High-Silica CHA Zeolite Membrane with Ultra-High Selectivity and Irradiation Stability for Krypton/Xenon Separation.

High-Silica CHA Zeolite Membrane with Ultra-High Selectivity and Irradiation Stability for Krypton/Xenon Separation.
复制标题

用于氪/氙分离的超高选择性和辐照稳定性的高硅CHA沸石膜

DOI:
10.1002/anie.202100172
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发表时间:
2021-04-12
期刊:
Angewandte Chemie (International ed. in English)
影响因子:
--
通讯作者:
Kapteijn F
Kapteijn F
中科院分区:
其他
文献类型:
--
作者:
Wang X;Zhou T;Zhang P;Yan W;Li Y;Peng L;Veerman D;Shi M;Gu X;Kapteijn F

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捕获和储存长寿命85 Kr是减少乏燃料后处理设施挥发性放射性核素排放的有效方法。然而,由于氪(Kr)的化学惰性和相似的物理性质,从氙(Xe)中分离氪(Kr)具有挑战性。本文中,我们制备了用于Kr/Na 2SO 4分离的具有超高选择性和辐照稳定性的高硅CHA沸石膜。合适的孔径尺寸和刚性框架使膜具有很强的尺寸排阻效应。高硅CHA沸石膜的51-152的Kr选择性以及0.7-1.3×10−8 mol m−2 s−1 Pa−1的Kr渗透率远远超过现有技术的聚合物膜。该膜是分离潮湿氪/氪混合物的最稳定的多晶膜之一。高硅CHA沸石膜具有优异的辐照稳定性,可将放射性氪与氚分离,从而显著减少挥发性核废料的储存量。高硅CHA沸石膜显示出超高的Kr/H2O选择性和上级水热稳定性。高硅CHA沸石膜具有辐照稳定性,可以为从氙中富集放射性85 Kr铺平道路,从而显著减少挥发性核废料的体积。
Capture and storage of the long‐lived 85Kr is an efficient approach to mitigate the emission of volatile radionuclides from the spent nuclear fuel reprocessing facilities. However, it is challenging to separate krypton (Kr) from xenon (Xe) because of the chemical inertness and similar physical properties. Herein we prepared high‐silica CHA zeolite membranes with ultra‐high selectivity and irradiation stability for Kr/Xe separation. The suitable aperture size and rigid framework endures the membrane a strong size‐exclusion effect. The ultrahigh selectivity of 51–152 together with the Kr permeance of 0.7–1.3×10−8 mol m−2 s−1 Pa−1 of high‐silica CHA zeolite membranes far surpass the state‐of‐the‐art polymeric membranes. The membrane is among the most stable polycrystalline membranes for separation of humid Kr/Xe mixtures. Together with the excellent irradiation stability, high‐silica CHA zeolite membranes pave the way to separate radioactive Kr from Xe for a notable reduction of the volatile nuclear waste storage volume. High‐silica CHA zeolite membranes show ultra‐high Kr/Xe selectivity and superior hydrothermal stability. Together with their irradiation stability, high‐silica CHA zeolite membranes can pave the way to enrich radioactive 85Kr from xenon for a notable decrease in the volatile nuclear waste volume.
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