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一体化处理:通过超稳定无机固体酸材料HMMoO·nH₂O(M = Ta,Nb)捕获和固定铯

All-in-one treatment: Capture and immobilization of Cs by ultra-stable inorganic solid acid materials HMMoO·nHO (M = Ta, Nb).

作者信息

Chen Zhihua, Jia Shaoqing, Sun Haiyan, Tang Junhao, Guo Yanling, Yao Yuexin, Pan Tianyu, Feng Meiling, Huang Xiaoying

机构信息

State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, PR China; University of Chinese Academy of Sciences, Beijing 100049, PR China.

HTA Co., Ltd., Beijing 102413, PR China.

出版信息

Water Res. 2024 May 15;255:121459. doi: 10.1016/j.watres.2024.121459. Epub 2024 Mar 12.

Abstract

Capture and immobilization of Cs is urgent for radioactive contamination remediation and spent fuel treatment. Herein, an effective all-in-one treatment method to simultaneously adsorb and immobilize Cs without high-temperature treatment is proposed. According to the strategy of incorporating high-valency metal ions into molybdates to increase the material stability and affinity towards radionuclides, layered HMMoO·nHO (M = Ta (1), Nb (2)) are prepared. Both materials exhibit excellent acid resistance (even 15 mol/L HNO). They maintain remarkable adsorption capacity for Cs in 1 mol/L HNO solutions and can selectively capture Cs under excessive competitive ions. Furthermore, they show successful cleanup for actual Cs-liquid-wastes generated during industrial production. In particular, adsorbed Cs can be firmly immobilized in interlayer spaces of materials due to the highly stable anionic framework. The removal mechanism is attributed to ion exchange between Cs and interlayer H by multiple characterizations. Study of the structure-function relationship shows that the occurrence of Cs ion exchange is closely related to plate-like layered structure. This work develops an efficient all-in-one treatment method for capturing and immobilizing radiocesium by ultra-stable inorganic solid acid materials with low energy consumption and high safety for radionuclide remediation.

摘要

捕获和固定铯对于放射性污染修复和乏燃料处理至关重要。在此,提出了一种无需高温处理即可同时吸附和固定铯的有效一体化处理方法。根据将高价金属离子引入钼酸盐以提高材料稳定性和对放射性核素亲和力的策略,制备了层状HMMoO·nHO(M = Ta (1),Nb (2))。两种材料均表现出优异的耐酸性(甚至在15 mol/L HNO中)。它们在1 mol/L HNO溶液中对铯保持显著的吸附容量,并且在存在过量竞争离子的情况下能够选择性地捕获铯。此外,它们对工业生产过程中产生的实际铯废液表现出成功的净化效果。特别地,由于高度稳定的阴离子骨架,吸附的铯能够牢固地固定在材料的层间空间中。通过多种表征手段,去除机制归因于铯与层间H之间的离子交换。结构 - 功能关系研究表明,铯离子交换的发生与板状层状结构密切相关。这项工作开发了一种高效的一体化处理方法,通过超稳定的无机固体酸材料捕获和固定放射性铯,具有低能耗和对放射性核素修复的高安全性。

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