A study of the mechanical and thermophysical properties of crystal matrices for the immobilization of high-level wastes

I. V. Kuznetsov, A. Y. Zobkova, M. Kalenova, A. S. Shchepin, O. N. Budin, V. A. Stepanov, I. M. Melnikova, O. I. Stefanovskaya, K. V. Klemazov
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Abstract

Objectives. The aim of the study was to confirm the compliance of the mechanical and thermophysical properties of titanate-zirconate mineral-like matrices intended for immobilization of the rare-earth-actinide fraction of high-level waste (HLW) with pyrochlore structures (Nd2ZrTiO7) and orthorhombic titanate of rare earth elements (Nd4Ti9O24+TiO2) with the Russian requirements for the final forms of radioactive waste sent for disposal. With regard to fractionated radioactive waste, this type of matrix is preferable when compared with conservative aluminophosphate and borosilicate glasses. This is due to larger capacity, and a better level of chemical, thermal, and radiation resistance.Methods. The synthesis of mineral-like matrices was carried out by remelting a granular precursor consisting of mineral-forming metal oxides and a solution imitating the rare earth-actinide fraction of HLW in an induction furnace with a cold crucible. The thermal diffusivity was determined by the laser flash method. The heat capacity of the matrix samples was measured by differential scanning calorimetry. Ultimate flexural and compressive strengths were determined using universal test machines. The elastic moduli (Young’s) were measured by the acoustic method. The temperature coefficients of linear expansion were determined using a high-temperature dilatometer.Results. The ultimate strength of the matrices (Nd2ZrTiO7) and (Nd4Ti9O24+TiO2) was found to be 150–179 and 20.6–57.8 MPa in compression and bending respectively. Young’s moduli vary from 3.7 ∙ 107 to 2.15 ∙ 108 kN/m2. With an increase in temperature from 50 to 500°C, the values of thermal conductivity have a pronounced tendency to decrease from 1.71 to 0.91 W/(m∙K). The temperature coefficients of linear expansion increase from 6.96 ∙ 10−6 to 1.01 ∙ 10−5 K−1 in the same temperature range.Conclusions. Comprehensive studies of titanate-zirconate mineral-like matrices show that their mechanical and thermal properties in certain cases significantly exceed the minimum requirements of regulatory documentation for the final forms of HLW.
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用于固定高浓度废物的晶体基质的机械和热物理特性研究
研究目的研究的目的是确认用于固定高放射性废物(HLW)中稀土-锕系元素部分的钛酸-锆酸盐类矿物基质的机械和热物理性能是否符合俄罗斯对送去处理的放射性废物最终形式的要求,这些基质具有热绿结构(Nd2ZrTiO7)和稀土元素正长钛酸盐(Nd4Ti9O24+TiO2)。就分馏放射性废物而言,与保守的磷酸铝和硼硅酸盐玻璃相比,这种基质更为可取。这是因为它具有更大的容量,以及更好的耐化学、耐热和耐辐射性。合成类矿物基质的方法是,在带有冷坩埚的感应炉中重熔由矿物形成金属氧化物和模仿 HLW 稀土-锕系元素部分的溶液组成的颗粒状前体。热扩散率是通过激光闪光法测定的。基体样品的热容量是通过差示扫描量热法测量的。极限抗折强度和抗压强度是用万能试验机测定的。弹性模量(杨氏模量)采用声学方法测量。线膨胀系数是用高温膨胀仪测定的。发现(Nd2ZrTiO7)和(Nd4Ti9O24+TiO2)基质在压缩和弯曲时的极限强度分别为 150-179 兆帕和 20.6-57.8 兆帕。杨氏模量从 3.7 ∙ 107 到 2.15 ∙ 108 kN/m2 不等。随着温度从 50°C 上升到 500°C,导热系数明显从 1.71 W/(m∙K) 下降到 0.91 W/(m∙K)。在相同的温度范围内,线膨胀系数从 6.96 ∙ 10-6 增至 1.01 ∙ 10-5 K-1。对钛酸锆矿物样基质的全面研究表明,在某些情况下,它们的机械和热性能大大超出了监管文件对高放射性废物最终形式的最低要求。
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