核废物处置安全评价的地质类比研究

本文简要论述了利用天然地质类似物（或类比体），类比评价核废物处置系统的安全性能。地质类比研究是安全评价核废物处置系统的重要方法之一，也是地质学科的新研究领域。目前已有的地质类比研究对象主要有火山玻璃，陨石玻璃，粘土矿物，铁陨石，铜矿床，铀矿床，含含Ｔｈ和ＲＥＥ的铁矿床，天然核反应堆（一种特殊的铀矿床）和火成岩接触带等。最后对我国今后从事同类研究提出了若干建议。     

Influence of Pore Fluid Chemistry on the Mechanical Properties of Clay-Based Materials

The producers of nuclear waste, within all countries exploring options, including Canada, have determined the long-term solution to be a deep geological repository. In the Canadian concept, within the deep geologic repository a number of clay-based barriers will separate the containers from the surrounding geosphere. Following placement the surrounding groundwater will infiltrate into the repository. In order to analyze the performance of the repository under very complex conditions, accurate material properties are required. The chemistry of the host rock is an important aspect as the behaviour of clay-based barrier materials could be affected by the saturating saline groundwater. This paper investigates the saturated mechanical behaviour of light backfill (composed of 50 % silica sand and 50 % Na-bentonite clay) and dense backfill (composed of 70 % crushed granite, 25 % glacial lake clay and 5 % Na-bentonite clay) and the quantifying the effect of pore fluid chemistry on the strength and compressibility behaviour of the materials. The results indicate that light backfill behaviour is strongly influenced by its pore fluid chemistry while dense backfill shows limited effects. The material parameters of light backfill and dense backfill are interpreted for input into numerical simulations. These results and interpretation enrich the understanding of the mechanical response of light and dense backfill, two components of the sealing system of the Canadian deep geologic repository.     

考虑膨胀效应UH模型的有限元实现

高庙子膨润土已被确定为我国高放废物地质处置的首选缓冲/回填材料,进行其力学特性及应用模拟研究对合理设计处置库具有十分重要的意义。考虑膨胀效应的UH模型是在超固结非饱和土本构模型（非饱和土UH模型）的基础上提出的,因引入了土体团粒的吸水膨胀作用,使其适用于非饱和膨润土。基于有限元软件ABAQUS的二次开发平台,利用Fortran语言编制模型的UMAT（user-difined material）材料子程序,进行了考虑膨胀效应UH模型的有限元实现。然后针对高放废物处置概念模型,利用编制的模型子程序对高放废物处置系统进行了三维有限元模拟,并对渗流场和应力场的演化规律进行了初步探究。模拟结果显示处置系统中膨润土的内应力增加,土体的稳定性较好,说明选择高庙子膨润土作为缓冲/回填材料的合理性,也同时验证了程序的正确性。     

高放废物地质处置研究中的矿物学问题

在高放废物地质处置研究中的一些矿物学问题应引起矿物学家的注意 。高放废物地 质处置库的缓冲/回填材料是选择以钠质蒙脱石为主要成分的钠基膨润土,还是以钙质蒙脱 石为主的钙基膨润土?怎样选择对99Tc、129I有较好吸附能力的硒汞矿、脆 硫锑铅矿和辉锑矿的替代物来作缓冲/回填材料中的添加剂,以能阻滞99Tc和129 I的迁移?沸石对某些放射性核素的吸附特征也需进一步研究。     

Performance evaluation of soil mixtures treated with graphite and used as barrier fill material for high-level radioactive waste repository

Buffer/backfill material is an important engineering barrier in a deep geological repository of high-level radioactive waste (HLW). Its thermo-hydro-mechanical (THM) performance is very important for the safe and stable operation of the HLW repository system. Natural graphite powder mixed with sodium bentonite forms a buffer/backfill material that can dissipate heat quickly and provide strong isolation. In this paper, the THM characteristics of bentonite–sand–graphite–polypropylene fiber (BSGF) mixtures, used as a buffer/backfill material, were studied through a series of laboratory tests. The influence of graphite and polypropylene fiber contents on thermal conductivity, swelling pressure, hydraulic conductivity, and strength properties of BSGF mixtures with different sand contents was analyzed. Experimental results indicated that the graphite content, the maximum graphite mesh number, and the initial dry density of bentonite–graphite mixtures influenced the thermal conductivity of bentonite–graphite mixtures. The addition of polypropylene fiber was found to enhance the shear strength and inhibit cracking without significantly affecting the expansivity, permeability, and thermal conductivity of the BSGF mixtures. This study provides a new buffer/backfill material that can improve the stability, functionality, and thermal efficiency of the HLW repository.

     

The effect of iron on montmorillonite stability. (I) Background and thermodynamic considerations

It is envisaged that high-level nuclear waste (HLW) will be disposed of in underground repositories. Many proposed repository designs include steel waste canisters and bentonite backfill. Natural analogues and experimental data indicate that the montmorillonite component of the backfill could react with steel corrosion products to produce non-swelling Fe-rich phyllosilicates such as chamosite, berthierine, or Fe-rich smectite. In K-bearing systems, the alteration of montmorillonite to illite/glauconite could also be envisaged. If montmorillonite were altered to non-swelling minerals, the swelling capacity and self-healing properties of the bentonite backfill could be reduced, thereby diminishing backfill performance. The main aim of this paper was to investigate Fe-rich phyllosilicate mineral stability at the canister-backfill interface using thermodynamic modelling. Estimates of thermodynamic properties were made for Fe-rich clay minerals in order to construct approximate phase-relations for end-member/simplified mineral compositions in logarithmic activity space. Logarithmic activity diagrams (for the system Al₂O₃-FeO-Fe₂O₃-MgO-Na₂O-SiO₂-H₂O) suggest that if pore waters are supersaturated with respect to magnetite in HLW repositories, Fe(II)-rich saponite is the most likely montmorillonite alteration product (if f_O2(g) values are significantly lower than magnetite-hematite equilibrium). Therefore, the alteration of montmorillonite may not be detrimental to nuclear waste repositories that include Fe, as long as the swelling behaviour of the Fe-rich smectite produced is maintained. If f_O2(g) exceeds magnetite-hematite equilibrium, and solutions are saturated with respect to magnetite in HLW repositories, berthierine is likely to be more stable than smectite minerals. The alteration of montmorillonite to berthierine could be detrimental to the performance of HLW repositories.     

The use of natural analogues to assess radionuclide transport

Predicting the long-term safety and performance of a repository for intermediate- to high-level radioactive wastes requires the evaluation of various scenarios which may influence the integrity of the repository system. One such scenario, radionuclide transport, is described, and some of the geochemical processes which serve to enhance or retard transport are illustrated with examples selected from natural analogue or natural system studies. These studies, as distinct from laboratory simulations, help considerably in understanding how near- and far-field radionuclide transport mechanisms work over geological timescales (thousands to hundreds of thousands of years), more in line with the anticipated lifespan of a repository.

Processes addressed include: stability of the spent fuel UO₂ matrix; bentonite backfill as a barrier to radionuclide diffusion; retention of radionuclides by absorption on fracture minerals; transport and diffusion of radionuclides controlled by interconnected bedrock porosity; geochemical influence and behaviour of repository construction materials on radionuclide transport.     

The potential effect of cementitious colloids on radionuclide mobilisation in a repository for radioactive waste

Colloid-facilitated transport of contaminants could enhance the release rate of radionuclides from the cementitious near field of a repository for radioactive waste. In the current design of the planned Swiss repository for intermediate-level radioactive waste, a gas-permeable mortar is employed as backfill material for the engineered barrier. The main components of the material are hardened cement paste (HCP) and quartz aggregates. The chemical condition in the backfill mortar is controlled by the highly alkaline cement pore water present in the large pore space. The interaction of pore water with the quartz aggregates is expected to be the main source for colloids. Colloid transport is facilitated due to the high porosity of the backfill mortar. Batch-type studies have been performed to generate colloidal material in systems containing crushed backfill mortar or quartz in contact with artificial cement pore water (ACW) at pH 13.3. The chemical composition of the colloidal material corresponds to that of calcium silicate hydrates (CSH). Batch flocculation tests show that, after about 20 days reaction time, the concentration of the CSH-type colloids is typically below 0.1 mg l⁻¹ due to reduced colloid stability in ACW. Uptake studies with Cs(I), Sr(II) and Th(IV) on a CSH phase (initial C:S ratio=1.09) have been carried out to assess the sorption properties of the colloidal material. The influence of uptake by colloids on radionuclide mobilisation is expressed in terms of sorption reduction on the immobile phase (HCP). Sorption reduction factors can be estimated on the assumption that the sorption properties of the colloidal material are either similar to those of the CSH phase or HCP, and that sorption is linear and reversible. A scaling factor accounts for the higher specific surface area of the colloidal material compared to the CSH phase and HCP. At colloid concentration levels typically encountered in highly alkaline cement pore waters, colloid-induced sorption reduction is predicted to be negligibly small even for strongly sorbing radionuclides, such as Th(IV). Thus, no significant impact of cementitious colloids on radionuclide mobilisation in the porous backfill mortar is anticipated.     

Investigation on healing behavior of unsaturated GMZ bentonite pellet mixture based on compressibility

Acta Geotechnica - Bentonite pellet mixture has been considered as an important candidate buffer/backfill material in deep geological repository for disposal of high-level radioactive waste. During...     

高放废物深地质处置：回顾与展望

文章对我国高放废物地质处置研究的历史进行了回顾,并对未来发展进行了展望。我国的高放废物深地质处置研究开发从1985年开始,迄今为止可初步分为3个阶段：①起步和跟踪研究阶段（1985～1998）;②逐步发展阶段（1999～2005）;③政府规划指导阶段（2006至今）。20多年来,我国在国家法律法规、战略规划、选址、工程屏障、核素迁移研究等方面取得了显著进展。我国已经提出在2020年前建成地下实验室、21世纪中叶建成高放废物处置库的目标。研究开发和处置库工程建设分成3个阶段：试验室研究开发和处置库选址阶段（2006～2020）;地下现场试验阶段（2021-2040）和处置库建设阶段（2041～本世纪中叶）。经过全国筛选对比,已初步选定甘肃北山地区为重点预选区,系统的场址评价工作正在进行。已确定采用膨润土作为处置库的回填材料,并初步确定内蒙古高庙子膨润土为我国高放废物处置库的首选缓冲回填材料。工程设计、核素迁移研究和安全评价也取得了一定进展。1999年起与国际原子能机构开展了3期高放废物地质处置技术合作项目,对提高我国的技术水平起到了积极作用。20多年的研究开发工作为我国在21世纪完成高放废物地质处置任务奠定了基础。     

中国高放废物地质处置缓冲材料大型试验台架和热-水-力-化学耦合性能研究

缓冲材料作为高放废物深地质处置库中一道重要的人工屏障,与高放废物容器和处置库围岩直接接触,在高放废物衰变热、辐射作用和地下水等影响下产生复杂的热-水-力-化学耦合作用,为了验证缓冲材料是否能长期有效地发挥其屏障材料的作用,核工业北京地质研究院利用高庙子钠基膨润土组装并运行了模拟中国高放废物地质处置室 尺寸的大型缓冲材料膨润土试验台架（China-Mock-Up）。建立了缓冲材料试验台架的安装和试验方法,依据实测数据和理论分析,揭示了热-水-力-化学耦合作用条件下膨润土中的相对湿度是在加热器的热效应和外部供水的湿效应共同作用下发生变化的,压实膨润土中应力的变化主要是由于膨润土遇水膨胀和加热器的热效应引起的,试验验证了模拟高放废物地质处置室内加热器（废物罐）运行初期的位移过程,为缓冲材料和高放废物地质处置库的设计提供了重要的工程参数和理论依据。     

新疆地区选建高放射性核废物处置库的可能性

高放废物选址是一项万年大计工程,需要多个预选场地的综合比较,决策废物处置库的具体选建场地。论述了高放废物处置库选址过程中需要考虑的主要问题,然后针对新疆的自然环境,水资源、花岗岩体和缓冲/回填材料的分布,以及区域地壳稳定性等因素,讨论了在新疆选建高放废物地质处置库的可能性,并提出了选址方法。     

Study on the Themal Conductivity of Compacted Buffer/Backfill Materials

The thermal property is one of the key properties for the design of the high-level radioactive waste (HLW) repository. In this study, the thermal properties transient automatic tester (HPP-F) is uesd to study the thermal conductivity of multiphase composite buffer/backfill material including the type B-Z and B-Z-P (Here B、Z、P represents bentonite、zeolite and pyrite respectively,the same as in the following.) in different dry density and moisture conditions. The results show that for the same moisture content (dry density), thermal conductivity of specimens increases as the dry density (moisture content) increases. As a result, the type B-Z-P which is highly compacted of 1.8 g/cm3 in dry density and 17.65% in moisture content performs well, it meets the requirements of the IAEA and is easy to be compacted ,so it can be recommend as a alternative material of high level radioactive waste disposal repository buffer/backfilling materials.     

Alteration geochemistry of the Nopal I uranium deposit (Sierra Peña Blanca,Mexico), a natural analogue for a radioactive waste repository in volcanic tuffs

Natural analogues provide an approach to characterize and test the long‐term modelling of a repository performance. This article presents geochemical information about the alteration conditions of the Nopal I uranium deposit, Mexico, an analogue for the proposed Yucca Mountain radioactive waste repository. Mineralization and hydrothermal alteration of volcanic tuffs are contemporaneous, according to petrographic observations. Trace element geochemistry (U, Th, REE) provides evidence for local mobilization of uranium under oxidizing conditions and further precipitation under reducing conditions. O‐ and H‐isotope geochemistry of kaolinite, smectite, opal and calcite suggests that argillic alteration proceeded at shallow depth with meteoric water at 25–75 °C, a low‐temperature context, unusual for volcanic‐hosted uranium deposits. This temperature range is compatible with some post‐closure evolution models of the proposed Yucca Mountain repository.     

地质系统热-水-力耦合作用的随机建模初步研究

热-水-力(THM)耦合作用是岩石力学与环境地质中的重要基础理论问题,核废料地质处置库周围的缓冲材料和围岩中的热-水-力耦合现象将影响其力学稳定性、热传导性和渗透性,进而影响放射性核素在裂隙岩体中的迁移规律。核废料或放射性废料的地下深埋处置是国际上正在研究的永久性隔离的有效方法之一。因此,对核废料地质处置法安全性评估的一个重要内容就是对裂隙岩体中力学稳定性与构造应力、地下水渗流及热载荷等的耦合作用之数值模拟和评估。这已成为当前刻不容缓的重要的环境影响评价课题。笔者研究了温度场-渗流场-应力场中热传导系数和渗透率以及岩体力学参数的空间变异性,用实验方法研究三场耦合效应及裂隙岩体的场性能等效处理,试图建立热-水-力耦合作用的随机性数学模型及可视化数值模拟方法,为核废料地质处置安全性评估提供直观的新方法。     

钠-蒙脱石地球化学性能模拟研究

膨润土已经被许多国家确定为高放废物深地质处置系统的缓冲/回填材料。钠-蒙脱石作为钠基膨润土的主要矿物,对钠基膨润土的地球化学稳定性能起着关键作用。以地球化学模拟软件PHREEQC和GWB为平台,对内蒙古高庙子膨润土的关键矿物——钠-蒙脱石在无氧和不同温度条件下的地球化学行为进行了模拟研究,分析了钠-蒙脱石在北山地下水体系中矿物成分、液相化学成分、pH值的长期演变规律。     

Critical issues in modelling the long-term hydro-thermomechanical performance of natural clay barriers

Performance assessment of deep repositories for heat-generating radioactive waste requires the capability of predicting reliably the evolution of the system during a time period commensurate with the hazardous life of the waste. In many repository designs clay barriers represent important elements of the waste isolation system.

In order to provide reasonable assurance that clay barriers will ensure long-term waste isolation, it is essential to understand their behaviour under a variety of conditions. Due to the variability of argillaceous materials, to the complexity of the phenomena that might take place in a waste repository and to the longevity of the required isolation, an adequate understanding of the behaviour and the capability to model the evolution of the clay barriers are not easy tasks. The factors that need to be understood and modelled include stress evolution, long-term strain or creep, thermal effects on solid skeleton, on interstitial fluids and on mineralogy. The difficulty of the task is increased by the facts that many effects are coupled, that their rates must be extremely low, in order to be realistic, and that the time period to be modelled defies the possibility of direct experimental observation. Several critical issues are identified and discussed briefly, such as: constitutive law to describe the thermo-mechanical behaviour of the clay skeleton, modelling of the fluid phase in clays and its response to heating, thermal fracturing and healing. Strategies are suggested for a rational approach to the experimental investigation of some relevant processes. The study of suitable natural analogues, for example the thermo-metamorphic halo occurring at Orciatico in Tuscany, could provide valuable insights in the thermal effects of heating clay barriers. It is conceivable that models describing a variety of relevant phenomena, such as dehydration, fracturing and permeability changes could be tested through the study of the Orciatico analogue.

In the end performance assessments of clay barriers would benefit through improvements in modelling: this would involve progress in understanding the basic phenomena and their coupled nature, improved conceptual and mathematical models and increased reliability for their calibration/validation. The improved understanding of phenomena requires additional experimental activities on various levels: molecular, microscopic, macroscopic, medium scale and in situ.     

Simplified evaluation for swelling characteristics of bentonites

Bentonite is currently planned to be used as buffer and backfill materials for repositories of high-level nuclear waste because these materials must have the swelling characteristics to seal the waste. In the design for buffer and backfill materials, we must choose the adequate bentonite among many kinds of bentonite in the world. The database of the swelling characteristics of various bentonites and its evaluation will be available when we will select the adequate bentonite. For this purpose, this study performed the laboratory tests on the swelling pressure and swelling deformation of four kinds of bentonite produced in Japan and the United States. These bentonites have different physicochemical properties. This study investigated the characteristics of swelling pressure and swelling deformation from the viewpoint of the physicochemical properties of each bentonite. Furthermore, this study also proposed the simplified evaluation of swelling characteristics of various bentonites on the basis of microscopic analysis.     

Numerical study of the performance of tunnel plugs

High axial flow rates within and along tunnels, excavated for deposition of high level nuclear waste, may increase the transport capacity of potential escape routes for radionuclides that have been released to the buffer surrounding the waste canisters, or to the tunnel backfill materials, from leaking fuel canisters. High flow rates may be found if the tunnel interior has a high permeability, either initially due to the composition of the backfill material or at later times due to degradation of low permeability backfill material components. If a disturbed rock zone, a DRZ, of increased permeability was created as a result of direct damage done to the wall region during tunnel excavation, this zone may contain additional possible escape routes. Low-permeability tunnel plugs, keyed into slots cut in the rock walls, have been suggested as means of reducing axial flow rates. This paper deals with different aspects of such tunnel-plug systems. A preliminary estimate of the potential for tunnel plugs to reduce axial flow rates is made using analytical expressions. A number of numerical techniques are employed to investigate the hydraulic, mechanical and hydromechanical performance. These include μFLOW (FEM flow calculations), FLAC (finite difference mechanical calculations) and 3DEC (distinct element mechanical calculations). The mechanical calculations concern the mechanical stability in the rock surrounding the slot and permeability changes in that rock caused by stress redistribution. The results show that the effects of tunnel plugs are very significant in most cases. A discussion on the validity of the results and the applicability of the used methods is provided.     

Eu(Ⅲ)溶液对膨润土-砂混合物渗透性能影响研究

在高放废物处置库长期运营过程中包封容器将发生破坏,核素会向外界迁移,缓冲回填材料的水力传导系数是评价处置库工程屏障性能的重要指标。采用柔性壁渗透仪,研究2.0×10-5 mol/L的Eu(III)溶液作为渗入液时膨润土-砂混合物的渗透特性。结果表明,膨润土-砂混合物的水力传导系数K=(2.07⁵.23)×10-10 cm/s;在05.23)×10-10 cm/s;在0⁵0%掺砂率范围内,膨润土-砂混合物吸水膨胀过程中渗透性能随掺砂率增大时没有明显的变化,能够满足高放废物处置库缓冲回填材料低渗透性的要求。使用有效黏土密度的概念,得到膨润土-砂混合物的体积膨胀率随初始有效黏土密度的增大呈指数增大的趋势;混合物水力传导系数的对数值与有效黏土密度存在良好的线性衰减关系;与蒸馏水相比,渗入液(ECDD)为2.0×10-5 mol/L的Eu(III)溶液时,膨润土-砂混合物的水力传导系数较小,可能是由于渗入液黏滞性的影响。