Interchain-expanded extra-large-pore zeolites

Zihao Rei Gao, Huajian Yu, Fei-Jian Chen, Alvaro Mayoral, Zijian Niu, Ziwen Niu, Xintong Li, Hua Deng, Carlos Márquez-Álvarez, Hong He, Shutao Xu, Yida Zhou, Jun Xu, Hao Xu, Wei Fan, Salvador R. G. Balestra, Chao Ma, Jiazheng Hao, Jian Li (), Peng Wu (), Jihong Yu () and Miguel A. Camblor ()
Additional contact information
Zihao Rei Gao: CSIC
Huajian Yu: CSIC
Fei-Jian Chen: Jilin University
Alvaro Mayoral: CSIC–Universidad de Zaragoza
Zijian Niu: Jilin University
Ziwen Niu: East China Normal University
Xintong Li: East China Normal University
Hua Deng: Chinese Academy of Sciences
Carlos Márquez-Álvarez: CSIC
Hong He: Chinese Academy of Sciences
Shutao Xu: Chinese Academy of Sciences
Yida Zhou: Chinese Academy of Sciences
Jun Xu: Chinese Academy of Sciences
Hao Xu: East China Normal University
Wei Fan: University of Massachusetts
Salvador R. G. Balestra: CSIC
Chao Ma: Nanjing University
Jiazheng Hao: Spallation Neutron Source Science Center
Jian Li: Nanjing University
Peng Wu: East China Normal University
Jihong Yu: Jilin University
Miguel A. Camblor: CSIC

Nature, 2024, vol. 628, issue 8006, 99-103

Abstract: Abstract Stable aluminosilicate zeolites with extra-large pores that are open through rings of more than 12 tetrahedra could be used to process molecules larger than those currently manageable in zeolite materials. However, until very recently1–3, they proved elusive. In analogy to the interlayer expansion of layered zeolite precursors4,5, we report a strategy that yields thermally and hydrothermally stable silicates by expansion of a one-dimensional silicate chain with an intercalated silylating agent that separates and connects the chains. As a result, zeolites with extra-large pores delimited by 20, 16 and 16 Si tetrahedra along the three crystallographic directions are obtained. The as-made interchain-expanded zeolite contains dangling Si–CH3 groups that, by calcination, connect to each other, resulting in a true, fully connected (except possible defects) three-dimensional zeolite framework with a very low density. Additionally, it features triple four-ring units not seen before in any type of zeolite. The silicate expansion–condensation approach we report may be amenable to further extra-large-pore zeolite formation. Ti can be introduced in this zeolite, leading to a catalyst that is active in liquid-phase alkene oxidations involving bulky molecules, which shows promise in the industrially relevant clean production of propylene oxide using cumene hydroperoxide as an oxidant.

Date: 2024
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DOI: 10.1038/s41586-024-07194-6

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