Boosting selective Cs+ uptake through the modulation of stacking modes in layered niobate-based perovskites
Haiyan Sun, Zhihua Chen, Bing Hu, Jun-Hao Tang, Lu Yang, Yanling Guo, Yuexin Yao, Mei‐Ling Feng, Xiao‐Ying Huang
Abstract
Selective separation of 137Cs is significant for the sustainable development of nuclear energy and environmental protection, due to its strong radioactivity and long half-life. However, selective capture of 137Cs+ from radioactive liquid waste is challenging due to strong coulomb interactions between the adsorbents and high-valency metal ions. Herein, we propose a strategy to resolve this issue and achieve specific Cs+ ion recognition and separation by modulating the stacking modes of layered perovskites. We demonstrate that among niobate-based perovskites, ALaNb2O7 (A = Cs, H, K, and Li), HLaNb2O7 shows an outstanding selectivity for Cs+ even in the presence of a large amount of competing Mn+ ions (Mn+ = K+, Ca2+, Mg2+, Sr2+, Eu3+, and Zr4+) owing to its suitable void fraction and space shape, brought by the stacking mode of layers. The Cs+ capture mechanism is directly elucidated at molecular level by single-crystal structural analyses and density functional theory calculations. This work not only provides key insights in the design and property optimization of perovskite-type materials for radiocesium separation, but also paves the way for the development of efficient inorganic materials for radionuclides remediation. Selective capture of radiocaesium is challenging due to strong coulomb interactions between adsorbents and high valent metal ions. Here, authors propose a strategy of modulating the stacking modes of layered perovskites to achieve specific Cs+ recognition and separation.