Heteroatom Manipulation of Zeolite Crystallization: Stabilizing Zn-FAU against Interzeolite Transformation.

Autor:	Mallette AJ; Department of Chemical and Biomolecular Engineering, University of Houston, Houston, Texas 77204, United States., Hong S; Department of Chemical and Petroleum Engineering, University of Pittsburgh, Pittsburgh, Pennsylvania 15213, United States., Freeman EE; Department of Chemical and Petroleum Engineering, University of Pittsburgh, Pittsburgh, Pennsylvania 15213, United States., Saslow SA; Pacific Northwest National Laboratory, Richland, Washington 99354, United States., Mergelsberg S; Pacific Northwest National Laboratory, Richland, Washington 99354, United States., Motkuri RK; Pacific Northwest National Laboratory, Richland, Washington 99354, United States., Neeway JJ; Pacific Northwest National Laboratory, Richland, Washington 99354, United States., Mpourmpakis G; Department of Chemical and Petroleum Engineering, University of Pittsburgh, Pittsburgh, Pennsylvania 15213, United States., Rimer JD; Department of Chemical and Biomolecular Engineering, University of Houston, Houston, Texas 77204, United States.
Jazyk:	angličtina
Zdroj:	JACS Au [JACS Au] 2022 Sep 06; Vol. 2 (10), pp. 2295-2306. Date of Electronic Publication: 2022 Sep 06 (Print Publication: 2022).
DOI:	10.1021/jacsau.2c00325
Abstrakt:	The preparation of metastable zeolites is often restricted to a limited range of synthesis conditions, which is exemplified in commercial syntheses lacking organics to stabilize the crystal structure. In the absence of an organic structure-directing agent, interzeolite transformation is a common phenomenon that can lead to undesirable products or impurities. Many studies have investigated the substitution of Si and Al in zeolite frameworks with alternative elements (heteroatoms) as a means of tailoring the properties of zeolites; however, relatively few studies have systematically explored the impact of heteroatoms on interzeolite transformations and their concomitant effects on zeolite crystallization. In this study, we examine methods to prepare isostructures of faujasite (FAU), which is one of the most commercially relevant zeolites and also a thermodynamically metastable structure. A survey of multivalent elements revealed that zinc is capable of stabilizing FAU at high temperatures and inhibiting its frequent transformation to zeolite gismondine (GIS). Using combined experimental and computational studies, we show that zinc alters the chemical nature of growth mixtures by sequestering silicates. Zinc heteroatoms incorporate in the FAU framework with a loading-dependent coordination. Our collective findings provide an improved understanding of driving forces for the FAU-to-GIS interzeolite transformation where we observe that heteroatoms (e.g., zinc) can stabilize zeolite FAU over a broad range of synthesis conditions. Given the growing interest in heteroatom-substituted zeolites, this approach to preparing zinc-containing FAU may prove applicable to a broader range of zeolite structures. Competing Interests: The authors declare no competing financial interest. (© 2022 The Authors. Published by American Chemical Society.)
Databáze:	MEDLINE
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