Liquid feed vitrification of high-level nuclear waste: Description and modeling of chemical reactions

IF 3.2 2区工程技术 Q3 MATERIALS SCIENCE, MULTIDISCIPLINARY Journal of Nuclear Materials Pub Date : 2025-02-10 DOI:10.1016/j.jnucmat.2025.155688

E. Sauvage , S. Schuller , Z. Nabyl , R. Podor , J. Lautru , P. Benigni , J. Klouzek , S. Mure , V. Benavent

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Abstract

In order to take into account the thermal effects associated with the decomposition of precursors (glass frit and waste, without prior calcination) in the multiphysics CFD (Computational Fluid Dynamics) simulations developed for cold crucible vitrification, mathematical modeling of denitration kinetics is proposed. On the basis of a run-rerun method applied to DTA-TGA analysis carried out at different temperature ramps (10 to 40 °C/minute), the degrees of conversion of the reactions have been determined and the kinetic parameters described by taking into account a weighted sum of 7 elementary reactions of order n, whose rate constant follows an Arrhenius law. This global approach makes it possible to describe the overall kinetics of each endothermic event satisfactorily, without having to consider the complexity of the decomposition reactions of the initial pure compounds. However, analysis of the gases emitted during the reactions using thermogravimetric analysis coupled with mass spectrometry (TGA-MS) and characterization by environmental scanning electron microscopy (ESEM) correlated with literature data enabled to describe the main chemical reactions associated with thermal events. This global approach can be transposed to other systems if the reactions are thermally activated.

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高放核废料的液体进料玻璃化：化学反应的描述和模拟

为了在冷坩埚玻璃化的多物理场CFD（计算流体动力学）模拟中考虑与前驱体（玻璃熔块和废料，未经事先煅烧）分解相关的热效应，提出了脱硝动力学的数学模型。在不同温度梯度（10 ~ 40°C/min）下进行DTA-TGA分析的运行-再运行方法的基础上，根据速率常数符合Arrhenius定律的7个n阶基本反应的加权和，确定了反应的转化程度和动力学参数。这种全局方法可以令人满意地描述每个吸热事件的总体动力学，而不必考虑初始纯化合物分解反应的复杂性。然而，利用热重联用质谱（TGA-MS）和环境扫描电子显微镜（ESEM）对反应过程中释放的气体进行分析，结合文献数据，能够描述与热事件相关的主要化学反应。如果反应是热激活的，这种全局方法可以转置到其他系统。

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来源期刊

Journal of Nuclear Materials 工程技术-材料科学：综合

CiteScore

5.70

自引率

25.80%

发文量

601

审稿时长

63 days

期刊介绍： The Journal of Nuclear Materials publishes high quality papers in materials research for nuclear applications, primarily fission reactors, fusion reactors, and similar environments including radiation areas of charged particle accelerators. Both original research and critical review papers covering experimental, theoretical, and computational aspects of either fundamental or applied nature are welcome. The breadth of the field is such that a wide range of processes and properties in the field of materials science and engineering is of interest to the readership, spanning atom-scale processes, microstructures, thermodynamics, mechanical properties, physical properties, and corrosion, for example. Topics covered by JNM Fission reactor materials, including fuels, cladding, core structures, pressure vessels, coolant interactions with materials, moderator and control components, fission product behavior. Materials aspects of the entire fuel cycle. Materials aspects of the actinides and their compounds. Performance of nuclear waste materials; materials aspects of the immobilization of wastes. Fusion reactor materials, including first walls, blankets, insulators and magnets. Neutron and charged particle radiation effects in materials, including defects, transmutations, microstructures, phase changes and macroscopic properties. Interaction of plasmas, ion beams, electron beams and electromagnetic radiation with materials relevant to nuclear systems.