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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 M n+ ions (M n+ = 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. |
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