当前位置: X-MOL 学术J. Hazard. Mater. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Retention Mechanism of Cesium in Chabazite Embedded into Metakaolin-Based Alkali Activated Materials
Journal of Hazardous Materials ( IF 13.6 ) Pub Date : 2022-08-08 , DOI: 10.1016/j.jhazmat.2022.129732
Raudhatul Islam Chaerun , Natatsawas Soonthornwiphat , Kanako Toda , Kazuma Kuroda , Xiaobo Niu , Ryosuke Kikuchi , Tsubasa Otake , Yogarajah Elakneswaran , John L. Provis , Tsutomu Sato

Disposal of cesium-137 (Cs-137)-loaded chabazite generated from decontaminating cooling water of the damaged reactor at the Fukushima Daiichi Nuclear Power Station (FDNPS) has become a crucial concern. The potassium aluminosilicate-based alkali activated material (K-AAM) matrix is one of the candidate encapsulation matrices proposed for encapsulating cesium-137. In this study, chabazite loaded with a low Cs concentration (1 mg/g of Cs), embedded into a K-AAM matrix (K-AAM-C), was analysed to determine its capability to immobilise Cs, which was investigated by batch leaching experiments, field emission–electron probe microscopy analysis (FE-EPMA), X-ray diffraction (XRD), transmission electron microscopy (TEM), and Raman spectroscopy. The leaching experiments revealed that K-AAM-C efficiently immobilised Cs, with only 3% of the Cs leached out after 360 days of leaching in deionised water. Characterisation using XRD, TEM, and Raman analysis confirmed that the alkali-activator was responsible for the phase transformation of chabazite. FE-EPMA demonstrated that K entered the chabazite structure. This phenomenon resulted in the breakdown and subsequent reconstruction of the chabazite structure. TEM observation showed that the Cs was concentrated into the aggregates of precipitates, heterogeneously forming a pollucite-like structure in the chabazite after the fabrication process. Thermodynamic calculations indicated that pollucite was preferably stable in an AAM environment. When immersed in water, the amount of nano-pollucite increased over time, leading to the structural re-arrangement of aluminosilicate rings of chabazite according to TEM and Raman analysis. Pollucite is well known as a Cs-bearing natural zeolite, which can encapsulate Cs in its structure. Therefore, Cs retention was achieved in the spent chabazite adsorbent embedded into the K-AAM due to the resultant pollucite structure formed during AAM fabrication.



中文翻译:

偏高岭土基碱活化材料包埋菱沸石中铯的滞留机理

福岛第一核电站 (FDNPS) 受损反应堆冷却水净化后产生的负载铯 137 (Cs-137) 菱沸石的处置已成为一个关键问题。铝硅酸钾基碱活化材料 (K-AAM) 基质是用于封装 cesium-137 的候选封装基质之一。在本研究中,负载低 Cs 浓度的菱沸石(1 分析嵌入 K-AAM 基质 (K-AAM-C) 中的 mg/g Cs) 以确定其固定 Cs 的能力,并通过批量浸出实验、场发射电子探针显微镜分析 (FE- EPMA)、X 射线衍射 (XRD)、透射电子显微镜 (TEM) 和拉曼光谱。浸出实验表明,K-AAM-C 有效地固定了 Cs,在去离子水中浸出 360 天后,只有 3% 的 Cs 被浸出。使用 XRD、TEM 和拉曼分析的表征证实了碱活化剂是菱沸石相变的原因。FE-EPMA 表明 K 进入菱沸石结构。这种现象导致菱沸石结构的分解和随后的重建。TEM观察表明,Cs集中在沉淀物的聚集体中,在制造过程后在菱沸石中不均匀地形成了类锂辉石结构。热力学计算表明,钙镁石在 AAM 环境中最好是稳定的。根据 TEM 和拉曼分析,当浸入水中时,纳米钙铝石的量随时间增加,导致菱沸石的硅铝酸盐环结构重新排列。锂辉石是众所周知的一种含 Cs 的天然沸石,它可以将 Cs 包裹在其结构中。因此,由于在 AAM 制造过程中形成的钙铝石结构,在嵌入 K-AAM 的用过的菱沸石吸附剂中实现了 Cs 保留。热力学计算表明,钙镁石在 AAM 环境中最好是稳定的。根据 TEM 和拉曼分析,当浸入水中时,纳米钙铝石的量随时间增加,导致菱沸石的硅铝酸盐环结构重新排列。锂辉石是众所周知的一种含 Cs 的天然沸石,它可以将 Cs 包裹在其结构中。因此,由于在 AAM 制造过程中形成的钙铝石结构,在嵌入 K-AAM 的用过的菱沸石吸附剂中实现了 Cs 保留。热力学计算表明,钙镁石在 AAM 环境中最好是稳定的。根据 TEM 和拉曼分析,当浸入水中时,纳米钙铝石的量随时间增加,导致菱沸石的硅铝酸盐环结构重新排列。锂辉石是众所周知的一种含 Cs 的天然沸石,它可以将 Cs 包裹在其结构中。因此,由于在 AAM 制造过程中形成的钙铝石结构,在嵌入 K-AAM 的用过的菱沸石吸附剂中实现了 Cs 保留。锂辉石是众所周知的一种含 Cs 的天然沸石,它可以将 Cs 包裹在其结构中。因此,由于在 AAM 制造过程中形成的钙铝石结构,在嵌入 K-AAM 的用过的菱沸石吸附剂中实现了 Cs 保留。锂辉石是众所周知的一种含 Cs 的天然沸石,它可以将 Cs 包裹在其结构中。因此,由于在 AAM 制造过程中形成的钙铝石结构,在嵌入 K-AAM 的用过的菱沸石吸附剂中实现了 Cs 保留。

更新日期:2022-08-08
down
wechat
bug