高酸Purex流程镎走向控制及其回收纯化工艺研究

文章介绍用逆流萃取串级实验方法研究高酸Purex萃取流程lA萃取器镎走向控制(与铀、钚共萃取)及自lAP中定量反萃镎、分离铀、钚工艺条件的实验结果。     

Solvent Extraction Calculation Model for Purex Process in Pulsed Sieve Plate Column

A new calculation code PULCO has been developed to simulate the Purex extraction process in a pulsed column. The model for the PULCO code is based on the mass transfer taking place at the interface between dispersed drops and continuous phase fluid. The following physical quantities of the moving drop are included in the model for each period of drop motion in a pulsed column:

1. Mass transfer coefficient from liquid drop to continuous phase

2. Diameter and velocity of moving drop in the pulsed column

3. Holdup of dispersed and continuous phases in the pulsed column

4. Longitudinal dispersion coefficient in the pulsed column.

To establish the validity of the PULCO code, experiments were performed using a 50 mm diameter pulsed column which had a sieve plate section height of 2 m and plates spaced 50 mm apart. The experiments were performed by CY tests with use of unirradiated U and Pu. The experimental concentration profiles fitted well with the calculated concentration profiles.     

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。     

Axial Dispersion Coefficient and Mass Transfer Rate in Pulsed Column

This work has investigated an improvement for the usual batch denitration by formic acid. It studied several destruction characteristics of nitric acid and formic acid in a continuous denitration process newly suggest in this work which consisted of a continuous denitration by formic acid and a residual acid-electrolytic destruction system. Also, the precipitation behaviors of a few metal ions such as Mo, Zr, Nd, and Fe during the denitration were investigated. The continuous denitration by formic acid reached a steady state in 30 min and showed a dependency of the final acidity on the residence time of the feeding solution in the reaction. In a Ti-IrO₂ electrolytic cell, the destructive rates of formic acid and nitric acid were 1.37×10^-2M-cm²/h-mA and 9.33×10^-3 Mcm²/hmA, respectively. The nitric acid was reduced at the Ti cathode and the formic acid was oxidized at the IrO₂ anode. The suggested denitration process combining a chemical system and an electrolytic system could treat continuously a feeding nitric acid of 2.0 M below about 0.1 M. The precipitation of the metal ions occurred almost totally in the denitration column.     

Purex过程中Np与HNO_2、HNO_3的反应

文章综述了Ｎｐ在Ｐｕｒｅｘ过程中与ＨＮＯ２、ＨＮＯ３的反应。在水相ＨＮＯ３及有机相ＴＢＰ中，ＮＰ（ＶＩ）可被还原为ＮＰ（Ｖ），ＮＰ（Ｖ）又可被氧化为ＮＰ（ＶＩ），且相互之间存在着平衡。在α、β，γ等射线辐照下，亦发生一系列氧化还原反应。     

微量锆在钚纯化循环中的行为

研究了相接触时间、相比、硝酸浓度对锆萃取性能的影响,并通过台架试验研究了流比、料液酸度、洗涤级数、萃取级数、铀浓度对Pu产品中Zr净化效果的影响。结果表明:流比(2AF∶2AX)、料液(2AF)中HNO3浓度、洗涤级数对Zr的净化具有显著的影响,而铀浓度对Zr的净化效果影响有限。台架温试验证明,选择的优化工艺可以满足Pu的收率和Pu产品中Zr的净化因子大于100的要求。     

硝酸羟胺对Pu(Ⅳ)的单级还原反萃数学模型研究

硝酸羟胺是Purex流程钚纯化过程的还原剂。本文建立了30%TBP/正十二烷体系中硝酸羟胺还原反萃Pu(Ⅳ)的单级迭代计算数学模型,并提出了相应的数学算法,编写了模拟连续逆流萃取器中的一级的计算机模拟程序,使用文献数据对模型和程序进行了验证。结果表明:模型计算值与文献实验值符合良好;本文模型计算结果的准确度高于文献模型。最后分析了计算时间单元长度对准确度的影响。     

Development of COMPAS,Computer Aided Process Flowsheet Design and Analysis System of Nuclear Fuel Reprocessing

A computer aided process flowsheet design and analysis system, COMPAS has been developed in order to carry out the flowsheet calculation on the process flow diagram of nuclear fuel reprocessing. All of equipments, such as dissolver, mixer-settler, and so on, in the process flowsheet diagram are graphically visualized as icon on a bitmap display of UNIX workstation. Drawing of a flowsheet can be carried out easily by the mouse operation. Not only a published numerical simulation code but also a user's original one can be used on the COMPAS. Specifications of the equipment and the concentration of components in the stream displayed as tables can be edited by a computer user. Results of calculation can be also displayed graphically. Two examples show that the COMPAS is applicable to decide operating conditions of Purex process and to analyze extraction behavior in a mixer-settler extractor.     

Decomposition of Solvent Extraction Media during Nuclear Reprocessing: Literature Review

Abstract

Reprocessing spent nuclear fuel is indispensable for the economical use of uranium in nuclear energy production, and has been used industrially for more than 40 years. These processes involve the use of an extractant/diluent (solvent) for separation of the reusable actinides from unwanted fission products. The most widely used processes employ tributyl phosphate (TBP) diluted with normal-paraffin hydrocarbon. However, on repeated use, the solvent becomes degraded due to thermal, radiolytic, and chemical attacks, resulting in chemical as well as physical damage. In view of the considerable expansion in the knowledge and understanding regarding the chemical and radiolytical decomposition of both TBP and the hydrocarbon diluent, an up-to-date review seemed appropriate. This review is concerned mainly with the mechanisms of the degradation of the solvent system. Schemes of TBP and diluent radiation-chemical transformations occurring on decomposition of the solvent system are presented.