期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 46, 页码 20672-20681出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202009648
关键词
acidity; molecular sieves; MTO reaction; structural dynamic process; water
资金
- National Natural Science Foundation of China [21972142, 21991092, 21991090, 91745109, 91545104]
- Liaoning Revitalization Talents Program [XLYC1807227]
- Key Research Program of Frontier Sciences, CAS [QYZDY-SSW-JSC024]
- International Partnership Program of CAS [12142KYSB20180007]
- Youth Innovation Promotion Association of CAS [2014165]
Water is the most important substance in nature. Imitating the formation of natural materials, molecular sieves have been synthesized under hydrothermal conditions and applied in industry. Herein, we reveal an unforeseen observation on a very special water-induced structural dynamic process of these materials. Dynamic and reversible breaking and forming of T-O-T bonds in silicoaluminophosphate (SAPO) occurs through interactions between gaseous water and the molecular-sieve framework under mild hydrothermal conditions and is confirmed by detection of the incorporation of(17)O from (H2O)-O-17 into molecular-sieve framework. Encapsulation of the bulky molecules trimethylphosphine and pyridine (kinetic diameters much larger than the pore size of SAPO-34) into CHA cavities consolidated the water-induced dynamic process. Consequently, new insights into the dynamic features of molecular sieves in water are provided. The ship-in-a-bottle strategy based on these findings also open new fields for fine acidity identification and gives extra boost in shape-selective catalysis.
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