Evaluation of the dissolution behavior of zircon using high-resolution phase-shift interferometry microscope

Evaluation of the dissolution behavior of zircon using high-resolution phase-shift interferometry microscope
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使用高分辨率相移干涉显微镜评价锆石的溶解行为

DOI:
10.1016/j.jnucmat.2021.153254
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发表时间:
2021
影响因子:
3.1
通讯作者:
KITAGAKI Toru
KITAGAKI Toru
中科院分区:
工程技术2区
文献类型:
--
作者:
Kitagaki Toru;Yoshida Kenta;Liu Pengfei;Shobu Takahisa;KITAGAKI Toru

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通过原位测量表面高度的变化,研究了锆石矿物(101)晶面在超纯水、1 M HCl(aq)和1 M NaOH(aq)中的溶解行为。利用高分辨率相移干涉显微镜(HR-PSI)测量了锆石在不同溶液中的表面高度变化速率,并考察了该方法在评价核材料溶解行为中的应用。在所有情况下,测得的表面高度线性下降,变化很小。虽然在这些条件下,在1 M NaOH(aq)中测得的锆石的高度变化是最小的,但在NaOH(aq)中溶解的Zr的浓度比在超纯水中高两个数量级。这表明在IM NaOH(aq)中溶解的大量Zr立即作为第二相沉淀在锆石表面上,并且表面形状几乎保持。另一方面,当在1 M HCl(aq)中测量锆石时,确认了以表面高度为基准的沉淀。这表明在1 M HCl(aq)中的沉淀发生在远离溶解点的地方,并且表面形状发生了变化。结果,成功地使用HR-PSI评估了极耐用矿物之一的锆石的表面变化速度和沉淀行为。这种相对快速的方法将有助于评估核材料(如燃料碎片,陶瓷废物形式和UO 2)在与各种溶液反应期间的详细表面变化行为,因为它最大限度地减少了辐射暴露时间以及测量期间产生的放射性废物量。
The dissolution behavior of the (101) plane of zircon mineral in ultrapure water, 1 M HCl (aq), and 1 M NaOH (aq), under room temperature and nearly atmospheric pressure was evaluated by in situ measurement of the change in the surface height. A high-resolution phase-shift interferometry microscope (HR-PSI) was employed to evaluate the velocity of the change in the surface height of zircon in different solutions, and the application of this method in evaluating the dissolution behavior of nuclear materials was examined. In all cases, the measured surface height decreased linearly with small variations. Although the measured change in height of zircon in 1 M NaOH (aq) was the smallest under these conditions, the concentration of dissolved Zr in NaOH (aq) was two orders of magnitude higher than that in ultrapure water. This indicates that a high amount of dissolved Zr in 1 M NaOH (aq) was immediately precipitated on the zircon surface as a secondary phase, and the surface shape was almost retained. On the other hand, the precipitation on the reference of the surface height was confirmed while measuring the zircon in 1 M HCl (aq). This shows that the precipitation in 1 M HCl (aq) occurred far from the dissolution points, and the surface shape changed. As a result, the velocity of surface change and the precipitation behavior of zircon, which is one of the extremely durable minerals, was successfully evaluated using HR-PSI. This relatively quick method would be useful for evaluating the detailed surface change behaviors of nuclear materials, such as fuel debris, ceramic waste forms, and UO2, during the reaction with various solutions, since it minimises radiation exposure times and also the amount of radioactive waste generation during measurement.
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