乏燃料后处理批次式溶解器数学模型及算法研究

Research on Mathematical Model and Algorithm of Batch Dissolverfor Spent Fuel Reprocessing

  • 摘要: 针对乏燃料后处理批次式溶解器中剪切-溶解联动操作缺乏数学模型与动态仿真分析的问题,基于物料守恒建立了剪切-溶解联动过程的数学模型,并基于Python语言搭建了数值仿真平台,实现了多种工艺条件下乏燃料剪切和溶解过程的动态模拟。仿真结果表明,在二氧化铀质量为523.4 kg、反应温度为95 ℃、硝酸浓度为6.1 mol/L的典型工况下,默认表面积修正因子为1,系统约于234 min时达到出料要求,而达到平衡所需的时间约为800 min,平衡时溶液中铀浓度为318.81 g/L、硝酸浓度为1.41 mol/L、溶解率为99.15%。与理论数据相比,仿真结果的相对误差为0.007 2%,模拟过程中各溶质浓度变化趋势与实际反应过程高度一致,验证了所建模型的准确性与数值模拟的稳定性。灵敏度分析结果显示,初始硝酸浓度对铀离子浓度的影响显著高于表面积修正因子,且二者灵敏度随反应进程整体呈下降趋势。研究表明,构建的动态仿真模型能够有效刻画批次式溶解器的动力学行为,具有良好的工程适用性和通用性,可为乏燃料后处理工艺优化与参数设计提供可靠的理论和数据支持。

     

    Abstract: Spent fuel reprocessing is a key step toward sustainable nuclear energy, and the Purex process which is a liquid to liquid extraction technique, has become the mainstream technology for the efficient and scalable recovery of uranium, plutonium, and other fission materials. The shearing-dissolution unit is the first chemical operation in the Purex process, responsible for converting fuel assemblies from solid to liquid, which has a significant impact on the safety and efficiency of subsequent separation and extraction steps. The batch dissolver is a typical reactor used at the front end of spent fuel reprocessing, and it controls the dissolution reaction process indirectly through intermittent feeding. However, due to the highly dynamic and multi-parameter coupled nature of the system, current mathematical modeling and dynamic simulation studies on batch dissolver systems remain relatively scarce, restricting process optimization and scale-up engineering. Based on the principle of mass conservation, in this work a coupled shearing-dissolution mathematical model for batch dissolvers was established, and key processes including fuel shearing, particle volume reduction, dissolution reaction kinetics, and mass transfer were systematically described. The model introduces cylindrical geometry and a surface area correction factor, incorporates sub-boiling dissolution and batch feeding operation, and is implemented using a Python-based numerical simulation platform. Under typical process conditions (uranium dioxide mass of 523.4 kg, temperature of 95 ℃, initial nitric acid concentration of 6.1 mol/L, and surface area correction factor of 1), the simulation shows that the system reaches the discharge criterion at 234 min and achieves compositional equilibrium at approximately 800 min. At equilibrium, the uranium ion concentration is 318.81 g/L, nitric acid concentration is 1.41 mol/L, and the dissolution rate of uranium dioxide reaches 99.15%. The model’s simulation of solute concentration evolution under typical conditions closely matches theoretical data, with a relative mass balance error of only 0.007 2%, thus verifying the accuracy and stability of the modeling and algorithm. Furthermore, parametric studies of varying shearing intervals, dissolver liquid volume, initial nitric acid concentration, and surface area correction factor provide deeper insight into the effects of key operating parameters on the dissolution process dynamics. A local sensitivity analysis using the finite difference method was conducted to investigate the parameter sensitivity of uranium ion concentration with respect to initial nitric acid concentration and surface area correction factor. The proposed model effectively characterizes the dynamic behavior of batch dissolvers and demonstrates good engineering applicability and generalizability, providing reliable theoretical and data support for the optimization and design of spent fuel reprocessing processes.

     

/

返回文章
返回