期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 -, 期 -, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202217992
关键词
Acidity; Electrostatic Interactions; NMR Spectroscopy; Temperature Programmed Desorption; Zeolites
The use of mineralizing agents (F- or OH-) in hydrothermal synthesis directly affects the distribution of Al sites in ZSM-5 zeolites. The Si/Al ratio impacts the proportions of Al sites for F-, whereas it remains constant for OH-. This understanding provides new and simple opportunities to control the acidity of zeolites.
Intensive research on improving the catalytic properties of zeolites is focused on modulating their acidity and the distribution of associated Al sites. Herein, by studying a series of ZSM-5 zeolites over a broad range of Al content, we demonstrate how the nature of the mineralizing agent (F- or OH-) used in hydrothermal syntheses directly impacts Al sites distribution. The proportions of Al sites, probed by Al-27 NMR, depend on the Si/Al ratio for F-, but remain identical for OH- (from Si/Al=30 to 760). This leads to contrasting variations in weak and strong acidities. Such opposite effect of mineralizers is explained by the spatial location of negative charges and the resulting balance between short- and long-range electrostatic interactions. This understanding paves the way for additional and simple opportunities to control zeolites' acidity.
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