Size-inverse molecular sieving xenon/krypton separation through cation-tuned gating effect within Linde Type A zeolites

作者：Daisong Chen, Tianyi Zhang, Xin Yin, Kai Jia, Yuying Wang, Boyu Zhang, Zhendong Liu, Liangchun Li, Qinfen Gu, Banglin Chen, Jin Shang · 发表于：Nature Communications · 年份：2025 · DOI：10.1038/s41467-025-64823-y · 被引用次数：8 · 研究领域：Zeolite Catalysis and Synthesis、Metal-Organic Frameworks: Synthesis and Applications、Catalytic Processes in Materials Science

Achieving highly selective xenon/krypton separation is a longstanding challenge due to the similar physicochemical properties of these noble gases. Here, we develop the cation-tuned gating sieving mechanism in Linde Type A zeolites to achieve a high xenon/krypton IAST selectivity over 1600. Through the cation exchange by Ag+ to introduce the preferential binding of xenon over krypton gas, followed by Ca²⁺ exchange to modulate cation density within the pore cavity so as to facilitate xenon uptake, the resulting Ag9Ca1.5A overcomes the kinetic limitations and achieves a dynamic xenon/krypton selectivity of 30 — the highest reported in the open literature — along with a high dynamic xenon uptake of 1.65 mmol/g. In this work, the sieving separation mechanism is exclusively established by the combined isothermal adsorption measurements, breakthrough experiments, synchrotron powder X-ray diffraction, X-ray absorption spectra, and ab initio density functional theory calculations. Zeolite with silver-tuned gating achieves counterintuitive size-inverse sieving, delivering record xenon/krypton separation and a scalable, energy-efficient path for challenging gas separations.