High burn-up operation and MOX burning in LWR; Effects of burn-up and extended cooling period of spent fuel on vitrification and disposal

Looking ahead to final disposal of high-level radioactive waste arising from further utilization of nuclear energy, the effects of high burn-up of light-water reactors (LWR) with UO₂ and MOX fuel and extended cooling period of spent fuel on waste management and disposal were discussed. It was assumed that the waste loading of waste glass is restricted by three factors: heat generation rate, MoO₃ content, and platinum group metal content. As a result of evaluation for effects of extended cooling period, the waste loading of waste glass from both UO₂ and MOX spent fuel could be increased in the current vitrification technology. For the storage of waste glass from MOX spent fuel with higher waste loading, however, those waste glass require long storage period prior to geological disposal because decay heat of ²⁴¹Am contributes significantly. Therefore, the evaluation of effects of Am separation on the storage period was performed. Furthermore, heat transfer calculation was carried out in order to evaluate the temperature of buffer material in a geological repository. The results showed, 70 to 90% of Am separation is sufficiently effective in terms of thermal feasibility of a repository.     

UO2燃料燃耗对高放废物管理的影响研究

从乏燃料的不同燃耗引起放射性和化学组成的变化出发,分析乏燃料经后处理后的衰变热、Mo及贵金属含量对玻璃固化工艺和玻璃固化体储存的影响,计算得到了不同燃耗乏燃料制得的高放玻璃的数量。计算结果认为：对于冷却8 a的乏燃料,决定玻璃固化体包容量的不是高放主组分的热功率;对于燃耗小于40 GW•d/tU的乏燃料,决定玻璃固化体包容量的是Mo元素含量;当燃耗大于45 GW•d/tU时,贵金属含量成为决定玻璃固化体包容量的主要因素,同时UO₂燃料燃耗与高放玻璃固化体数量上存在线性关系,燃耗增加会导致高放废物玻璃固化体数量增加。随着燃耗的增加,以Mo含量及贵金属含量计算得到的玻璃固化体数量比以衰变热计算得到的玻璃固化体数量多,因此,高放废物玻璃固化前将Mo及贵金属进行分离有利于减少高放废物玻璃固化体数量。对于UO₂燃料,燃耗加深对于高放废物玻璃固化体暂存时间几乎无影响。     

Helium diffusion coefficient measurements in R7T7 nuclear glass by He(d,α)H nuclear reaction analysis

The immobilization of fission products and minor actinides by vitrification is the reference process for industrial management of high-level radioactive wastes generated by spent fuel reprocessing. Radiation damage and radiogenic helium accumulation must be specifically studied to evaluate the effects of minor actinide alpha decay on the glass long-term behavior under repository conditions.A specific experimental study was conducted for a comprehensive evaluation of the behavior of helium and its diffusion mechanisms in borosilicate nuclear waste glass. Helium production was simulated by external implantation with ³He ions at a concentration (≈1 at.%) 30 times higher than obtained after 10,000 years of storage. Helium diffusion coefficients as a function of temperature were extracted from the depth profiles after annealing. The ³He(d,α)¹H nuclear reaction analysis (NRA) technique was successfully adopted for low-temperature in situ measurements of depth profiles. Its high depth resolution revealed helium mobility at temperatures as low as 253 K and the presence of a trapped helium fraction. The diffusion coefficients of un-trapped helium atoms follow an Arrhenius law between 253 K and 323 K. An activation energy of 0.55 ± 0.03 eV was determined, which is consistent with a process controlled by diffusion in the glass free volume.     

A new method for monitoring the radiation damage in nuclear waste containers using ion channelling

Immobilizing nuclear wastes has been one of the most important challenges in nuclear technology. A method to quantify and monitor the radiation damage to waste immobilizing crystalline materials like zircon is proposed. This method will make use of proton/ion channelling measurements of the crystalline containment sample or test crystalline sample placed in the crystalline or amorphous containment of nuclear waste for a long time from years to a few decades and the mathematical method to determine the structure collapse rate of the containment material using channelling measurements. Implementation procedure of this method/technique for radiation damage measurement in nuclear waste container materials is described.     

乏燃料处置的必要性及其处置库环境化学行为

为了确保核燃料循环的安全性，不宜处理的乏燃料也应该同玻璃固化体一样作为高放废物进行深地质处置。本文综述了一些前期工作，归纳了空气侵入和水的辐解产生氧化性产物是导致乏燃料UO2基体氧化溶解的主要因素; 核燃料浸出实验结果显示铀和锕系镧系元素每天的浸出量是相应核素总量的1/107，比裂变产物的浸出速率小一个数量级。铁金属被各国选为高放废物处置容器材料的原因是其低价格、高强度和优秀的还原能力。在最不利的地下水侵入深地质处置库、近场处置容器防腐层破损的情景下，铁容器材料表面与地下水反应产生氢气，氢气通过还原反应消耗辐解产生的氧化性自由基和分子, 并能还原乏燃料表面的U（Ⅳ），大幅度减缓乏燃料的腐蚀和溶解；乏燃料中裂变产物贵金属合金颗粒对氢气有催化作用；处置容器表面铁金属能还原沉积溶解的多价态核素U（Ⅵ）、Np（Ⅴ）、Tc（Ⅶ）、Se（Ⅳ）和Se（Ⅵ）。希望本文对我国确立以铁基金属为处置容器材料的包括乏燃料在内的高放废物深地质处置概念有参考作用。     

高放玻璃多重屏障介质多因素耦合处置方法研究

地下水透过多重屏障介质与高放玻璃固化体直接接触后,放射性核素会从固化体中释放,因此成为高放废物处置库安全评价的源项。为更精确地预测玻璃固化体长期处置行为,本文考察了围岩、回填材料等因素对模拟高放玻璃固化体中各关键元素浸出的影响,实验处置温度为90 ℃,模拟高放玻璃固化体依据德国配方制备。结果表明,围岩对玻璃体中不同元素的阻滞作用有所差异。B、Re和U的浸出浓度在二长花岗岩中最大;膨润土含水量高时,玻璃体中元素释出量大;而含水量低时,释出量小;在膨润土中添加5%的素玻璃粉,对玻璃的腐蚀有抑制作用。     

Failure model and Monte Carlo simulations for titanium (grade-7) drip shields under Yucca Mountain repository conditions

A failure model was developed for the titanium alloy drip shield proposed for the Yucca Mountain nuclear waste repository. The degradation modes considered are hydrogen-induced cracking (HIC) and general aqueous corrosion, processes which are inextricably linked. Failure by HIC is controlled by the environment, the corrosion rate, the material properties, and the hydrogen absorption efficiency which is assumed to decrease parabolically with time. This model includes both oxygen and water reduction coupled to corrosion, and allows for the release of the absorbed hydrogen as the alloy containing the hydrogen converts to oxide. Monte Carlo simulations were employed to predict drip shield lifetimes, and to investigate the effects of the hydrogen absorption efficiency, the critical HIC concentration, the corrosion rate, and the fraction of corrosion supported by water reduction, on the susceptibility of the material to HIC.     

2013—2018年山西省放射性废物库库区环境γ辐射水平监测

为了进一步加强对放射性废物库的安全管理,确保辐射环境安全,对2013—2018年山西省放射性废物库库区环境γ辐射剂量率的监测结果进行了分析。结果表明,库区环境γ辐射水平满足《核技术利用放射性废物库选址、设计与建造技术要求(试行)》中有关库房内源坑盖板上方0.5 m处γ辐射剂量率不超过20 μGy／h、源库墙外表面0.2 m处γ辐射剂量率不超过2.5 μGy／h的规定要求,各年度间环境电离辐射水平处于本底涨落范围内,未对周围环境产生辐射影响,辐射环境质量总体良好。此外,健全的库区安全防范也为促进我省核技术利用和安全、健康、可持续发展提供了坚强保障。     

地球化学工程学在放射性废物处置中的应用

介绍了应用地球化学工程学治理环境的基本依据,常用的放射性废物处置工程模式和工程屏障的功能,并以某放射性废物处置场地球化学工程屏障物料研究为例,说明地球化学工程学在放射性废物处置中的应用。研究结果表明,采用地球化学工程学方法来改良放射性废物处置场址的天然缺陷,可大大提高放射性废物处置的安全性。     

Simulations of H2O2 concentration profiles in the water surrounding spent nuclear fuel

A simple mathematical model describing the hydrogen peroxide concentration profile in water surrounding a spent nuclear fuel pellet as a function of time has been developed. The water volume is divided into smaller elements, and the processes that affect hydrogen peroxide concentration are applied to each volume element. The model includes production of H₂O₂ from α-radiolysis, surface reaction between H₂O₂ and UO₂ and diffusion. Simulations show that the surface concentration of H₂O₂ increases fairly rapidly and approaches the steady-state concentration. The time to reach steady-state is sufficiently short to be neglected compared to the times of interest when simulating spent fuel dissolution under deep repository conditions. Consequently, the steady-state approach can be used to estimate the rate for radiation-induced spent nuclear fuel dissolution.     

Ceramic matrices for plutonium disposition

One of the major issues related to the expanded use of nuclear power and the development of advanced nuclear fuel cycles is the fate of plutonium and “minor” actinides. In addition, substantial quantities of plutonium and highly enriched uranium from dismantled nuclear weapons now require disposition. There are two basic strategies for the disposition of the actinides: (1) to “burn” or transmute the actinides using nuclear reactors or accelerators; (2) to “sequester” the actinides in chemically durable, radiation-resistant materials that are suitable for geologic disposal. This paper deals with actinide-bearing materials that support the latter approach. During the past two decades, a considerable amount of research and development has been done in an effort to develop matrices for the immobilization of plutonium and the “minor actinides”, Np, Am and Cm. A variety of waste form materials – oxides, silicates and phosphates – have been developed that have a high capacity for the incorporation of actinides, are chemically durable and, in some cases, resistant to the radiation-induced transformation to the aperiodic state. These waste forms can be selected depending on the composition of the waste stream that contains the actinides, the desired materials' properties of the waste form, and the geochemical and hydrologic conditions of the specific repository. The present state-of-knowledge for these materials is such that now one can design materials for very specific conditions, such as the thermal history and accumulated radiation dose, in a repository.     

Corrosion issues in nuclear waste disposal

This paper summarized some corrosion issues specific to nuclear waste disposal and illustrates them by the French geological clay concept for the reliable prediction of container degradation rate and engineering barrier integrity over extended periods, up to several thousands years. Among the items, the following are included:

• The importance of the underground repository conditions.

• The necessity of developing comprehensive semi-empirical models and also predictive models that must be based on the mechanisms of corrosion phenomena.

• The use of archaeological artefacts to demonstrate the feasibility of long term storage and to provide a database for testing and validating the models.

Design and thermal modeling of radially configured nuclear waste packages

A series of radial design configurations for packaging nuclear wastes are described. These radial arrangements for used nuclear fuel assemblies in containers are effective techniques for packaging significantly more radioactive waste in the available internal container volume. The radial package designs can be applied to packaging the nuclear waste for permanent storage at the Yucca Mountain (YM) repository. The radially configured containers will have high degree of structural strength and will be efficient in transferring heat from the waste form to the package surface due to the minimization of internal gaps. Radial configurations are reported for packaging the Boiling Water Reactor (BWR) and Pressurized Water Reactor (PWR) used fuel assemblies. These configurations can be varied for co-packaging the colder, i.e. vitrified high level waste (HLW), canisters. Details of the geometry and the materials selected are discussed. Thermal analysis of the radial designs was conducted which confirm the feasibility of the designs demonstrating that no over-heating occurs in the contained nuclear waste in spite of the significantly extra amount of waste. The larger amount of packaged waste per container coupled with efficient heat transfer characteristics of these designs favor hotter and drier conditions for container surfaces in the YM emplacement drifts.     

开挖损伤区（EDZ）对核素迁移的影响

随着核电的发展,核电站产生的乏燃料处理处置受到了大众的高度关注。通过对嬗变法、稀释法和隔离法等方法的综合对比,目前,高放废物深地质处置是国内外公认处理核废物的最佳办法。在处置库建造阶段,由于开挖使得围岩中应力重新分布,围岩发生扰动,岩体内部原生裂隙出现扩展、连通,产生新生的微裂隙,岩体的渗透系数变大,这种区域即为开挖损伤区（excavation damaged zone, EDZ）。EDZ位于高放废物处置库工程屏障和远场围岩中间,是放射性核素迁移的重要迁移通道。地下水流经深部围岩裂隙与扰动层破碎带发生水岩反应导致成分发生变化,进而影响高放废物中核素释出速率与迁移参数,需要在地下实验室开挖过程中获取大尺度裂隙围岩及扰动层破碎带,建立核素释出和迁移装置,获得地下水侵入深部围岩裂隙与扰动破碎带导致高放废物核素释出与迁移参数变化规律,对于整个地质处置场的安全评价具有重要意义。研究人员通过实验和计算机软件进行模拟分析发现,EDZ区的裂隙水、Eh pH、裂隙充填物、裂隙中的胶体以及裂隙中的腐殖酸等,均会对核素迁移产生影响。开展EDZ对高放废物体核素源项释放的影响研究和深部围岩条件下核素迁移行为研究,掌握关键核素在深部地质条件下的释出规律及其在EDZ区域和裂隙中的迁移规律,优化迁移模型,将为地下实验室运行阶段开展核素迁移实验提供技术储备,为我国高放废物处置库场址比选、概念设计和安全评价提供技术支撑和科学依据。     

膨润土-砂混合物缓冲层轴向热传导性研究

膨润土-砂混合物作为高放废物处置库缓冲材料,在高放废物衰变释热作用下,其物理力学性能对处置库的稳定和安全性具有重要影响。本研究采用自行设计的装置,对按比例缩小后的不同干密度、含水率、掺砂率试样进行热传导模拟试验,并对缓冲层热-力耦合过程进行数值模拟分析,得到了缓冲层温度、应力和应变的变化及分布情况,重点分析了温度的影响。结果表明,增大试样干密度、含水率和掺砂率均可提高其导热性,应变也随之增大,应力受温度影响较早达到平衡;缓冲层靠近热源的位置温度、应力和应变最大,沿轴向方向递减,初始时刻变化明显。     

Colloid-facilitated effects on migration of radionuclides in fractured rock with a kinetic solubility-limited dissolution model

<正>Nuclides can move with groundwater either as solutes or colloids,where the latter mechanism generally results in much shorter traveling time as the nuclides interact strongly with solid phases,such as actinides.In the performance assessment,it is therefore essential to assess the relative importance of these two transport mechanisms for different nuclides.The relative importance of colloids depends on the nature and concentration of the colloids in groundwater.Plutonium(Pu),neptunium(Np),uranium(U) and americium(Am) are four nuclides of concern for the long-term emplacement of nuclear wastes at potential repository sites.These four actinides have a high potential for migrating if attached to iron oxide,clay or silica colloids in the groundwater.Strong sorption of the actinides by colloids in the groundwater may facilitate the transport of these nuclides along potential flow paths.The solubility-limited dissolution model can be used to assess the safety of the release of nuclear waste in geological disposal sites.Usually,it has been assumed that the solubility of the waste form is constant.If a nuclide reaches its solubility limit at an inner location near the waste form,it is unlikely that the same nuclide will reach its solubility limit at an outer location unless this nuclide has a parent nuclide.It is unlikely that the daughter nuclides will exceed their solubility limit due to decay of their parent nuclide.The present study investigates the effect of colloids on the transport of solubility-limited nuclides under the kinetic solubility-limited dissolution(KSLD) boundary condition in fractured media.The release rate of the nuclides is proportional to the difference between the saturation concentration and the inlet aqueous concentration of the nuclides.The presence of colloids decreases the aqueous concentration of nuclides and,thus,increases the release flux of nuclides from the waste form.     

Review of the development of the transportation,aging, and disposal (TAD) waste disposal system for the proposed Yucca Mountain geologic repository

The U.S. Department of Energy (DOE) began studying Yucca Mountain in 1978 to determine whether it would be suitable for the nation’s first long-tem geologic repository for over 70,000 metric tons of spent (or used) nuclear fuel and high-level radioactive waste. The purpose of the continuing Yucca Mountain study, or project, is to comply with the Nuclear Waste Policy Act of 1982 as amended in 1987 and develop a national disposal site for spent nuclear fuel and high-level radioactive waste disposal. In 2005, DOE shifted the design of the proposed repository from a concept of unloading spent nuclear fuel from transportation canisters and loading into disposal canisters (which required a great deal of handling radioactive material at the repository site) to a “clean” facility, unveiling the transportation, aging, and disposal (TAD) canister system. The TAD waste system consists of a canister loaded with commercial spent nuclear fuel.This review paper provides a comprehensive review on the status of TAD, technical and licensing requirements, the work that has been done so far, and the challenges and issues that must be addressed before TAD can be successfully implemented. Though the future of the Yucca Mountain project is bleak at this point, the progress that has come in the field of TAD will be one of its lasting legacies.     

Impact of Partitioning and Transmutation on High-Level Waste Disposal for the Fast Breeder Reactor Fuel Cycle

The impact of partitioning and/or transmutation (PT) technology on high-level waste management was investigated for the equilibrium state of several potential fast breeder reactor (FBR) fuel cycles. Three different fuel cycle scenarios involving PT technology were analyzed: 1) partitioning process only (separation of some fission products), 2) transmutation process only (separation and transmutation of minor actinides), and 3) both partitioning and transmutation processes. The conventional light water reactor (LWR) fuel cycle without PT technology, on which the current repository design is based, was also included for comparison. We focused on the thermal constraints in a geological repository and determined the necessary predisposal storage quantities and time periods (by defining a storage capacity index) for several predefined emplacement configurations through transient thermal analysis. The relation between this storage capacity index and the required repository emplacement area was obtained. We found that the introduction of the FBR fuel cycle without PT can yield a 35% smaller repository per unit electricity generation than the LWR fuel cycle, although the predisposal storage period is prolonged from 50 years for the LWR fuel cycle to 65 years for the FBR fuel cycle without PT. The introduction of the partitioning-only process does not result in a significant reduction of the repository emplacement area from that for the FBR fuel cycle without PT, but the introduction of the transmutation-only process can reduce the emplacement area by a factor of 5 when the storage period is extended from 65 to 95 years. When a coupled partitioning and transmutation system is introduced, the repository emplacement area can be reduced by up to two orders of magnitude by assuming a predisposal storage of 60 years for glass waste and 295 years for calcined waste containing the Sr and Cs fraction. The storage period of 295 years for the calcined waste does not require a large storage capacity because the number of waste packages produced is significantly reduced by a factor of 5 from that of the glass waste package in the FBR fuel cycle without PT.     

城市放射性废物库设计探讨

针对江苏省放射性废物的特点,提出城市放射性废物库库型、吊装工具、防洪抗震、安全防御及污染防治等方面的设计方案,既保证江苏省放射性废物和废旧放射源能得到安全收贮,又确保库区环境不受污染,促进江苏省核技术利用企业的发展。     

Status of the FRG activities on direct disposal of spent LWR-fuel

As stipulated by the German Atomic Energy Act, reprocessing is the reference waste management route for LWR's in the Federal Republic of Germany (FRG).Spent fuel disposal without reprocessing is being developed to technical maturity for those fuel elements for which reprocessing is either technically not feasible or economically not justifiable. The reference concept for direct disposal is the emplacement of large and heavily-shielded casks in drifts of a repository mine located in a salt dome. Moreover, a back-up solution is being pursued which results in smaller canisters which are emplaced in boreholes.The mining authorities have pointed out that the feasibility of direct disposal is to be demonstrated before a license for industrial scale deployment could be granted. Demonstration tests are necessary in the following areas: shaft transport of large and heavily shielded casks, handling of the casks in the repository and thermal and rock mechanics investigations with respect to the drift emplacement concept.The results of the demonstrations tests as well as the results from layout and optimization studies for a common repository for both reprocessing waste and spent fuel will be available early enough to be incorporated into the licensing procedure for the FRG's first repository for heat-generating nuclear wastes. This means that direct disposal of spent fuel not suitable for reprocessing could be introduced in the future in addition to the reprocessing and recycling waste management concept.