反应堆中气体裂变产物释放问题的研究

在对反应堆气体裂变产物的研究中,需要了解作为固体裂变产物子体的氪、氙气体的释放率问题.本文对有较长半衰期前驱物的135Xe的测量数据进行了具体分析,根据在不同取样时间下分析所得的裂变反应事件数量应一致的原则,得到哪种释放模型更符合真实情况的结论.以期能对释放问题给出一个有价值的参考意见.     

事故情况下裂变产物从核燃料中的释放

过去研究中源项估计过高,可安全地降到更现实的值。影响裂变产物从核燃料中释放的因素很多,要精确预测裂变产物的释放率是困难的,还需做许多工作。     

气体裂变产物的活度计算

从裂变产物的衰变规律出发，导出了利用HPGeγ谱仪测量的裂变产物γ峰计数计算裂变产物零时刻总核数的公式。利用该公式计算了^239Pu裂变产生的气体裂变产物。^85Kr^m,^87K4,^88Kr^88Kr,^133Xe^m,^133X3,^135Xe^m,^135Xe和^133Xe的核数目随时间的变化关系，并计算了距相对效率为60％的HPGe探测器表面25cm处各气体裂变产物γ峰计数率变化，为气体裂变产物的实验分析提供了参考。     

气体裂变产物的动态计算方法

与利用导出公式得出裂变产物核数目随时间的变化关系不同,本文从放射性的几率衰变规律出发,对已知初始状态的衰变链,将时间推移矢量分为若干时间微元,在每一个时间微元以上一个时间微元为基础使用计算机程序计算衰变链上每个核素的动态数目,直至计算到目标时间点.最后模拟化学取样和物理测量的实际过程,得出一个可用于裂变发生数诊断的计算过程.     

一个放射性氪、氙净化装置简介

本文介绍了放射性氪、氙净化装置的功用、特性和概况。实验数据表明,活性炭吸附氪的透过时间计算方法是正确的。     

高浓铀快堆裂变产物的反应性效应及假想裂变产物的等效方法

本文利用高浓铀快堆燃耗近似计算方法对230种裂变产物进行了非均匀燃耗计算。以裂变产物的反应性效应为依据,研究了三种假想裂变产物的等效方法。我们推荐其中一种等效方法,它将所有裂变产物等效成两种假想裂变产物,其反应性效应在整个燃耗过程中的最大误差仅约2%。     

燃料氧化对裂变产物扩散释放的影响研究

分析燃料氧化对裂变产物扩散释放的影响,得出结论:燃料氧化后,燃料中铀原子空位增多对裂变产物释放的影响要大于导热率降低后燃料温度上升带来的影响;裂变产物释放份额随氧铀比升高而增大,燃料棒线功率密度越高,效应越明显。     

氢型丝光沸石在净化和回收裂变惰性气体氪、氙中的应用

氢型丝光沸石具有良好的除水和除氮氧化物的性能。为了检验它是否可用于净化和回收裂变惰性气体氪、氙前的预处理,进行了本试验。实验表明,在吸附过程中当 NO_2穿透吸附器时,氢型丝光沸石对~(85)Kr 仅有微量的吸附,在解吸时又能全部被解吸下来。操作循环过程中吸附器内没有~(85)Kr 的积累。结论认为,从溶解器排气中净化和回收裂变惰性气体氪、氙的流程中用氢型丝光沸石吸附器作为除水和氮氧化物的预处理手段是可行的。     

HPGe测量气体裂变产物中微量123Xe的理论模拟

利用MCNP模拟计算了大量气体裂变产物中微量123Xe的HPGeγ能谱,分析了气体裂变产物对123Xe测量的影响,结果表明:直接测量气体样品中的123Xe是不可能的,但可以通过测量其子体123I来推算123Xe,推荐的测量方法是:对原始气体样品不做Kr/Xe分离,衰变6.59 h后,将气体去除,再衰变2 h后,采用HPGe测量123I。     

Fission Product Gas Release in Burst Region of Uranium Monocarbides

Uranium enrichment in a thermally driven countercurrent gas centrifuge is studied theoretically on the basis of dander's separation theory and the short-bowl flow solution proposed recently by Sakurai and Matsuda. The separation factor is computed and compared with experimental results by Groth. Agreement of the computed results with experiment is fairly good, except for very low feed rates. Further improvements are discussed.     

干馏法从铀的裂变产物中分离131I

¹³¹I是一种重要的医用放射性同位素,但因湿法分离技术上的缺陷,使得从铀裂变产物中获取¹³¹I的工艺具有环境污染严重、提取效率低的缺点。因铀裂变产物中¹³¹I的产额较高,为拓展¹³¹I的获取途径,提高铀裂变产物的利用效率,开展铀裂变产物中¹³¹I分离的新工艺研究十分必要。与传统湿法分离工艺不同,本工作采用了干馏法进行铀裂变产物中¹³¹I的分离。为了得到高的¹³¹I分离效率,将分离过程分为低温粉化、高温干馏和中低温保温三个阶段,并研究高温干馏阶段温度对131I分离效率的影响。实验发现：当干馏温度高于950 ℃时,¹³¹I的分离效率≥98%。此外,研究结果还表明,在该干馏温度下,碘和¹⁰³Ru 均可挥发出铀靶片,但产物收集液中却仅含有碘。为了解释这一现象,对碘的分离过程进行分析,结合实验结果和理论计算,推测挥发物中碘和¹⁰³Ru分离的原因为：¹⁰³Ru与氧反应生成挥发性RuO₄,从铀的裂变产物挥发出;因加热管内温度较高,RuO₄在迁移过程中发生了分解,生成RuO₂沉积在加热管内部。因此,利用干馏法从铀的裂变产物中分离¹³¹I时,为了得到放化纯度高的碘产品,不仅要合理规划分离过程,还需科学设计加热管的长度。     

低温下活性炭吸附分离Kr和Xe

研究了低温下活性炭吸附分离Kr和Xe的方法。Kr和Xe混合气在-78 ℃活性炭吸附柱上进行富集,根据Kr、Xe在活性炭柱上脱附条件的差异实现了Kr和Xe的分离。结果表明,Kr和Xe的回收率均大于90%,Kr样品中Xe的去污系数达10⁴以上,Xe样品中Kr的去污系数达10³以上。     

Release Behavior of Fission Gas from Coated Fuel Particles under Irradiation

TRISO coated fuel particles for HTGR were irradiated by two sweep gas capsules in order to study the release behavior of the fission gas and try to predict the failure fraction of the particles on the basis of the measurement. For verification of the predicted failure fraction, post irradiation examination was conducted, and failure fraction in a visual inspection and acid leaching fraction were measured. Agreement between the predicted failure fraction and the acid leaching fraction was good for these samples except one. From the release behavior from the intact particles, in-pile diffusion coefficients of Kr in LTI-PyC were estimated and expressed as D=(2.9–6.0)×10⁴exp(-2.55×10°/RT) (cm²/s), where R ids the gas constant (=8.314 J/K) and T the absolute temperature. It was recognized that the release from failed particles was controlled by diffusion at 1,600°C and that from intact particles, predominantly by recoil at 1,400°C.     

HPGe测量气体裂变产物中微量77Kr的可行性分析

针对气体裂变产物中微量⁷⁷Kr的测量问题,利用MCNP模拟计算了气体裂变产物对⁷⁷Kr的影响。结果表明,HPGe不可能直接测量气体样品中的⁷⁷Kr,但可通过测量其子体⁷⁷Br来推算⁷⁷Kr。     

Effects of Temperature Cycling and Heating Rate on Fission Gas Release of BWR Fuels

The effects of temperature cycling and heating rate on the release behavior of ⁸⁵Kr have been studied for U0₂ pellets irradiated in a commercial BWR during 3 and 4 cycles (burn-up: 23 and 28GWd/t), by using a post irradiation annealing technique. In addition, characteristics of intergranular bubbles in base-irradiated and annealed specimens (burn-up: 6~28GWd/t) have been examined by SEM fractography.

No significant difference in the release of ⁸⁵Kr was observed between the cyclic heating from 700 to 1,400°C and isothermal heating at 1,400°C. The maximum release rate of ⁸⁵Kr during heating up to 1,800°C became lower with decreasing heating rate in the range of 0.03–10°C/s, while its cumulative fractional releases were about 20~30%, almost independent of heating rate. The fractional coverage of the grain face area occupied by intergranular bubbles saturated around 40~50 for the specimens annealed at 1,600-1,800°C, independent of specimen burn-up and heating conditions (temperature, heating rate and duration). A relationship between intergranular bubble concentration N_g per unit area of grain face and average bubble diameter d_g was expressed as N_g∝d_{g 2.1}     

Fission Products Release from Irradiated FBR MOX Fuel during Transient Conditions

Out-of-pile experiments on the release of fission products (FPs) under transient heating conditions were carried out for mixed oxide fuels. The fuels used in the experiments, the plutonium content of which was 30 wt%, were irradiated up to 65 GWd/t in the experimental fast reactor JOYO. The experiments consisted of two runs, FP-1 and FP-2. In FP-1, the fuel sample was first heated to 2,000°C and then up to 3,000°C. The holding time was 30 min at each temperature. In FP-2, the terminal temperatures were 1,500°C and 2,500°C, and the holding time was 30 min in the same manner.

The release ofCs, a volatile FP, was detected as soon as the fuel sample was heated up. The release rate, after peaking in several minutes, decreased gradually via a diffusion process in the fuel matrix. The “gross” diffusion coefficient agreed well with the data reported in other experiments using LWR fuels. The release fractions were identical in both experiments, namely Cs ～100%, Sb ～100%, Ru ～10%, Ce ～0% and Eu ～0%.     

快中子诱发裂变测定铀同位素丰度

铀同位素丰度分析是核燃料循环中重要的分析项目。本工作在中子活化基础上提出用T(d,n)⁴He反应产生的快中子诱发裂变铀样品来测定铀同位素丰度的分析方法。该方法利用铀同位素丰度与特定裂变产物的平均产额比呈指数关系的特点,选择〖AKY-〗(⁹²Sr)/〖AKY-〗(¹⁰⁵Ru)、〖AKY-〗(⁹²Sr)/〖AKY-〗(¹³⁵I)与铀同位素丰度间的关系曲线作为工作曲线,并对模拟样品进行分析。结果表明,〖AKY-〗(⁹²Sr)/〖AKY-〗(¹⁰⁵Ru)、〖AKY-〗(⁹²Sr)/〖AKY-〗(¹³⁵I)计算结果与模拟样品的相对偏差分别为0.8%和1.8%,RSD优于3%,与γ能谱法的分析结果相符合。     

电沉积铀靶制备技术研究

研究了在水溶液体系中采用电沉积法制备铀靶的方法。以0.15mol/L草酸铵为电解液,铂丝为电极,通过考察阴极处理工艺、电流密度、电沉积时间、pH、温度、搅拌速度、镀液中UO2(NO3)2浓度等对电沉积效率及镀层质量的影响,确定了制备电沉积铀靶的最佳工艺参数,其中,沉积效率通过紫外分光光度法测得。在pH=2～3、电流密度60mA/cm2、保持温度60℃、镀液中UO2(NO3)2浓度约1.67mg/mL时沉积效率可达约98%。采用红外光谱、X射线能谱和扫描电镜等对铀沉积层进行了测试。结果显示,铀以水合聚合物的形式存在,可能的结构为[UO2(H2O)4-O-UO2(H2O)4-O],铀的沉积层的纯度较高,除检测到铀(65.35%)、氧(27.38%)、碳(5.46%)和铂(1.81%)外未引入其他杂质,镀层表面平整、致密,与衬底结合牢固。单次铀的电沉积层厚度可达6mg/cm2,采用高温烧结后重复电镀的方法可将电沉积铀的密度提高到6～8mg/cm2。     

Diffusion and Evaporation of Fission Products in Coated Fuel Particles

Fractional releases of ¹³³Xe, ¹⁴⁰Ba and ⁸⁹Sr from slightly-irradiated pyrolytic-carbon-coated and SiC-coated particles were measured over a temperature range of 1,200°–1,750°C. The results are analyzed mathematically in order to obtain the diffusion and evaporation coefficients relevant to PyC and SiC. The resulting expressions for the coefficient of diffusion in PyC are 2.9x10-⁷ exp(-61x10³/RT) for ¹³³Xe and 4.7x10-² exp(51x10³/RT) for ¹⁴⁰Ba. For the coefficients of evaporation of ¹⁴⁰Ba from PyC, the expression is 3.5x10³ exp(-42x10³ /RT). As for SiC, the diffusion and evaporation coefficients of these nuclides are given for a temperature of 1,750°C. A high diffusivity path for the diffusion of ¹⁴⁰Ba is postulated to explain the difference in diffusion behavior between ¹³³Xe and ¹⁴⁰Ba in PyC.