Study on PUREX 1B Process Simulation Based on MPMS Calculation Model
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摘要: 为模拟铀钚氧化还原萃取（PUREX）的U/Pu分离流程（简称1B流程），以多级混合澄清槽为萃取设备，以化学反应体系和经验萃取体系为基础，基于MPMS计算模型框架建立了以NH3OH+-N2H4（HAN-HYD）作为还原萃取剂的1B流程数学模型。通过对比文献数据，验证了模型的有效性。应用该数学模型探究了某低流速高酸洗涤液在特定参数条件下的1B流程中发挥的效应，结果表明该低流速高酸洗涤液的引入会降低U/Pu回收率。为进一步评估不同条件下低流速高酸洗涤液对1B流程分离效率和回收效率的影响，通过改变模型中低流速高酸洗涤液的工艺参数获得不同的U/Pu分离效果。计算结果表明，在不引入低流速高酸洗涤液的条件下，1B流程能获得最优的U/Pu分离效率。该数学模型将为基于多级混合澄清槽的1B流程工艺评估和预测等提供有益帮助。Abstract: In order to simulate the U/Pu separation (1B) process of uranium plutonium redox extraction (PUREX), a mathematical model of 1B process with NH3OH+-N2H4 (HAN-HYD) as reducing extractant was established based on the framework of MPMS calculation model, using multi-stage mixer-settler as extraction equipment, and based on the chemical reaction system and empirical extraction system. The validity of the model is verified by comparing with the literature data. The mathematical model is applied to explore the effect of a low flow rate and high acid cleaning solution in 1B process under specific parameters. The results show that the introduction of the low flow rate and high acid cleaning solution will reduce the recovery of U/Pu. In order to further evaluate the effect of low flow rate and high acid cleaning solution on the separation efficiency and recovery efficiency of 1B process under different conditions, different U/Pu separation effects were obtained by changing the process parameters of low flow rate and high acid cleaning solution in the model. The calculation results show that the optimal U/Pu separation efficiency can be obtained by 1B process without introducing low flow rate and high acid cleaning solution. The mathematical model will provide useful help for the process evaluation and prediction of 1B process based on multi-stage mixer-settler.
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Key words:
- MPMS /
- 1B process /
- Simulation /
- Model application
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图 1 水相硝酸对硝酸羟胺还原反萃Pu的影响
Figure 1. Effect of Aqueous Nitric Acid on Reduction and Stripping of Pu by Hydroxylamine Nitrate
图 2 基于18级混合澄清槽的二次洗涤1B流程
Figure 2. 1B Process of Secondary Cleaning Based on 18-stage Mixer-Settler
图 3 模拟1B流程中ρPu计算数据与实验数据对比
Figure 3. Comparison of ρPu Calculation Data and Experimental Data in the Simulated 1B Process
图 4 基于18级混合澄清槽的一次洗涤1B流程
Figure 4. 1B Process of Primary Cleaning Based on 18-stage Mixer-Settler
图 5 2种1B流程各级混合澄清槽中的ρU、ρPu比较
Figure 5. Comparison of ρU and ρPu in Mixer-Settler of Two 1B Processes
表 1 1B流程关键物质的经验萃取公式集
Table 1. Empirical Extraction Set of Key Substances in 1B Process
序号 经验萃取式 R1 ${K}_{ {\mathrm{H} }_{1} }=\left(0.1416{C}_{\rm{aq} , {\mathrm{N}\mathrm{O} }_{3}^{-} }^{0.6724}+0.006058{C}_{\rm{aq} ,{\mathrm{N}\mathrm{O} }_{3}^{-} }^{3.418}\right)(1-0.54{\mathrm{e} }^{-15F})$ R2 $ {K}_{{\mathrm{H}}_{2}}={K}_{{\mathrm{H}}_{1}} $ R3 $\begin{array}{l}{K}_{\mathrm{U}\left(\mathrm{V}\mathrm{I}\right)}=\left(5.284{C}_{\rm{aq} ,{\mathrm{N}\mathrm{O} }_{3}^{-} }^{1.582}+1.557{C}_{\rm{aq} , {\mathrm{N}\mathrm{O} }_{3}^{-} }^{3.843}+0.01267{C}_{\rm{aq} , {\mathrm{N}\mathrm{O} }_{3}^{-} }^{7.447}\right)\\ \qquad\quad\;\;\;\left(4{F}^{-0.17}-3\right)\end{array}$ R4 ${K}_{\mathrm{P}\mathrm{u}\left(\mathrm{I}\mathrm{I}\mathrm{I}\right)}=0.04{C}_{\rm{aq} , {\mathrm{N}\mathrm{O} }_{3}^{-} }^{1.8}+0.000156F{C}_{\rm{aq} ,{\mathrm{N}\mathrm{O} }_{3}^{-} }^{7}$ R5 ${K}_{\mathrm{P}\mathrm{u}\left(\mathrm{I}\mathrm{V}\right)}={K}_{\mathrm{U}\left(\mathrm{V}\mathrm{I}\right)}\left(0.3429+0.009552{C}_{\rm{aq} , {\mathrm{N}\mathrm{O} }_{3}^{-} }^{2.154}\right)$ R6 ${K}_{ {\mathrm{H}\mathrm{N}\mathrm{O} }_{2} }=24.8{C}_{\rm{aq} ,{\mathrm{H} }_{}^{+} }^{-0.28}-3.209{C}_{\rm{aq} ,{\mathrm{H} }_{}^{+} }^{-0.653}$ Ki—物质i在有机相和水相的分配比；F—有机相中萃取剂TBP的体积比；下标H1、H2—HNO3与TBP结合的2种形态：HNO3TBP1、HNO3TBP2；Caq,i—反萃后萃余相中物质i的摩尔浓度，mol/L 
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表 2 不同流速高酸洗涤液工艺条件下，1B流程萃取相和萃余相中U、Pu质量浓度
Table 2.
Mass Concentrations of U and Pu in the Extraction Phase and Residual Phase of 1B Process under the Process Conditions of High Acid Cleaning Solution at Different Flow Rates 流速/(mol·min−1) ${ {\;\rho }_{\mathrm{U} } }_{\mathrm{o}\mathrm{r}\mathrm{g} }$/(g·L−1) ${\;\rho }_{\mathrm{P}{\mathrm{u} }_{\mathrm{o}\mathrm{r}\mathrm{g} } }$/(10−7g·L−1) ${\;\rho }_{ {\mathrm{U} }_{\mathrm{a}\mathrm{q} } }$/(10−7g·L−1) ${\;\rho }_{\mathrm{P}{\mathrm{u} }_{\mathrm{a}\mathrm{q} } }$/(10−2g·L−1) $\varphi$/1010 ${\;\mu }_{\mathrm{U} }$ ${\;\mu }_{\mathrm{P}\mathrm{u} }$ $\;\mu$ 0 0.2675 9.212 6.347 7.734 3.5378 0.9973 0.9822 0.9795 0.1 0.2675 13.84 4.301 7.629 3.4295 0.9974 0.9806 0.9780 0.2 0.2675 13.63 3.066 7.526 4.8178 0.9974 0.9790 0.9765 0.3 0.2675 14.30 2.279 7.441 6.1092 0.9974 0.9795 0.9770 0.4 0.2675 6.665 1.759 7.338 1.6743 0.9975 0.9772 0.9748 0.5 0.2675 6.184 1.399 7.251 2.2419 0.9975 0.9770 0.9746
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