Dealumination of small-pore zeolites through pore-opening migration process with the aid of pore-filler stabilization.
Dealumination of small-pore zeolites through pore-opening migration process with the aid of pore-filler stabilization.
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DOI：
10.1126/sciadv.abo3093
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发表时间：
2022-06-24
期刊：
影响因子：
13.6
通讯作者：
Wakihara, Toru
中科院分区：
文献类型：
--
作者：
Yoshioka, Tatsushi;Iyoki, Kenta;Hotta, Yuusuke;Kamimura, Yoshihiro;Yamada, Hiroki;Han, Qiao;Kato, Takeharu;Fisher, Craig A. J.;Liu, Zhendong;Ohnishi, Ryohji;Yanaba, Yutaka;Ohara, Koji;Sasaki, Yukichi;Endo, Akira;Takewaki, Takahiko;Sano, Tsuneji;Okubo, Tatsuya;Wakihara, Toru
小孔沸石由于其上级催化性能而受到越来越多的关注。尽管是关键的催化活性和寿命，合成后调整的体积Si/Al比的小孔沸石尚未实现与保存良好的结晶度，因为有限的质量转移的铝物种通过狭窄的微孔。在这里，我们展示了一种合成后的方法来调整小孔沸石的组成，使用以前未开发的策略命名为开孔迁移过程（POMP）。通过有机阳离子在沸石孔中的稳定化来辅助酸处理被证明是成功的，用于通过POMP从沸石中去除Al物种。此外，脱铝AFX沸石通过缺陷修复进行处理，这产生了对苛刻蒸汽条件的上级水热稳定性。我们的研究结果可以通过铝含量控制和缺陷愈合促进小孔沸石的工业应用，并可以阐明无机微孔材料的结构重构和排列过程。使用开孔迁移过程的合成后方法使得能够调节小孔沸石组合物。
Small-pore zeolites are gaining increasing attention owing to their superior catalytic performance. Despite being critical for the catalytic activity and lifetime, postsynthetic tuning of bulk Si/Al ratios of small-pore zeolites has not been achieved with well-preserved crystallinity because of the limited mass transfer of aluminum species through narrow micropores. Here, we demonstrate a postsynthetic approach to tune the composition of small-pore zeolites using a previously unexplored strategy named pore-opening migration process (POMP). Acid treatment assisted by stabilization of the zeolite framework by organic cations in pores is proven to be successful for the removal of Al species from zeolite via POMP. Furthermore, the dealuminated AFX zeolite is treated via defect healing, which yields superior hydrothermal stability against severe steam conditions. Our findings could facilitate industrial applications of small-pore zeolites via aluminum content control and defect healing and could elucidate the structural reconstruction and arrangement processes for inorganic microporous materials. A postsynthetic approach using a pore-opening migration process enables tuning of small-pore zeolite compositions.
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