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Dealumination of small-pore zeolites through pore-opening migration process with the aid of pore-filler stabilization.
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.
Afiliación
  • Yoshioka T; Department of Chemical System Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan.
  • Iyoki K; Department of Chemical System Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan.
  • Hotta Y; Precursory Research for Embryonic Science and Technology (PRESTO), Japan Science and Technology Agency (JST), Kawaguchi, Saitama 332-0012, Japan.
  • Kamimura Y; Mitsubishi Chemical Corporation, Science and Innovation Center, Kamoshida-cho, Aoba-ku, Yokohama 227-8502, Japan.
  • Yamada H; Research Institute for Chemical Process Technology, National Institute of Advanced Industrial Science and Technology, Tsukuba Central 5-2, 1-1-1 Higashi, Tsukuba, Ibaraki 305-8565, Japan.
  • Han Q; Japan Synchrotron Radiation Research Institute/SPring-8, 1-1-1 Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5198, Japan.
  • Kato T; Mitsubishi Chemical Corporation, Science and Innovation Center, Kamoshida-cho, Aoba-ku, Yokohama 227-8502, Japan.
  • Fisher CAJ; Japan Fine Ceramics Center, 2-4-1 Mutsuno, Atsuta-ku, Nagoya 456-8587, Japan.
  • Liu Z; Japan Fine Ceramics Center, 2-4-1 Mutsuno, Atsuta-ku, Nagoya 456-8587, Japan.
  • Ohnishi R; Department of Chemical System Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan.
  • Yanaba Y; Institute of Engineering Innovation, The University of Tokyo, 2-11-16 Yayoi, Bunkyo-ku, Tokyo 113-8656, Japan.
  • Ohara K; Mitsubishi Chemical Corporation, Science and Innovation Center, Kamoshida-cho, Aoba-ku, Yokohama 227-8502, Japan.
  • Sasaki Y; Institute of Industrial Science, The University of Tokyo, 4-6-1 Komaba, Meguro-ku, Tokyo 153-8505, Japan.
  • Endo A; Japan Synchrotron Radiation Research Institute/SPring-8, 1-1-1 Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5198, Japan.
  • Takewaki T; Japan Fine Ceramics Center, 2-4-1 Mutsuno, Atsuta-ku, Nagoya 456-8587, Japan.
  • Sano T; Research Institute for Chemical Process Technology, National Institute of Advanced Industrial Science and Technology, Tsukuba Central 5-2, 1-1-1 Higashi, Tsukuba, Ibaraki 305-8565, Japan.
  • Okubo T; Mitsubishi Chemical Corporation, Science and Innovation Center, Kamoshida-cho, Aoba-ku, Yokohama 227-8502, Japan.
  • Wakihara T; Institute of Engineering Innovation, The University of Tokyo, 2-11-16 Yayoi, Bunkyo-ku, Tokyo 113-8656, Japan.
Sci Adv ; 8(25): eabo3093, 2022 Jun 24.
Article en En | MEDLINE | ID: mdl-35731864
ABSTRACT
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.