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阳离子插层层状二硫化钼吸附剂实现对铯的高选择性捕获。

Cation-Intercalated Lamellar MoS Adsorbent Enables Highly Selective Capture of Cesium.

作者信息

Wang Jing, Zhang Jianfeng, Ni Shan, Xing Huifang, Meng Qiyu, Bian Yangyang, Xu Zihao, Rong Meng, Liu Huizhou, Yang Liangrong

机构信息

Key Laboratory of Green and High-End Utilization of Salt Lake Resources, State Key Laboratory of Biochemical Engineering, CAS Key Laboratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, P. R. China.

School of Chemical Engineering, University of Chinese Academy of Sciences, Beijing 100049, P. R. China.

出版信息

ACS Appl Mater Interfaces. 2023 Oct 25;15(42):49095-49106. doi: 10.1021/acsami.3c08848. Epub 2023 Oct 11.

Abstract

Highly selective capture of cesium (Cs) from complex aqueous solutions has become increasingly important owing to its (Cs) indispensable role in some cutting-edge technologies and the environmental mobility of radioactive nuclide (Cs) from nuclear wastewater. Herein, we report the development of cation-intercalated lamellar MoS as an effective Cs adsorbent with the advantages of facile synthesis and highly tunable layer spacing. Two types of cations, including Na and NH, were employed for the intercalations between adjacent layers of MoS. The results demonstrated that the adsorption capacity of the NH-intercalated material (M-NH, 134 mg/g) for Cs clearly outperformed the others due to higher loading percentages of cations and larger layer spacing. The cesium partition coefficients for M-NH in the presence of 100-fold competing ions all exceed 1 × 10 mL/g. A simulated complex aqueous solution containing 15.37 mg/L Cs and highly excess of competing ions Li, Na, K, Mg, and Ca (20-306 times higher) was introduced to prove the practical application potential using our best-performing M-NH, showing a good to excellent partition ability of Cs among other cations, especially for Cs/K and Cs/Na with separation factors of 58 and 212, respectively. The adsorption and selectivity mechanisms were clearly elucidated using various advanced techniques, such as scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy. These results revealed that the good selectivity for Cs can be ascribed to the differences in Lewis acidities, hydration energy, cation sizes, and in particular, the divergence of coordination modes which was successfully achieved after tuning the layer distance via the cation intercalation strategy. In addition, the material has fast kinetics (<30 min), wide range of pH tolerance (4-10), and good reusability. Overall, our studies point out that the tunable lamellar MoS-based materials are promising adsorbents for Cs capture and separation.

摘要

由于铯(Cs)在一些前沿技术中发挥着不可或缺的作用,且核废水中放射性核素铯具有环境迁移性,因此从复杂水溶液中高选择性捕获铯变得越来越重要。在此,我们报道了阳离子插层的层状二硫化钼(MoS)作为一种有效的铯吸附剂的开发,该吸附剂具有合成简便和层间距高度可调的优点。两种类型的阳离子,包括Na和NH,被用于MoS相邻层之间的插层。结果表明,NH插层材料(M-NH,134 mg/g)对Cs的吸附容量明显优于其他材料,这是由于阳离子负载百分比更高和层间距更大。在存在100倍竞争离子的情况下,M-NH的铯分配系数均超过1×10 mL/g。引入了一种含有15.37 mg/L Cs以及大量过量竞争离子Li、Na、K、Mg和Ca(高出20 - 306倍)的模拟复杂水溶液,以使用我们性能最佳的M-NH证明其实际应用潜力,结果表明Cs在其他阳离子之间具有良好至优异的分配能力,特别是对于Cs/K和Cs/Na,分离因子分别为58和212。使用各种先进技术,如扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线衍射(XRD)、X射线光电子能谱(XPS)和拉曼光谱,清楚地阐明了吸附和选择性机制。这些结果表明,对Cs的良好选择性可归因于路易斯酸度、水合能、阳离子尺寸的差异,特别是通过阳离子插层策略调整层间距后成功实现的配位模式的差异。此外,该材料具有快速动力学(<30分钟)、宽pH耐受性范围(4 - 10)和良好的可重复使用性。总体而言,我们的研究指出,基于层状MoS的可调谐材料是用于Cs捕获和分离的有前景的吸附剂。

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