一步法制备MgO-Nd2Zr2O7复相陶瓷惰性燃料基材的热物理性能

Thermophysical Property of MgO-Nd2Zr2O7 Composite Ceramic Inert Matrix Prepared by One-step Method

  • 摘要: MgO-Nd2Zr2O7(M-NZO)复相陶瓷作为一种潜在的惰性燃料基材,可以用于替代(U,Pu)O2混合氧化物燃料中的UO2,并将PuO2弥散在其中以制备惰性基材燃料。本文采用一步法在1 500 ℃烧结24 h制备了M-NZO复相陶瓷,在物相组成、微观形貌的分析基础上,系统研究了其热导率和热膨胀系数等热物理性能。结果表明利用一步法制备的M-NZO复相陶瓷仅由MgO和Nd2Zr2O7烧绿石两相组成,两相的平均晶粒尺寸为0.75 μm和0.70 μm,且制备的复相陶瓷结构致密、孔隙率低。热物理性能测试结果表明一步法制备的M-NZO复相陶瓷在1 400 ℃时的热导率是UO2陶瓷的2.1~3.8倍,且在测试温度范围内,一步法制备的M-NZO复相陶瓷具有更加优异的热导率,在高温下(800 ℃)比文献中采用两步法制备的M-NZO复相陶瓷高出约2 W·m-1·K-1。热膨胀方面,一步法制备的M-NZO复相陶瓷的热膨胀系数为12.3×10-6~14.1×10-6/K,与两步法制备的M-NZO复相陶瓷热膨胀系数相当。此外,M-NZO复相陶瓷的热导率和热膨胀系数均随MgO含量的增大而变高,结合理论最小热导率计算结果可以得出,最佳的M-NZO复相陶瓷化学组成为0.5M-0.5NZO。以上结果表明,一步法制备的M-NZO复相陶瓷具有优异的热导率和稳定的热膨胀性能,为其在惰性基材燃料中的应用提供了更多的选择和热物理性能基础数据上的支持。

     

    Abstract: Inert matrix fuel (IMF) can effectively burn hazardous nuclides (such as Pu and minor actinides) as transmutation targets in reactors, making it an attractive option for nuclear waste management. IMF is a dispersion type of fuel that diffuses fissile phase, PuO2, in a neutron-transparent inert matrix (IM). MgO-Nd2Zr2O7 (M-NZO) composite ceramic is a potential IM that can replace UO2 in (U, Pu)O2 mixed oxide fuel (MOX) and to produce IMF by dispersing PuO2 in it. In this work, MgO, Nd2O3, ZrO2 powders were chosen as the raw materials, and series of ωM-(1-ω)NZO (ω=0.3, 0.4, 0.5, 0.6, 0.7 within mass percent) composite ceramics were prepared by one-step method at 1 500 ℃ for 24 h. Based on the analysis of phase composition and morphology, the thermophysical properties such as thermal conductivity and the coefficient of thermal expansion (CTE) for as-prepared M-NZO composite ceramics were systemically investigated. It is indicated that the as-prepared M-NZO composite ceramics show the remarkable densification and the mass fractions of MgO and Nd2Zr2O7 phases are almost the same as the designed nominal chemical composition. The average grain size of MgO phase and Nd2Zr2O7 phase is about 0.75 μm and 0.70 μm, respectively. The thermophysical properties results show that the thermal conductivity of all as-prepared M-NZO composite ceramics is 2.1-3.8 times that of UO2 ceramics at 1 400 ℃, suggesting the excellent thermal conductivity. And the thermal conductivity of M-NZO composite ceramics prepared by one-step method is higher than that of M-NZO composite ceramics fabricated by two-step method in the literatures within the tested temperature range, and the highest difference value is about 2 W·m-1·K-1 at high temperature (800 ℃). In terms of thermal expansion, the CTE value of as-prepared M-NZO composite ceramics ranges from 12.3×10-6-14.1×10-6/K and is comparable to that of UO2 ceramics. In addition, an incremental quantity of the thermal conductivity and CTE for ωM-(1-ω)NZO composite ceramics will merge with increasing MgO content. Combining the minimum thermal conductivity results for M-NZO composite materials, 0.5M-0.5NZO is the optimal sample composition, in which the mass percent of MgO in the composites stays the same as that of Nd2Zr2O7. In conclusion, M-NZO composite ceramics prepared in this work exhibits good thermal conductivity and stable thermal expansion property. And these thermal physical properties of M-NZO composite ceramics are superior to that of traditional UO2 ceramics. It is suggested that M-NZO composite ceramics can meet the thermal physical performances of IMF.

     

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