Cooperativity of silanol defect chemistry in zeolites

Chen, Ya-Fan; Schroeder, Christian; Lew, Christopher M; Zones, Stacey I.; Koller, Hubert; Sierka, Marek

doi:10.1039/d2cp05218k

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2024

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Cited by 4 publications

References 57 publications

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Outlooks for zeolite catalysts in a low-carbon scenario

Serrano,

Centi,

Diddams

et al. 2024

Catalysis Today

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Outlooks for zeolite catalysts in a low-carbon scenario

Serrano,

Centi,

Diddams

et al. 2024

Catalysis Today

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The role of defects in high-silica zeolite hydrolysis and framework healing

Liu,

Grajciar,

Heard

2024

Microporous and Mesoporous Materials

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Enhancing the Acidity Window of Zeolites by Low-Temperature Template Oxidation with Ozone

Devos,

Sushkevich,

Khalil

et al. 2024

J. Am. Chem. Soc.

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Revisiting the impact of the first and often deemed trivial postsynthetic step, i.e., a high-temperature oxidative calcination to remove organic templates, increases our understanding of thermal acid site evolution and Al distributions. An unprecedented degree of control over the acidity of high-silica zeolites (SSZ-13) was achieved by using a low-temperature ozonation approach. Fourier transform infrared spectroscopy of adsorbed probe molecules and solid-state NMR spectroscopy reveal the complexity of the thermal evolution of acid sites. Lowtemperature activated (ozonated) zeolites maintain the original Brønsted acidity content and high defect content and have virtually no Lewis acidity. They also preserve the "as-made" Al distribution after crystallization and show a clear link between synthesis conditions and divalent cation capacity, as measured with aqueous cobalt ion uptake. The synthesis protocol is found to be the main contributor to Al proximity, yielding record high exchange capacity when ozonated. After conventional calcination at 500−600 °C, however, the presence of water leads to the gradual depletion of Brønsted acid sites, in particular, in small crystals. This work indicates that low-temperature ozonation followed by thermal activation at different temperatures can be used as a novel tool for tuning the amount and nature of acid sites, providing insights into the activity of zeolites in acid-catalyzed reactions, such as CO 2 hydrogenation to dimethyl ether, and thereby expanding the possibilities of rational acidity tuning.

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Cooperativity of silanol defect chemistry in zeolites

Abstract: Deboronation treatment of zeolite B-SSZ-55 can generate vacancy defects consisting of four silanol groups (silanol nests). However, 1H solid-state NMR spectroscopy indicates the prevalence of two silanol groups (silanol dyads)...

Cited by 4 publications

References 57 publications

Outlooks for zeolite catalysts in a low-carbon scenario

Outlooks for zeolite catalysts in a low-carbon scenario

The role of defects in high-silica zeolite hydrolysis and framework healing

Enhancing the Acidity Window of Zeolites by Low-Temperature Template Oxidation with Ozone

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