Development and Validation of a Flowsheet Simulation Model for Neptunium Extraction in an Advanced PUREX Process

An Advanced PUREX process has been developed for separation and recycling of neptunium from spent nuclear fuel. This work presents a new flowsheet simulation model for the extraction of neptunium using centrifugal contactors, where mass transfer is modeled using two-film theory and a linear driving force. Distribution coefficients and neptunium redox reactions are modeled using published models. Mass transfer between the organic and aqueous phases in the phase separation zone is shown to have a negligible effect. The model is applied to a previously tested flowsheet and its predictions are shown to be in good agreement with the experimental results.     

A Remark to a Formula in K. Ishimatsu's Paper on “Continuous γ-ray Spectrometry with Scintillation Counters”

Spatial distribution of the Cd-ratio of Au foils were measured for various lattice pitches in a natural uranium-light water system. Comparison of the experimental results with theoretical calculation using the THERMOS-code shows some divergence of the theoretical Cd-ratio toward larger than experimental values in the fuel rod.     

TBP-TEVA萃取色层分离-α能谱法测定辐照镎靶溶解液中痕量236Pu的可行性

²³⁶Pu的含量控制是钚热源的一项重要参数,通过α能谱准确测量镎靶溶解液中痕量²³⁶Pu,建立镎靶辐照靶件溶解液中钚的分离方法。根据杂质组成特点采用TBP-TEVA萃取色层双柱分离,用氨基磺酸亚铁以及亚硝酸钠对钚进行调价,对靶件溶解液中的Al、Fe、U、Th和Np等进行分离,去污系数均大于10⁴,钚的回收率为90.7%。研究大量²³⁸Pu对α能谱测定²³⁶Pu的干扰,结果表明,大量²³⁸Pu会造成仪器本底升高,²³⁸Pu能谱峰分辨率降低;在7 500 Bq ²³⁸Pu干扰下,测量4.3 h 时,²³⁶Pu的最小可检测活度为1.20×10^-2 Bq（当量质量为6.11×10^-16 g）。计算结果表明,镎靶溶解液样品中钚的同位素比值n(²³⁶Pu)/n(²³⁸Pu) ≥4.63×10^-8时,取合适的样品量使得电沉积源中²³⁸Pu 活度在 450~7 500 Bq范围内,均可测量其中的痕量²³⁶Pu,同时可准确测定同位素比值n(²³⁶Pu)/n(²³⁸Pu)。     

镎在北山五一井水中的溶解度计算分析

环境放射化学种态分析软件利用实验测定的感兴趣元素的热力学数据,根据所研究体系的组分及相应的分析浓度,从数据库中搜索由这些组分经化学反应可能生成的物种及相应的平衡常数,计算各种元素可能存在的化学种态和平衡浓度,从而得到相应元素在所研究体系中的化学种态分布.本工作利用北京大学编写的环境放射化学种态分析软件CHEMSPEC计...     

Actinide Third Phase Formation in 1.1 M TBP/Nitric Acid/Alkane Diluent Systems

Abstract

Additional information on the organic phase speciation of Np and Pu was obtained in order to further understand the impact on third phase formation. In the Np(VI) extraction system, indications of the presence of a species associated with the absorbance at 1210 nm appears to be consistent with an increased tendency for third phase formation. Attempts to couple this absorption peak to a higher order nitrate species were inconclusive, and further study is required. For Pu(VI), continued evidence has emerged suggesting a role of higher order nitrate species in third phase formation.     

百克量级花岗岩中痕量镎的分离纯化方法研究

镎的高生物毒性和长半衰期（t_1/2＝2.14×10⁶ a）以及在环境中易迁移的性质,使之成为环境放射性污染普查及核设施监测过程中主要关注的核素之一。本文利用酸式消解法实现了百克量级花岗岩的全溶解。以自制的DMDODGA/CMG20树脂作为分离材料,利用其对氢氟酸中镎的吸附特性,建立了大体积溶解液中痕量镎的富集-分离流程。同时采用Dowex 1×4阴离子交换树脂进一步实现了对镎的浓缩和纯化。在此基础上,提出了百克量级花岗岩的分离流程,并对流程进行了实验验证。结果表明,花岗岩溶解液澄清、无残渣,分离流程对镎的回收率为87.6%,对岩石基体元素和铀的去污因子均大于1.0×10⁵。     

Measurements of gamma-ray emission probabilities of 241, 243Am and 239Np

Gamma-ray emission probabilities of ^{241, 243}Am and ²³⁹Np have been precisely measured with gamma- and alpha-ray spectroscopic methods. The activities of the samples were determined by measuring alpha particles using a Si semiconductor detector. Gamma rays emitted from the samples were measured with a planar type High-Purity Germanium (HPGe) detector. An efficiency curve of the HPGe detector was derived with uncertainties from 0.7% to 2.5% by combining measured efficiencies and Monte Carlo simulation. The gamma-ray emission probabilities for the major gamma rays of these nuclides were determined with uncertainties less than 1.2%.     

Minor actinide transmutation in fast reactor metal fuels irradiated for 120 and 360 equivalent full-power days

An irradiation experiment on uranium–plutonium–zirconium (U–Pu–Zr) alloys containing 5 wt% or less minor actinides (MAs) and rare earths was carried out in the Phénix fast reactor. The isotope compositions of the fuel alloys irradiated for 120 and 360 equivalent full-power days (EFPDs) were chemically analyzed by inductively coupled plasma–mass spectrometry after 3.3–5.3 years of cooling. The results of chemical analysis indicated that the discharged burnups of the fuel alloys irradiated for 120 and 360 EFPDs were 2.1–2.5 and 5.3–6.4 at%, respectively. The changes in the isotopic abundances of plutonium, americium, and curium during the irradiation experiment were assessed to discuss the transmutation performance of MA nuclides added to U–Pu–Zr alloy fuel. Multigroup three-dimensional diffusion and burnup calculations accurately predicted the changes in these isotopic abundances after fuel fabrication. An evaluation of the MA transmutation ratio based on the results of chemical analysis revealed that the quantity of MA elements in the U–19Pu–10Zr–5MA (wt%) alloy decreased by about 20% during the irradiation experiment for 360 EFPDs.     

NpO_2~+与UO_2~(2+)阳阳离子络合对Np(Ⅵ)/Np(Ⅴ)表观电位及可逆性的影响

通过分光光度法考察了阳阳离子络合物的形成,并研究了不同酸度和不同U(Ⅵ)浓度对Np(Ⅵ)/Np(Ⅴ)表观电位及其可逆性的影响。结果表明:溶液中U(Ⅵ)的存在会影响Np(Ⅵ)/Np(Ⅴ)的表观电位;随着U浓度的不断升高,Np(Ⅵ)/Np(Ⅴ)表观电位不断升高,同时该氧化还原反应的可逆性逐渐变差;随着溶液中酸度的提高,Np(Ⅵ)/Np(Ⅴ)表观电位不断降低。