钨掺杂陶瓷微囊UO2芯块的制备与性能研究

Preparation and Property of Tungsten Added Ceramic Microcell UO2 Pellet

  • 摘要: 微囊UO2芯块属于耐事故燃料中的UO2芯块掺杂改性技术方向。在微囊UO2芯块中,金属或非燃料氧化物构成薄壁的连续网络结构,封装UO2颗粒,从而增强对强放射性、腐蚀性裂变产物的滞留能力。基于国内外微囊芯块的研究进展,本文设计了一种钨掺杂的陶瓷微囊UO2芯块,通过包含混料、成型、烧结在内的粉末冶金方法,制备了具备微囊结构特征的芯块,并对其组织结构、热物理性能以及吸收Cs的性能进行了研究。结果显示,作为原材料的混合粉末,化学成分均匀,烧结芯块外观良好,具备微囊结构特征的芯块的密度高于理论密度的95%,热导率与参比UO2芯块相当,微囊结构对Cs具有较强的吸收能力。以上结果证明了添加金属和非燃料氧化物的微囊UO2芯块的设计、制备和应用可行性。

     

    Abstract: Accident tolerant fuel (ATF) attracts extensive attention in recent years, which can provide longer accident response time and mitigate the impacts of accidents. ATF improves the safety of nuclear power plants, especially the safety performance of fuel in accident conditions, without reducing economic efficiency. Microcell UO2 pellets belong to the technical direction of doping modification of UO2 pellet among ATFs. In microcell UO2 pellets, metals or nonfuel oxides form a thinwalled continuous network structure, encapsulating UO2 particles, and enhancing the retention capability of highly radioactive and corrosive fission products. Based on the worldwide research progress of microcell pellets, and considering the thermophysical properties, phase stability and neutron absorption cross section, a kind of tungsten (W) added ceramic microcell UO2 pellet was designed in this paper. By powder metallurgy processes including blending with threedimensional blender, forming with automatic pressing machine and sintering in hydrogen sintering furnace, W added ceramic microcell UO2 pellets were prepared. By randomly sampling and analyzing the chemical composition of the upper, middle and lower layers of the blended powders of UO2, W and nonfuel oxide (Al2O3 or TiO2) after threedimensional blending, blend uniformity was studied. In addition, the microstructure, density and thermophysical properties of W added ceramic microcell UO2 pellets were studied by Xray diffraction (XRD), scanning electron microscopy (SEM), Archimedes’ principle, simultaneous thermal analysis (STA) and laser pulse thermal conductivity meter analysis. Besides, the Cs absorption experiment of the pellets was conducted by burying both W added ceramic microcell pellets and conventional UO2 pellets into cesium chloride (CsCl), heating to 650 ℃ and maintaining for 3 h. The element distribution of the pellets after Cs absorption experiment was analyzed by energy dispersive spectrometry (EDS). The results show that after threedimensional blending, the chemical composition of the blended powders is uniform and good blending effect is achieved. The uniformity of W component in UO28.5W(0.5/1.0)Al2O3 and UO28.5W(0.5/1.0)TiO2 is within ±10%, and the relative deviation of Al and Ti contents among the layers is below 10%. Four kinds of pellets prepared by forming and sintering with these blended powders have good appearance without obvious cracks. Microstructural study shows that the pellets added with Al2O3 powder (whose average particle size is 8.982 μm) do not form microcell structure. Meanwhile, the pellets added with TiO2 powder (whose average particle size is 2.890 μm) form microcell structure. It is inferred that the particle size of nonfuel oxide is the key factor which determines whether microcell structure can be formed. The W added ceramic microcell UO2 pellets have a density beyond 95% of the theoretical value. The thermal conductivity of UO28.5W1.0TiO2 pellets with microcell structure is equivalent to that of the conventional UO2 pellets. Cs absorption experiment show that Cs is enriched in the TiO2 microcell structure after being absorbed by W added ceramic microcell UO2 pellets. It is demonstrated that TiO2 microcell structure has a larger Cs absorption capacity. Therefore, this work demonstrates the feasibility of the design, preparation and application of W and nonfuel oxide added microcell UO2 pellets.

     

/

返回文章
返回