4.8 Article

Water-Induced Structural Dynamic Process in Molecular Sieves under Mild Hydrothermal Conditions: Ship-in-a-Bottle Strategy for Acidity Identification and Catalyst Modification

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 46, Pages 20672-20681

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202009648

Keywords

acidity; molecular sieves; MTO reaction; structural dynamic process; water

Funding

  1. National Natural Science Foundation of China [21972142, 21991092, 21991090, 91745109, 91545104]
  2. Liaoning Revitalization Talents Program [XLYC1807227]
  3. Key Research Program of Frontier Sciences, CAS [QYZDY-SSW-JSC024]
  4. International Partnership Program of CAS [12142KYSB20180007]
  5. Youth Innovation Promotion Association of CAS [2014165]

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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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