Operando Two-Dimensional Solid-State NMR Unveils Dual-Template Collaboration and Competition in SAPO-34 Zeolite Crystallization.

Authors

Daoning Wu, Xinlong Yao, Lixin Liang, Quanzheng Deng, Lu Han, Guangjin Hou, Weili Dai

Published in

Journal of the American Chemical Society. May 19, 2025. Epub May 19, 2025.

Abstract

Unraveling the mechanism of zeolite crystallization, especially in a complex system containing dual-template agents, remains a critical challenge. In this work, we introduced, for the first time, novel operando two-dimensional (2D) solid-state NMR spectroscopy under extreme conditions of high temperature and high pressure, allowing for observations with atomic-level spatial and temporal resolution, thereby enabling unprecedented insights into the crystallization of SAPO-34 zeolite. By utilizing operando 2D ³¹P{¹H} HETCOR, ²⁷Al{¹H} HMQC NMR techniques, we clarified the intricate cooperative and competitive interactions of dual-template agents and highlighted the synergistic effect between templates and hydroxyl groups during CHA zeolite crystallization. Furthermore, operando ¹H, ²⁷Al, and ³¹P MAS NMR revealed a previously unreported induction period, which precedes intermediate formation. This innovative approach advances the understanding of molecular dynamics, crystallization mechanism, and synthesis method for zeolites, representing a significant leap forward in the field of operando two-dimensional solid-state NMR spectroscopy.

PMID:
40388714
Bibliographic data and abstract were imported from PubMed on 20 May 2025.

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