An Extra-Large Pore Zeolite Enabled by 1D-to-3D Topotactic Condensation

21 April 2022, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

Zeolites are microporous silicates that find an ample variety of applications as catalysts, adsorbents, and cation exchangers. Natural and synthetic zeolites possess a fully connected three-dimensional network of corner-sharing SiO4 tetrahedra (i.e. they are tectosilicates or framework silicates, with Si occasionally substituted by other atoms). Stable silica-based zeolites with increased porosity are of interest to allow processing of large molecules, but challenge our synthetic ability. Here we report a novel zeolite, ZEO-3, with a multidimensional, interconnected system of extra-large pores open through windows made by 16 and 14 SiO4 tetrahedra, which, with a specific surface area of over 1000 m2/g and an extraordinary performance for Volatile Organic Compounds abatement, is the less dense polymorph of silica known so far. This zeolite, however, is not directly synthesized as a tectosilicate but is the first three-dimensional zeolite that is obtained by topotactic condensation from a one-dimensional chain silicate (inosilicate, ZEO-2), a process that bears a 17% contraction of the structure but that does not alter the topology of the chain silicate (hence the term “topotactic”). This discovery challenges concepts deeply-rooted into zeolite science, and opens up the possibility of chain silicates as precursors for the crystallization of zeolites.

Keywords

Zeolites
topotactic condensation
1D-to-3D
electron crystallography
cRED
High Resolution Scanning Transmission Electron Diffraction
VOCs abatement
Large molecule adsorption
Extra-large pores
low density silica polymorph
Stable Zeolite

Supplementary materials

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Title
Supplementary Information for An Extra-Large Pore Zeolite Enabled by 1D-to-3D Topotactic Condensation
Description
Additional characterization (methods, SEM, cRED, difference e- density maps, 13C, 31P, 1H NMR, PXRD study of the condensation, TG, HRSTEM, energy vs density, FTIR, crystallographic data, topology analysis, framework density of silica polymorphs, references)
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