Chemical characterisation of degraded nuclear fuel analogues simulating the Fukushima Daiichi nuclear accident
Chemical characterisation of degraded nuclear fuel analogues simulating the Fukushima Daiichi nuclear accident
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模拟福岛第一核事故的降解核燃料类似物的化学表征
DOI：
10.1038/s41529-022-00219-3
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发表时间：
2022
影响因子：
5.1
通讯作者：
Ding H
中科院分区：
文献类型：
--
作者：
Ding H
福岛第一核电站事故产生了降解的核燃料材料，与其他反应堆组件混合，称为熔融堆芯混凝土相互作用（MCCI）材料。模拟MCCI材料的合成，不包括高放射性裂变产物，含有贫化U，并将Ce作为Pu的替代品。多模态微焦点X射线分析显示，除了结晶硅酸盐相CaSiO 3、SiO2-方石英和含Ce的透闪石（Ce，Nd）2Si 2 O 7之外，还存在预期的一套含U-Zr-O矿物。贫U-Zr-O的Ce-Nd-O熔体与硅酸盐（SiO2）熔体反应生成了钙钛矿。确定大部分U以U4+存在，而观察到Ce以Ce 3+存在，这与高度还原的合成条件一致。一系列的含铁相，其特征在于不同的平均氧化态进行了鉴定，据推测，它们的形成诱导的局部氧势的异质性，影响铈的氧化态。
The Fukushima Daiichi accident generated degraded nuclear fuel material, mixed with other reactor components, known as molten core-concrete interaction (MCCI) material. Simulant MCCI material was synthesised, excluding highly radioactive fission products, containing depleted U, and incorporating Ce as a surrogate for Pu. Multi-modal µ-focus X-ray analysis revealed the presence of the expected suite of U-Zr-O containing minerals, in addition to crystalline silicate phases CaSiO3, SiO2-cristobalite and Ce-bearing percleveite, (Ce,Nd)2Si2O7. The formation of perclevite resulted from reaction between the U-Zr-O-depleted Ce-Nd-O melt and the silicate (SiO2) melt. It was determined that the majority of U was present as U4+, whereas Ce was observed to be present as Ce3+, consistent with the highly reducing synthesis conditions. A range of Fe-containing phases characterised by different average oxidation states were identified, and it is hypothesised that their formation induced heterogeneity in the local oxygen potential, influencing the oxidation state of Ce.
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