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独居石型磷酸钐作为潜在核废料固化体:离子束辐照和原子模拟对辐射效应的见解

Monazite-Type SmPO as Potential Nuclear Waste Form: Insights into Radiation Effects from Ion-Beam Irradiation and Atomistic Simulations.

作者信息

Leys Julia M, Ji Yaqi, Klinkenberg Martina, Kowalski Piotr M, Schlenz Hartmut, Neumeier Stefan, Bosbach Dirk, Deissmann Guido

机构信息

Nuclear Waste Management and Reactor Safety, Institute of Energy and Climate Research (IEK-6), Forschungszentrum Jülich GmbH (FZJ), 52425 Jülich, Germany.

Institute for Applied Materials (IAM), Karlsruhe Institute of Technology (KIT), 76021 Karlsruhe, Germany.

出版信息

Materials (Basel). 2022 May 10;15(10):3434. doi: 10.3390/ma15103434.

DOI:10.3390/ma15103434
PMID:35629458
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9146725/
Abstract

Single-phase monazite-type ceramics are considered as potential host matrices for the conditioning of separated plutonium and minor actinides. Sm-orthophosphates were synthesised and their behaviour under irradiation was investigated with respect to their long-term performance in the repository environment. Sintered SmPO pellets and thin lamellae were irradiated with 1, 3.5, and 7 MeV Au ions, up to fluences of 5.1 × 10 ions cm to simulate ballistic effects of recoiling nuclei resulting from -decay of incorporated actinides. Threshold displacement energies for monazite-type SmPO subsequently used in SRIM/TRIM simulations were derived from atomistic simulations. Raman spectra obtained from irradiated lamellae revealed vast amorphisation at the highest fluence used, although local annealing effects were observed. The broadened, but still discernible, band of the symmetrical stretching vibration in SmPO and the negligible increase in P-O bond lengths suggest that amorphisation of monazite is mainly due to a breaking of -O bonds. PO groups show structural disorder in the local environment but seem to behave as tight units. Annealing effects observed during the irradiation experiment and the distinctively lower dose rates incurred in actinide bearing waste forms and potential -radiation-induced annealing effects indicate that SmPO-based waste forms have a high potential for withstanding amorphisation.

摘要

单相独居石型陶瓷被认为是用于处理分离钚和次要锕系元素的潜在主体基质。合成了钐正磷酸盐,并研究了它们在辐照下的行为,以了解它们在储存库环境中的长期性能。用1、3.5和7兆电子伏特的金离子辐照烧结的磷酸钐颗粒和薄片,辐照通量高达5.1×10离子/平方厘米,以模拟由掺入的锕系元素的α衰变产生的反冲核的弹道效应。随后用于SRIM/TRIM模拟的独居石型磷酸钐的阈位移能是通过原子模拟得出的。从辐照薄片获得的拉曼光谱显示,在使用的最高通量下出现了大量非晶化现象,尽管观察到了局部退火效应。磷酸钐中对称拉伸振动的谱带变宽但仍可分辨,且P-O键长增加可忽略不计,这表明独居石的非晶化主要是由于Si-O键的断裂。PO基团在局部环境中显示出结构无序,但似乎表现为紧密单元。在辐照实验中观察到的退火效应以及含锕系元素的废物形式中产生的明显较低的剂量率和潜在的γ辐射诱导的退火效应表明,基于磷酸钐的废物形式具有很高的抗非晶化潜力。

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本文引用的文献

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Front Chem. 2019 Apr 3;7:197. doi: 10.3389/fchem.2019.00197. eCollection 2019.
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Irradiation effects in monazite-(Ce) and zircon: Raman and photoluminescence study of Au-irradiated FIB foils.独居石(铈)和锆石中的辐照效应:金离子辐照聚焦离子束箔片的拉曼光谱和光致发光研究
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