导致239+240Pu和137Cs峰型的无序化。 6、受人为扰动较弱的湖泊中137Cs比活度和239+240Pu比活度成良好的线性相关,表明239+240Pu蓄积峰的信息能够为此类型湖泊沉积物提供有效的近期沉积年代学数据;对受人为扰动比较大的湖泊来说,137Cs和239+240Pu蓄积峰在近期沉积物计年的方面各有优劣,计年数据的可靠性不强;青海湖各沉积物岩芯的沉积物计年结果表明湖泊的沉积物累积率或沉积速度存在区域性差异。
其他摘要Plutonium isotopes and radio-cesium are anthropogenic radionuclide with strong chemical toxicity and high irradiation risk respectively. Their enrichment in environment and transfer through food-chains will raise threat to human health. Some researches about plutonium and radio-cesium have been carried out on the analytical method, radiation dose and lacustrine geology. The fact is, however, that these works were just on the threshold of studies on artificial radionuclide in China. Moreover, it is of great importance to recognize the source, distribution and destination of anthropogenic radionuclide in lakes or reservoirs as a result of both lakes and reservoirs are the main sources of drink-water or agricultural irrigation water. Since lake sediment which is regarded as the destination of all pollutants could effectively preserve the contaminating history of drainage area, it can be used to elucidate the polluting process and provide the basic information for water quality controlling. The plutonium and radio-cesium can provide significant recent chronology data for these environmental researches due to their exclusively characteristic. In this paper, some special lakes and reservoirs were selectively studied as different location, type and disturbance to understand the distribution and transportation of plutonium and 137Cs in China and elucidate their sedimentary mechanisms in lakes by using the traditional 137Cs analytical method based on gamma spectrometry and plutonium analytical method which was developed in this work for freshwater lake sediment. Furthermore, we also discussed the availability of 239+240Pu as a type of recent chronology for lakes. The main conclusions are as follows. 1、We measured Pu isotopes in freshwater lake sediments by ICP-SF-MS after separation and purification using AG1-X8 resin followed by a strong base resin of AG MP-1M. The high U decontaminated factor, suficient recovery and the high sensitivity of ICP-SF-MS demonstrated that this analytical method for Pu isotopes is suitable for studies on recent lake sedimentation. Moreover, the interference of PbCl+ on plutonium isotopes was effectively eliminated by using the concentrated HBr as the final eluent for Pu elution, so this analytical method is also suitable for the analysis of 241Pu. 2、The 239+240Pu inventory, 137Cs inventory, 240Pu/239Pu atom ratio, 239+240Pu/137Cs activity ratio and vertical distribution of 239+240Pu activity and 137Cs activity in lakes demonstrated that Lake Bosten which is located at the west of Lop Nor have been contaminated partially by the re-suspending particle of soluble aerosol radionuclide and hot-particle which originated from China’s Nuclear Tests, and whole Lake Bosten may have also been contaminated by those radionuclide which were transported by surface runoff from Lop Nor. The plutonium isotope ratio in sediment core of Lake Bosten is close to the value of global fallout, suggesting that CNT’s Pu has similar 240Pu/239Pu atom ratio to that of global fallout. This phenomenon was also supported by results of Lake Sugan and Shuangta reservoir, both them are close to the east of Lop Nor. Lake Sugan and Shuangta reservoir have also been polluted by aerosol particles of radionuclide re-suspended from Lop Nor. About 40 percent of 137Cs and 27 percent of 239+240Pu in Lake Sugan were originated from CNT, and CNT contributed about 30 percent of 137Cs and 27 percent of 239+240Pu to Shuangta reservoir. 3、As for Lake Qinghai, it is hard to resolve the Pu pollution of CNT from global fallout due to its extremely low sediment rate. However, the evidently low 240Pu/239Pu atom ratio around 0.06 in sediment layer under the 1964 marked layer indicate that Lake Qinghai may have gotten Pu contamination from the Chinese nuclear weapon producing base named “Atomic City” which was built in 1957 and is about 10km far from the northwest bank of Lake Qinghai. 4、Regarding this case for lakes in southwest China, part of 137Cs in sediment core of Lake Chenghai may from CNT by long-term transportation. More evidences are, nevertheless, extremely required to confirm this hypothesis, such as the source of Pu and 137Cs in lakes which locate in Tibet Plateau and Sichuan Basin. Both the Pu isotope ratio and the Pu vertical distribution in lakes, including other lakes in southwest China, Lake Sihailongwan (Northwest China), Lake Taihu and Lake Poyang (East China) demonstrated that all radionuclide in these lakes were originated from global fallout. 5、A maar lake is a broad, low relief crater that is caused by a phreatic eruption or explosion caused by groundwater contact with hot lava or magma. Under the condition that the lake has never been disturbed, maar lake could keep the best record of depositional history, in which inapparent diffusion of deposit radio-cesium and plutonium is the main transfer pattern. As for shallow lakes, frequent human activities, hurricane and inter-convection between surface water and bottom water of lake may cause intensive re-suspending of sediment and strengthen the diffusion of deposit radio-cesium and plutonium. So as to those shallow lakes have been given inhomogeneous loss on 137Cs and Pu, and the vertical distribution of 137Cs and Pu in sediment core became out-of-order. 6、Lakes which have a little disturbance presented well linear correlation between 137Cs activity and 239+240Pu activity in sediment core, indicating that the 239+240Pu accumulation peak in such lakes can provide effective recent chronology information for lacustrine science. However, 137Cs and Pu couldn’t be used to date sediment in those intensively disturbed lakes. The sedimentation rates of different core in Lake Qinghai are evidently different from each other, suggesting that sedimentation rates or sedimentary accumulation rates in different locations of the same lake are changed.
页数110
语种中文
文献类型学位论文
条目标识符http://ir.gyig.ac.cn/handle/352002/3260
专题研究生_研究生_学位论文
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廖海清. 放射性钚和铯在湖泊中的时空分布特性及近期沉积年代学应用[D]. 地球化学研究所. 中国科学院地球化学研究所,2008.
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