两花岗岩体接触带铀系核素迁移的初步模拟

随着世界各国大力发展核电，放射性废料的安全处置已成为当今研究热点和前沿学科。高放废物深地质处置的安全性主要取决于处置库内放射性核素向生物圈的迁移程度。在侵入岩中，放射性核素主要是通过地下水沿岩石孔隙从处置库向生物圈迁移的。为了理解放射性核素在花岗岩体接触带的迁移行为，本文根据两花岗岩体接触带中样品的铀系核素放射性活度比值（^234U/^238U,^230Th/^234U,^226Ra/^230Th,^230Th/^238U)，利用 α-反冲（弹射）作用引起的放射性不平衡理论，计算了铀系核素子体^234U,^230Th,^226Ra在后期地下水的作用下在花岗岩体接触带及其裂隙内的迁出率、迁入率、并进行了质量平衡的计算。结果表明，经α-反冲作用进入流体的核素的迁出率要远大于因核素自然衰变的消亡率；裂隙充填物及裂隙能阻滞大量核素的迁移，其沉淀核素来自接触带花岗岩；花岗岩能强烈阻滞核素的迁移，可作为阻止放射性核素从核废料地下处置库向外迁移的有利天然屏障。     

高放废物地质处置黏土岩处置库围岩研究现状

世界上很多国家都对处置库的可能围岩进行了详细研究。通过对比,认为花岗岩、黏土岩、岩盐比较适合作为处置库围岩,而黏土岩由于具有自封闭性、渗透率低等其他岩石类型不可比拟的优点,因而将黏土岩作为高放废物地质处置库围岩越来越受到各国的关注。文章同时介绍了瑞士、法国、比利时等国家在黏土岩中所进行的大量研究,均认为在黏土岩中处置高放废物和乏燃料是安全的。文章还对黏土岩处置库概念设计、黏土岩处置库围岩地下实验室研究,以及我国开展黏土岩处置库研究的意义等进行了综述。     

处置单元核素135Cs迁移数值模拟研究

根据高放废物地质处置库概念设计,以北山花岗岩为参考岩性,内蒙古高庙子膨润土为参考缓冲材料,使用数值模拟软件tough2对放射性核素¹³⁵Cs在处置单元及其围岩中的迁移行为进行了数值模拟研究,考虑放射性核素衰变释热对核素迁移的影响。研究表明:膨润土对核素具有较强的滞留作用,模拟200000年后核素在花岗岩中迁移了1 m左右,且峰值为10-6个数量级;前10 a模型的温度变化最剧烈且温差最大,10 a后模型整体温度开始降低,2 000 a后整体温度接近于初始温度;温度的变化会引起核素迁移速率的改变,但总体温度对核素迁移的影响不大。     

核素迁移的示踪试验研究综述

按地下实验室或处置库的不同主岩,简述了以花岗岩,岩盐,粘土岩和凝灰岩等作处置库主岩的核素迁移示踪试验的研究现状,重点介绍了以花岗岩作高效废物处置库主岩的示踪试验方法和进展。     

铀在北山花岗岩中的吸附迁移影响因素研究

运用水文地球化学模拟软件PHREEQC-Ⅱ,对铀元素进入中国高放废物处置预选场研究区地下水后的状况进行了模拟和预测。模拟得到核素铀进入研究区地下水后的元素浓度分布和迁移情况及外界因素变化引起地下水中铀迁移的行为,同时采用批式法测定不同条件下铀在甘肃北山花岗岩中的分配系数,研究了岩石粒径、溶液初始浓度、水相pH和温度对分配系数的影响,实验结果表明花岗岩对铀的吸附能力较弱,其中溶液初始浓度、粒径、温度影响较小,pH值对岩石的吸附性能有较大影响,在接近中性条件下影响达到最大,这与采用模拟软件模拟结果基本吻合。通过模拟和实验对比,能更好地研究在北山预选区处置条件下地下水-废物-岩石的相互作用过程中核素的迁移行为,从而为处置库系统安全评价提供有关依据。     

~(239)Pu在某核废物处置预选区包气带的迁移预测

在西北某核废物处置库选址研究的基础上,对放射性核素239Pu在研究区包气带中的迁移进行了计算预测。结果表明,由于降水入渗量少、岩土介质对溶解形式Pu的吸附作用强,在24万年的时间跨度内,239Pu难以穿越处置库下方包气带进入潜水含水层;偏保守地考虑胶体可能促使Pu以水流速度迁移时,239Pu至迁移潜水面需480 a以上。研究认为,可溶性239Pu通过地下水途径对生态环境产生不可接受影响的可能性小;采用Kd模式可能导致对239Pu迁移速率的严重低估,应重视在水动力作用下239Pu胶体迁移景象的后果评价。     

花岗岩裂隙中~(134)Cs表面活度直接测量

测定岩石中放射性核素的浓度分布 ,是研究放射性核素在处置库周围岩石中的迁移、扩散和滞留规律 ,从而确定处置库隔离能力的必要手段。本文研究了花岗岩裂隙表面 13 4Cs活度的直接测定方法 ,并对有关影响因素进行了讨论     

高放废物深地质处置地下水数值模拟应用综述

开展地下水数值模拟研究是高放废物处置场地安全评价的重要组成部分,然而深地质处置介质类型的复杂性、基岩深部资料的相对匮乏性导致模拟结果存在不确定性,如何刻画深部地下水动力场并评估可能引起的风险已成为高放废物处置安全评价中重点关注的问题。在大量文献调研的基础上,综述了世界典型国家高放废物深地质处置场地的地下水数值模拟与不确定性分析应用,并归纳总结该领域研究经验,得到以下认识:（1）深地质处置场深部构造、裂隙的发育与展布决定了地下水循环条件,探究适用于基岩裂隙地区新的水文地质试验方法是提高地下水数值模型仿真性的基础;（2）不同尺度模型融合是解决深地质处置地下水模拟的有效技术方法,区域尺度多采用等效连续介质法,场地尺度使用等效连续多孔介质和离散裂隙网络耦合模型,处置库尺度使用离散裂隙网络方法,其次需重点关注未来大时间尺度下放射性核素在地质体中的迁移转化规律,模拟预测场址区域地下水环境长期循环演变对核素迁移的潜在影响;（3）考虑到不同的处置层主岩岩性以及在多介质中发生的THMC（温度场—渗流场—应力场—化学场）过程,目前国内外常用的地下水模拟软件有:Porflow、Modflow、GMS及MT3DMS等用于模拟孔隙或等效连续介质,Connectflow、Feflow及FracMan等用于模拟地下水和核素在结晶岩、花岗岩等裂隙中的迁移,TOUGH系列软件主要应用于双重介质的水流、溶质及热运移模拟;（4）指导开展有针对性的模型和参数的不确定性分析工作,减少投入工作量,提高模型精度,并可针对处置库长期演变、废物罐失效、极端降雨等多情景预测模拟,为处置库安全评价及设计提供基础数据支撑;（5）针对我国深地质处置地下水数值模拟研究现状,下一步应加强区域地质、水文地质、裂隙测量以及现场试验等相关的调查及监测工作,多介质耦合、多场耦合模拟及不确定性分析研究将会是未来的研究重点。     

热-水-应力耦合条件下三项因素对核素迁移影响的有限元分析

目前在放射性核素随地下水迁移的研究中还很少涉及温度场和应力场的影响。针对这一问题,引入渗透迁移方程,将所开发的饱和-非饱和孔隙介质中热-水-应力耦合弹塑性模型及其二维有限元程序进行了扩展和改进,使之可以同步地对温度场、渗流场、应力场和放射性核素浓度场的变化进行解析。对一个假想的核废料处置库算例,通过分别改变影响地下水中核素迁移的3个因素：渗透系数、分配系数和分子扩散系数,考察了在热-水-应力-迁移耦合作用条件下近场放射性核素浓度的分布及变化,从而认识到：当缓冲层的渗透系数小到一定程度后,缓冲层中核素迁移基本不再受渗流场的影响;缓冲层分配系数越小,分子扩散系数越大,核素迁移越快。     

324铀矿床近地表矿体中长寿命铀系核素和类比微量元素迁移特征

对一近地表铀矿体中某些铀系长寿命核素的放射性平衡状态和１４种微量元素迁移特征研究得出，自该铀矿床６３Ｍａ前生成至今，仅近１Ｍａ来，当上覆花岗岩遭剥蚀使矿体近地表时，矿石中天然放射性核和微量元素才因水－岩反应沿围岩破碎带，裂隙发生迁移；裂隙两侧岩石受水－岩反应影响的范围较小，裂隙面的化学组分以溶失为主，裂隙两侧粘土化花岗岩中则以核素、元素的扩散和吸附为主，最后阐述了本研究结果对高放废物处置库安全评价     

近海核电厂核素地下水释放通量的模型计算方法

为了定量计算陵区近海核电站排水管线泄漏情景下核素通过地下水途径向海洋环境的释放通量，以某近海核电站为例进行研究。首先，应用GOCAD软件建立三维地形地质模型，刻画地层的分布、剥蚀以及倾向等特点；然后，运用地下水数值模拟软件FEFLOW精细刻画丘陵区地下水系统的补给、径流和排泄特征；最后，以不被吸附滞留的核素³H和被吸附滞留的核素⁹⁰Sr、¹³⁷Cs为对象，通过实验测定了⁹⁰Sr、¹³⁷Cs在不同岩土介质中的分配系数，模拟计算了排水管线连续渗漏60 a后³H、⁹⁰Sr、¹³⁷Cs在地下水中的放射性分布及释放。结果表明：³H迁移速度基本与地下水流速一致，地下水中的最大放射性浓度为0.285 0 Bq/L，第20 000天时向收纳水域的释放通量达到最大值，约526 Bq/d；⁹⁰Sr吸附性能相对较弱，最大迁移距离约80 m，地下水中的最大放射性浓度为0.032 1 Bq/L；¹³⁷Cs吸附能力较强，相当长的时间内被滞留在管线附近，地下水中最大放射性浓度分别为6.840×10^-3 Bq/L，释放通量为0 Bq/d。由弥散度的不确定分析可知，弥散度越大，地下水中³H的最大放射性浓度越小，向海洋环境的释放通量越多。     

A Continuum One——Dimensional Model for Radionuclide Migration Testing in Unsaturated Loess

Unsaturated radionuclide migration experiments were conducted in a pit inside thetesting hall.Several types of radionuclides were used in the experiments.Tritium wasused as a tracer for water movement in unsaturated loess.Other kinds of radionuclideswere also used in order to obtain fundamental parameters for radionuclide migration sothat further environmental assessment of low—level radioactive waste disposal can be car-ried out.Mechanisms governing unsaturated flow in loess,that is,principles ofone—way lateral flow,are presented qualitatively in this paper.And a continuumone—dimensional model for radionuclide migration testing is developed based on the ex-periments conducted under the particular conditions at the test site.The data measuredfrom the tests were compared with solutions of this one—dimensional model.Resultsshow that this model is feasible for modeling radionuclide migration in unsaturatedloess.     

放射性核素在地下介质中迁移机理与模型研究

介绍了铀尾矿库的物理、化学概念模型和其中重金属、放射性核素迁移的一般过程 ;论述了沉淀作用、络合作用和胶体作用对放射性核素迁移的影响 ;重点讨论了描述吸附作用的离子交换模型和表面络合模型的建模机理 ;对定量模拟放射性核素迁移行为的 Kd模型、表面络合模型及“反应 -运移模型”的应用进行了评述。     

高放废物处置库天然类比及其有关的地球化学问题

介绍了高放废物处置库天然类比研究的主要内容,重点阐述了类比研究中涉及的地球化学问题,包括核素溶解度和化学形态研究、核素迁移速率研究、核素迁移影响因素研究,并总结相关问题研究取得的成果和认识.     

An overview of dissolved organic carbon in groundwater and implications for drinking water safety

Dissolved organic carbon (DOC) is composed of a diverse array of compounds, predominantly humic substances, and is a near ubiquitous component of natural groundwater, notwithstanding climatic extremes such as arid and hyper-arid settings. Despite being a frequently measured parameter of groundwater quality, the complexity of DOC composition and reaction behaviour means that links between concentration and human health risk are difficult to quantify and few examples are reported in the literature. Measured concentrations from natural/unpolluted groundwater are typically below 4 mg C/l, whilst concentrations above these levels generally indicate anthropogenic influences and/or contamination issues and can potentially compromise water safety. Treatment processes are effective at reducing DOC concentrations, but refractory humic substance reaction with chlorine during the disinfection process produces suspected carcinogenic disinfectant by-products (DBPs). However, despite engineered artificial recharge systems being commonly used to remove DOC from recycled treated wastewaters, little research has been conducted on the presence of DBPs in potable groundwater systems. In recent years, the capacity to measure the influence of organic matter on colloidal contaminants and its influence on the mobility of pathogenic microorganisms has aided understanding of transport processes in aquifers. Additionally, advances in polymerase chain reaction techniques used for the detection, identification, and quantification of waterborne pathogens, provide a method to confidently investigate the behaviour of DOC and its effect on contaminant transfer in aquifers. This paper provides a summary of DOC occurrence in groundwater bodies and associated issues capable of indirectly affecting human health.     

Subterranean microorganisms and radioactive waste disposal in Sweden

In 1987, microbiology became a part of the Swedish scientific program for the safe disposal of high level nuclear waste (HLW). The goal of the microbiology program is to understand how subterranean microorganisms will interact with the performance of a future HLW repository. The Swedish research program on subterranean microbiology has mainly been performed at two sites in granitic rock aquifers at depths ranging from 70 m down to 1240 m, the Stripa research mine in the middle of Sweden and the Äspö Hard Rock Laboratory (HRL) situated on the south eastern coast of Sweden. Some work has also been performed in cooperation with other national or international research groups in Sweden, Canada and at the natural analogue sites Oklo in Gabon and Maqarin in Jordan. The following conclusions are drawn. There is a very high probability of the existence of a deep subterranean biosphere in granitic rock. The documented presence of a deep biosphere implies that relevant microbial reactions should be included in the performance assessment for a HLW repository. A HLW repository will be situated in a subterranean biosphere that is independent of solar energy and photosynthetically produced organic carbon. The ultimate limitation for an active microbial life will be the availability of hydrogen as energy source over time, and hydrogen has indeed been found in most deep groundwaters. Sulphide producing microorganisms are active in environments typical for a Swedish HLW repository, and the potential for microbial corrosion of the copper canisters must be considered. The bentonite buffer around the copper canisters will be a hostile environment for most microbes due to the combination of radiation, heat and low water availability. Discrete microbial species can cope with each of these constraints, and it is theoretically possible that sulphide producing microbes may be active inside a buffer, although the experiments conducted thus far have shown the opposite. Microorganisms have the capability to enzymatically recombine radiolysis oxidants formed by radiation of water. It has earlier been concluded that the migration of radionuclides due to sorption on microorganisms can be neglected. The influence of microbially produced complexing agents remains to be studied at realistic conditions in deep groundwater. Microorganisms have been found in natural alkaline groundwaters, but it could not be conclusively demonstrated that they were in situ viable and growing, rather than just transported there from neutral groundwater. A possible hypothesis based on the obtained results from investigations of natural alkaline groundwaters is that fresh concrete may be a bit too extreme for active life even for the most adaptable microbe – but this remains to be demonstrated.     

The effect of fulvic acid on the sorption of actinides and fission products on granite and selected minerals

Organic material is present at low concentrations, typically 1–2 mg/l in terms of dissolved organic carbon (DOC), in groundwaters deep in granitic rock. Hydrophobic and hydrophilic acids may complex inorganic contaminants and change their sorption behaviour on geological materials. This report describes a series of experiments performed under aerobic conditions to investigate the effects of fulvic acid over a concentration range of 0–5 mg/I DOC on the sorption of⁸⁵Sr,¹³⁷Cs,²³³U,²³⁸Pu and²⁴¹'Am by crushed granite, biotite, goethite, montmorillonite and quartz. In addition, similar solutions were used to study the effects of dissolved fulvic acid on the sorption of⁹⁹Tc and¹²⁵I on each of the above solids except quartz. The fulvic acid was extracted from groundwater collected at a depth of 240 m in the granitic rock of the Underground Research Laboratory near Lac du Bonnet, Manitoba.In all experiments, the sorption of the fulvic acid by the geological materials was in the order goethite montmorillonite > biotite > granite > quartz. No sorption of Tc was observed from any of the solutions on any of the solids. Low sorption of I on montmorillonite occurred in the presence of the dissolved organic material. No sorption of I was observed with the other solids used. Only montmorillonite sorbed any appreciable amount of Sr in this study with the fulvic acid having no effect on this sorption. All the solids except quartz sorbed substantial amounts of Cs, but sorption was not affected by the organic material in solution. Each of the solids sorbed U with no difference in sorption observed due to the dissolved organic. In general, Pu sorption decreased as the concentration of dissolved fulvic acid increased. However, sorption of Pu on quartz remained at approximately the same levels regardless of the concentration of organic in solution. Generally high sorption of Am was found. Lowest sorption of Am on all solids occurred from the solution with the highest concentration of fulvic acid. Sorption of Am on granite decreased as the concentration of the organic in solution increased.This study indicated that, under aerobic conditions, the effect of dissolved organic material on sorption of radioisotopes depends on the radioisotope in question and the concentration of the organic in solution.     

Groundwater chemistry of Al under Dutch sandy soils: Effects of land use and depth

Aluminium has received great attention in the second half of the 20th century, mainly in the context of the acid rain problem mostly in forest soils. In this research the effect of land use and depth of the groundwater on Al, pH and DOC concentration in groundwater under Dutch sandy soils has been studied. Both pH and DOC concentration play a major role in the speciation of Al in solution. Furthermore, the equilibrium with mineral phases like gibbsite, amorphous Al(OH)₃ and imogolite, has been considered. Agricultural and natural land use were expected to have different effects on the pH and DOC concentration, which in turn could influence the total Al concentration and the speciation of Al in groundwater at different depths (phreatic, shallow and deep). An extensive dataset (n = 2181) from the national and some provincial monitoring networks on soil and groundwater quality was used. Land use type and groundwater depth did influence the pH, and Al and DOC concentrations in groundwater samples. The Al concentration ranged from <0.4 μmol L⁻¹ at pH > 7 to 1941 μmol L⁻¹ at pH < 4; highest Al concentrations were found for natural-phreatic groundwater. The DOC concentration decreased and the median pH increased with depth of the groundwater. Natural-phreatic groundwater showed lower pH than the agricultural-phreatic groundwater. Highest DOC concentrations were found for the agricultural-phreatic groundwater, induced by the application of organic fertilizers. Besides inorganic complexation, the NICA-Donnan model was used to calculate Al³⁺ concentrations for complexation with DOC. Below pH 4.5 groundwater samples were mainly in disequilibrium with a mineral phase. This disequilibrium is considered to be the result of kinetic constraints or equilibrium with organic matter. Log K values were derived by linear regression and were close to theoretical values for Al(OH)₃ minerals (e.g. gibbsite or amorphous Al(OH)₃), except for natural-phreatic groundwater for which lower log K values were found. Complexation of Al with DOC is shown to be an important factor for the Al concentrations, especially at high DOC concentrations as was found for agricultural-phreatic groundwater.