Partition of soluble fission products between the grey phase, ZrO2 and uranium dioxide
Partition of soluble fission products between the grey phase, ZrO2 and uranium dioxide
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可溶性裂变产物在灰相、ZrO2 和二氧化铀之间的分配
DOI：
10.1016/j.jnucmat.2013.02.082
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发表时间：
2013
影响因子：
3.1
通讯作者：
R. Grimes
中科院分区：
文献类型：
--
作者：
M. Cooper;S. Middleburgh;R. Grimes
用原子尺度模拟方法计算了从UO_2或UO_2 +_x中分离裂变产物并将其并入BaZrO_3、SrZrO_3（灰相组成相）和ZrO_2的能量。这些能量为可溶裂变产物在UO 2或UO 2 + x与燃料系统的这些二次氧化物成分之间的分配提供了热力学驱动。四价阳离子分配到BaZrO3，SrZrO3和ZrO2是唯一优选的物种半径小于Zr 4+，无论二氧化铀的化学计量。在化学计量的条件下，较大和较小的三价阳离子被发现偏析BaZrO 3，但只有较小的燃料添加剂元素Cr 3+和Fe 3+偏析SrZrO 3。UO2 + x的分配总是不利于三价阳离子。添加过量的Cr3+（作为燃料添加剂）的预测，使分区成BaZrO3和SrZrO3更有利于从UO2为较大的三价阳离子。半径小于或等于Sm 3+的三价裂变产物被确定为从UO2中仅分离成ZrO 2。没有偏析的SrO或BaO的预测。
The energies to remove fission products from UO2or UO2+xand incorporate them into BaZrO3, SrZrO3(grey phase constituent phases) and ZrO2have been calculated using atomistic scale simulation. These energies provide the thermodynamic drive for partition of soluble fission products between UO2or UO2+xand these secondary oxide constituents of the fuel system. Tetravalent cation partition into BaZrO3, SrZrO3and ZrO2was only preferable for species with smaller radii than Zr4+, regardless of uranium dioxide stoichiometry. Under stoichiometric conditions both the larger and the smaller trivalent cations were found to segregate to BaZrO3but only the smaller fuel additive elements Cr3+and Fe3+segregate to SrZrO3. Partition from UO2+xwas always unfavourable for trivalent cations. Additions of excess Cr3+(as a fuel additive) are predicted make the partition into BaZrO3and SrZrO3more favourable from UO2for the larger trivalent cations. Trivalent fission products with radii smaller than or equal to that of Sm3+were identified to segregate into ZrO2only from UO2. No segregation to SrO or BaO is predicted.