Fuel cycle strategies and plutonium management in Europe

An overview of current nuclear power generation and fuel cycle strategies in Europe is presented, with an emphasis on options for the management of separated plutonium in the medium to long term. Countries which have opted for reprocessing of spent fuel have had to contend with increasing inventories of separated plutonium. Of the various potential options for utilisation or disposition of these stockpiles, only light water reactor (LWR) mixed-oxide (MOX) fuel programmes are sufficiently technologically mature to be fully operational in several European countries at present. Such reprocessing-recycling programmes allow for a stabilisation of the overall separated plutonium stocks, but not for a significant reduction in the stockpile. Moreover, the quality of recycled plutonium decreases at each potential step of re-irradiation. Therefore, optimised or new ways of managing the plutonium stocks in the medium to long term are required. In the present overview we consider the most promising options for reactor utilisation of plutonium in both near-term future reactor and Generation IV systems.     

含钚材料恐怖事件的后果分析

基于数值仿真计算手段,定量分析了含钚材料恐怖事件中炸药爆炸条件下钚材料气溶胶的转化份额;针对不同可吸入气溶胶比例,应用HotSpot核事故后果评价模型计算了有关辐射特征量。结果表明,不同可吸入气溶胶比例对于辐射危害防护及处置有着明显的影响。     

乙异羟肟酸改善Purex流程铀产品中U-Pu的分离

研究采用新的无盐络合剂乙异羟肟酸（ＡＨＡ）来改善Ｐｕｒｅｘ流程铀线Ｕ－Ｐｕ分离。萃取及洗涤体系中Ｐｕ（Ⅳ）及Ｕ（Ⅵ）的分配实验结果表明：ＡＨＡ能够很好地络合Ｐｕ（Ⅳ）,它既能抑制水相中Ｐｕ（Ⅳ）被３０％ＴＢＰ／ＯＫ萃取,又能有效地把萃取到３０％ＴＢＰ／ＯＫ中的Ｐｕ（Ⅳ）洗涤到水相。同时,ＡＨＡ的存在不影响３０％ＴＢＰ／ＯＫ对Ｕ（Ⅵ）的萃取。     

环境土壤样品微波消解及钚的ICP-MS测量

钚是环境放射性污染调查和核事故应急监测重点关注的污染核素,土壤样品中钚的定量分析包括样品消解、化学分离和仪器测量等3个步骤。为缩短样品消解时间、提高化学分离效率,对土壤样品微波消解和钚的阴离子交换分离进行了研究,建立了微波消解-阴离子交换分离-电感耦合等离子体质谱（ICP-MS）测量 同位素稀释法定量分析污染土壤样品中²³⁹Pu的流程。以6 mol/L盐酸为浸取试剂,在浸取液体积与土壤质量之比为4∶1~5∶1 mL/g时,5 g土壤样品中²³⁹Pu的加标回收率大于99%。以氢氟酸、硝酸和盐酸的混酸为消解试剂,在氢氟酸浓度为13.2 mol/L时,1 g土壤样品中²³⁹Pu的加标回收率大于94%。用所建流程测得的IAEA-375土壤标准样品中²³⁹Pu的含量与参考值无显著差异,该流程对1 g土壤样品中²³⁹Pu的检出限为84 mBq/kg。     

钚及其裂变产物钯 、银 、镉 、锡 、锑 、锆的系统分离方法

描述了钚及其6种裂变产物钯、银、镉、锡、锑、锆的系统分离方法：在强碱性阴离子交换树脂柱上将盐酸介质的辐照靶溶解液中的这些元素分为5组,然后再针对各组目标元素进行分离和纯化,可简便快速地从同一份靶溶解液中分离以上7种元素。采用辐照铀靶对分离方法进行了验证,结果表明,分离流程对6种裂变产物的化学回收率均大于70%,对γ谱仪测量干扰的主要核素去污因子均大于1.0×10³,可满足²³⁹Pu裂变谷区核素裂变产额测量对化学分离的要求。     

离子色谱分离-峰面积比值法测定核燃料元件中的钚

建立了用离子色谱法和峰面积比值法分离U并测量核燃料元件中钚的方法。该方法可以消除铀等基体的干扰,色谱条件在一定范围内变化时对测量结果无影响。在一定色谱条件下,通过实验获得相同含量的钚铀峰面积之比后,实际测量时可不采用钚标准溶液对仪器进行校准。方法的检出限为0.05 mg/L。该方法适用于各种乏燃料元件中钚含量的测定。     

Corrosion of Type 304L Stainless Steel in Concentrated Plutonium Nitrate Solution

Dryout experiments of water have been conducted in an annulus with inside heating (heat flux from inner wall only) under high-pressure, low-flow and mixed inlet conditions which are of importance in the core thermal-hydraulic behavior during a loss-of-coolant accident (LOCA) and also partially during an anticipated transient without scram (ATWS) of a nuclear reactor. The experimental conditions have covered ranges of pressure of 3 MPa, mass flux from 105 to 320 kg/m²·s and inlet quality from 0.15 to 0.90. The dryout data have been compared with several existing empirical critical heat flux (CHF) correlations and a new correlation. The Katto correlation predicts best the CHF among the existing correlations examined. However, even the Katto correlation overpredicts the CHF by factors up to 2 at about 1/6 data points of the present dryout data. The present dryout data are divided into two groups (regions) according to the value of a non-dimensional number l _bo/d _he, where l _bo is the assumed boiling length and dh, the heated equivalent diameter. A new correlation covering both the regions has been developed by correlating the present dryout data in terms of two non-dimensional numbers. The new correlation performs best among the correlations examined in predicting the present dryout data.     

Re-evaluation of the phase relationship between plutonium and zirconium dioxides

The phase relationship between ZrO₂ and PuO₂ was examined in a low PuO₂ content region, from 3.1 to 11.2 mol% PuO₂, at temperatures between 1273 K and 1473 K, by high temperature X-ray diffractometry. The measurements were carried out in air. At 1273 K, the samples in this composition range consisted of two phases, monoclinic and cubic. Another phase, tetragonal, was observed at 1373 K. The low temperature monoclinic phase disappeared at 1473 K. It was confirmed that the monoclinic phase disappears around 1463 K; the disappearance temperature does not depend on the composition of the sample. It was, thus, inferred that there should be a eutectoid line in the phase diagram. Though the eutectoid point is not clear, the PuO₂ content at the point should be less than 3.1 mol%.     

Purex流程铀钚分离工艺单元数学模型研究

在铀钚分离工艺单元单级数学模型和混合澄清槽瞬态数学模型的基础上,建立了以U(Ⅳ)-N₂H₄为还原反萃剂、混合澄清槽为萃取设备的Purex流程铀钚分离工艺单元数学模型,开发了计算机模拟程序,并使用台架实验数据对程序的可靠性进行了验证。结果表明,模拟程序的计算值和实验值符合良好。在此基础上,利用模拟软件对铀钚分离工艺单元的工艺参数进行了计算分析,结果表明：1BX₁加入位置、1BS和1BX₂酸度对钚反萃率无太大影响,但1BX₁加入位置和补萃级数对钚中去铀系数SF_U/Pu有一定影响。     

絮凝沉淀处理含盐量较高的铀、钚低放废水

针对含盐量较高的低放废水开展了絮凝沉淀处理技术研究.结果表明,钚在碱性条件下可被有效去除,增大絮凝剂投加量及降低废水初始pH可以提高铀的絮凝效果.pH的控制是获得铀的高去除率的关键.当Fe2 投加量为100 mg/L、废水初始pH为6时,铀的去除率可达95.5%以上.采用两次絮凝沉淀的方法,第二次沉淀时调节pH<7.0,Fe2 投加量控制在80 mg/L左右,可以使出水铀质量浓度降到10 μg/L以下.