放射性核素在地质介质中的迁移研究

利用拉普拉斯变换给出了迁移方程在一维近似条件下的解析解，并且研究了核素表观扩散系数和地下水流速等参数对扩散的影响，结果表明，在核素迁移过程中，核素的扩散作用是主要的，而地下水的输运作用是次要的。     

新疆伊犁盆地南缘地下水的演变及对层间氧化带的空间定位分析

分析了伊犁盆地地下水的发展演变历史和地下水对层间氧化带的改造作用,层间氧化带水文地球化学分带特征及其水岩作用机理、水中铀的迁移转化规律等。阐明了地下水是控制层间氧化带发育和铀矿化的重要因素之一。     

地下水模型系统GMS在核电厂地下水核素迁移数值模拟中的应用

福岛事故后,核电厂地下水环境影响评价逐渐成为人们关注的焦点。本文针对某内陆核电厂,基于地下水模型系统GMS,对某厂址及其附近区域地下水进行三维数值模拟,并对重要核素H-3、Cs-137和Sr-90在地下水中的迁移行为和影响范围进行预测和评价。结果表明:一旦发生放射性废液泄漏事故,H-3迁移速度较快,会影响厂址及其附近区域地下水,但不会对厂址北部河流造成影响;Cs-137和Sr-90迁移速度缓慢,影响范围仅局限在泄漏点周围100 m范围内,不会造成厂外影响。     

裂隙场址条件下处置场核素迁移的计算

核素随地下水在裂隙中的迁移与在孔隙中的迁移比较,不论从地下水与岩石的接触过程还是介质对核素的吸附作用来说都有很大不同。本文以国内某基岩裂隙场址低中放射性固体废物处置场为例,运用Ecolego软件对核素在裂隙中的迁移过程进行模拟,深入探讨了计算过程中的模型建立、参数选取等关键问题,并对计算结果进行了分析,得出裂隙对核素迁移影响的结论。     

基于GMS的某铀矿地下水中铀迁移模拟

为了掌握某地浸铀矿地下水中铀的迁移状况,结合某地浸铀矿的地质条件和相关参数,建立了此地浸矿的三维水流模型和地下水水质迁移模型。通过应用GMS软件数值模拟软件,模拟某地浸铀矿采区地下水中铀的运移范围和运移规律,通过模拟结果,发现铀的迁移随地下水流场的影响较大,在低水头区域有浓度富集现象的存在。模拟1、5、10、20年后,区域内的铀浓度逐渐趋向稳定,模拟结果可以铀矿地下水污染防治提供数据依据。     

放射性核素有机迁移形式与性能评价

人们在以往的性能评价中大多注意地下水中放射性核素的无机迁移形式,而对其有机迁移形式则关注不够,这无疑会影响处置库系统性能评价的置信度。本文重点讨论了天然有机质在地下水中的分布及其对高放废物处置库系统性能评价的可能影响。最近研究结果表明:黏土岩一般为不透水层,DOC、HA和FA在黏土岩孔隙水中的质量浓度要远比在花岗岩地下水中的高。因此,对黏土岩中的预选场址要十分关注放射性核素有机迁移形式及其对性能评价的影响。花岗岩地下水中虽然DOC甚低,但是否可完全不考虑放射性核素有机迁移形式对性能评价的影响,现在未作定论,尚在进一步研究之中。     

放射性核素迁移的包气带-饱和带耦合模拟研究

为了使地下水环评结果更加真实,通过试验和拟三维方法数值模拟开展包气带-饱和带耦合模拟工作。为进一步说明包气带对核素迁移的迟滞(延迟和滞留)作用,开展了不考虑包气带的模拟并与耦合模拟结果对比。结果表明:(1)由于包气带对核素迁移的迟滞作用,吸附性较强的Se-79、Pd-107、Cs-135和Sn-126迁移至潜水面处的浓度远小于泄漏的放射性液体核素浓度,所致公众食入年待积有效剂量已小于剂量限值0.1 mSv,只有吸附性较弱的C-14所致公众食入年待积有效剂量大于0.1 mSv,需进行耦合模拟;(2)C-14在对流作用下不断向下游迁移,在弥散作用下污染范围逐渐增大,在地下水稀释及衰变、吸附作用下浓度逐渐降低。通过耦合模拟得到的地下水中放射性核素所致公众食入年待积有效剂量小于剂量限值0.1 mSv;(3)包气带对核素迁移的迟滞作用使地下水中C-14的浓度大大降低、迁移距离明显变小:地下水中C-14峰值浓度在考虑包气带时为2.15 Bq/L,不考虑包气带时为9.4×10⁴ Bq/L;事故发生后第1、5和10年,考虑包气带时C-14迁移距离分别为1.5 m、4 m和4.2 m,不考虑包气带时分别为3 m、12 m和17 m。     

高放废物地质处置库预选场址水文地质研究进展

深地质处置是目前国际上普遍接受的高放废物最终处置方案。对于这种处置方案而言，最有可能使处置库系统中放射性核素释放并进入生物圈的机制是地下水的作用。本文阐述了这种地下水的作用，包括地下水与工程屏障的相互作用、地下水在地质屏障中的核素迁移作用及核素滞留作用；介绍了处置库场址评价中水文地质研究的国际进展和动向；重点介绍了我国高放废物处置库预选场址水文地质研究进程和概况。     

地下水作用与沉积铀矿床

在同生、同成岩和外生3种主要类型沉积铀矿床的定位过程中，水文地质作用是十分重要的。在各自情况下，沉积富集铀的循环基本包括：(1)低品位蚀源区铀的淋滤或侵蚀；(2)铀由地表水或地下水迁移；(3)铀通过机械作用、地球化学或物理化学作用富集。虽然地表水对早前寒武纪铀矿床的形成有一定贡献，但在显生宙和晚前寒武纪沉积铀矿床的定位过程中，地下水作用是主要因素。在大气降水或来源较深的地下水中，铀一般通过透水砂砾石层在溶液中迁移，直到这些铀在还原条件下沉淀。同成岩矿床，典型地在还原的湖相和沼泽环境中富集，而外生铀矿床，沿矿化前锋或板状边界堆积。地下水的作用在南得克萨斯铀矿省河床沉积系统中得到很好地展示。在氧化大气水流富集铀和其他次生矿物之前，深部还原性卤水的向上迁移使主岩具备了富集条件。迁移铀的地下水与渗透含水层间的相互作用，同样反映在怀俄明早第三纪盆地的铀矿化前锋上。类似的情况可见于科罗拉多高原的板状铀矿床中。     

铀尾矿库区浅层地下水中U(Ⅵ)迁移的模拟

在详细分析中国南部某大型铀水冶尾矿库的结构特点、运营情况和库区水文地质条件的基础上，对库区水文地质条件进行概述，运用溶质反应-运移模拟软件PHREEQC-Ⅱ，建立研究区U(Ⅵ)在浅层地下水中迁移的一维溶质反应-输运耦合模型，并分析在不同时间、距离、扩散系数、弥散度等条件下铀在铀尾矿库区浅层地下水中的迁移，即铀浓度随时间及距离的变化。模拟结果与现场观测资料基本吻合，表明该软件能较好地模拟U(Ⅵ)的迁移情况，证明了该模型的可行性。研究还表明，弥散作用对铀迁移有显著影响，弥散度的取值是模拟可靠与否的关键参数，而分子扩散对本模拟的影响可忽略不计。      

共振物质的重子化学势和奇异子化学势计算

在高能重离子碰撞统计模型中，根据一定温度下的净重子密度和净奇异子密度计算出共振物质的重子化学势和奇异子化学势，并进一步分析净重子密度和净奇异子密度与重子化学势和奇异子化学势之间的关系。计算结果表明：重子化学势和奇异子化学势均随净重子密度和净奇异子密度的增大而增大，而净重子密度比净奇异子密度变化的影响要大得多。     

乏燃料后处理厂主工艺中的主要化学安全问题

水法后处理工艺过程涉及很多化学反应,反应条件和反应产物不同,需要关注的化学安全问题也不同。描述了后处理主工艺不同阶段的化学反应,分析了各阶段应关注的主要化学安全问题,为商用后处理厂的设计和事故分析提供参考。     

Simulation of chemical kinetics in sodium-concrete interactions

Sodium-concrete interaction is a key safety-related issue in safety analysis of Liquid metal cooled fast breeder reactors （LMFBRs）. The chemical kinetics model is a key component of the sodium-concrete interaction model. Conservation equations integrated in sodium-concrete interaction model cannot be solved without a set of relationships that couple the equations together, and this may be done by the chemical kinetics model. Simultaneously, simulation of chemical kinetics is difficult due to complexity of the mechanism of chemical reactions between sodium and concrete. This paper describes the chemical kinetics simulation under some hypotheses. The chemical kinetics model was integrated with the conservation equations to form a computer code. Penetration depth, penetration rate, hydrogen flux, reaction heat, etc. can be provided by this code. Theoretical models and computational procedure were recounted in detail Good agreements of an overall transient behavior were obtained in a series of sodium-concrete interaction experiment analysis. Comparison between analytical and experimental results showed that the chemical kinetics model presented in this paper was creditable and reasonable for simulating the sodium-concrete interactions.     

Chemical diffusion coefficient calculation of U3+ in LiCl-KCl molten salt

Self-diffusion coefficient denotes the intrinsic diffusion of elements without the chemical gradient; generally, it is different from the chemical diffusion coefficient that is used in Fick's law. However, the self-diffusion coefficient can be converted to the chemical diffusion coefficient by considering the concentration-dependent activity coefficient of solute. In this study, the multiple time origins method was applied to calculate the self-diffusion coefficient of U³⁺ in LiCl-KCl eutectic salt at different temperatures and concentrations. The chemical diffusion coefficient was obtained based on the calculated results and thermodynamic theory. Calculated results show that self-diffusion coefficient decreases with concentration however chemical diffusion coefficient indicates to change little initially but appears to increase followed by decrease later within the concentration range of 0–3 at%.     

Kinetic study of key species and reactions of atmospheric pressure pulsed corona discharge in humid air

In this study, we examined the key particles and chemical reactions that substantially influence plasma characteristics. In summarizing the chemical reaction model for the discharge process of N2–O2–H2O(g) mixed gases, 65 particle types and 673 chemical reactions were investigated. On this basis, a global model of atmospheric pressure humid air discharge plasma was developed, with a focus on the variation of charged particles densities and chemical reaction rates with time under the excitation of a 0–200 Td pulsed electric field. Particles with a density greater than 1% of the electron density were classified as key particles. For such particles, the top ranking generation or consumption reactions (i.e. where the sum of their rates was greater than 95% of the total rate of the generation or consumption reactions) were classified as key chemical reactions. On the basis of the key particles and reactions identified, a simplified global model was derived. A comparison of the global model with the simplified global model in terms of the model parameters, particle densities, reaction rates (with time), and calculation efficiencies demonstrated that both models can adequately identify the key particles and chemical reactions reflecting the chemical process of atmospheric pressure discharge plasma in humid air. Thus, by analyzing the key particles and chemical reaction pathways, the charge and substance transfer mechanism of atmospheric pressure pulse discharge plasma in humid air was revealed, and the mechanism underlying water vapor molecules' influence on atmospheric pressure air discharge was elucidated.     

Chemical Analysis of NO2 Removal Under Different Reduced Electric Fields

This work presents a chemical kinetic analysis of different species involved in nitrogen-oxygen mixed gas induced by stationary corona discharge at room temperature and at- mospheric pressure. This study takes into account twenty different chemical species participating in one hundred and seventy selected chemical reactions. The reaction rate coefficients are taken from the literature, and the density is analyzed by the continuity equation without the diffusion term.     

机组临时停机停堆期间的化学监督与控制

目前的化学与放射化学程序和措施,都是针对正常功率运行和按部就班有计划的大修状态而设置,如遇到机组跳堆、跳机或冷停堆等紧急情况,则没有相应的应急预案或相关程序进行提前或有目的地干预。基于这种情况,电厂化学人员经过多年的实践和不断经验反馈,总结并编写了专门针对紧急停机停堆的化学监督与控制应急预案。通过停堆过程和停堆后的不同状态,启机过程的化学与放射化学监测,监督燃料包壳状态,控制一回路的剂量水平,以防止设备腐蚀。     

用核孔滤膜净化超纯试剂的中间试验

核孔滤膜可适用于11种超纯试剂的净化。已完成了对过氧化氢、负型光刻显影剂和盐酸三种试剂的中间试验,各自达到BVI和MOS级超纯试剂水平。结果表明,自制核孔德膜可直接应用于超纯试剂工业生产上。     

Progress in understanding fission-product behaviour in coated uranium-dioxide fuel particles

Supported by results of calculations performed with two analytical tools (MFPR, which takes account of physical and chemical mechanisms in calculating the chemical forms and physical locations of fission products in UO₂, and MEPHISTA, a thermodynamic database), this paper presents an investigation of some important aspects of the fuel microstructure and chemical evolutions of irradiated TRISO particles. The following main conclusions can be identified with respect to irradiated TRISO fuel: first, the relatively low oxygen potential within the fuel particles with respect to PWR fuel leads to chemical speciation that is not typical of PWR fuels, e.g., the relatively volatile behaviour of barium; secondly, the safety-critical fission-product caesium is released from the urania kernel but the buffer and pyrolytic-carbon coatings could form an important chemical barrier to further migration (i.e., formation of carbides). Finally, significant releases of fission gases from the urania kernel are expected even in nominal conditions.     

Microscopic model for chemical etchability along radiation damage paths in solids

It would be very interesting to develop a picture about removal of atoms from the radiation damaged paths or latent nuclear tracks and undamaged bulk material in track detectors. Here, theory of chemical etching is described briefly and a new model for chemical etching along radiation damaged paths in solids is developed based on basic scientific facts and valid assumptions. Dependence of chemical etching on radiation damage intensity and etching conditions is discussed. A new parameter for etching along radiation damaged paths is introduced, which is useful for investigation of relationship between chemical etchability and radiation damage in a solid. Results and discussion presented here are also useful for further development of nuclear waste immobilization.