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

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Water-Induced Structural Dynamic Process in Molecular Sieves under Mild Hydrothermal Conditions: Ship-in-a-Bottle Strategy for Acidity Identification and Catalyst Modification.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-07-24 , DOI: 10.1002/anie.202009648
Tantan Sun _{1,

2} , Shutao Xu ₁ , Dong Xiao ₃ , Zhiqiang Liu ₄ , Guangchao Li _{2,

4} , Anmin Zheng ₄ , Wenjuan Liu _{2,

5} , Zhaochao Xu ₅ , Yi Cao ₁ , Qiang Guo ₁ , Nan Wang _{1,

2} , Yingxu Wei ₁ , Zhongmin Liu _{1,

3,

4}

Affiliation

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 ¹⁷O from H₂¹⁷O 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.

中文翻译：

温和水热条件下分子筛中水诱导的结构动力学过程：瓶装策略，用于酸度鉴定和催化剂改性。

水是自然界中最重要的物质。模仿天然材料的形成，分子筛已经在水热条件下合成并应用于工业。在这里，我们揭示了对这些材料非常特殊的水诱导结构动力学过程的意外观察。硅铝磷酸盐（SAPO）中T-O-T键的动态可逆断裂和形成是通过在温和的热液条件下气态水与分子筛骨架之间的相互作用而发生的，并通过检测到H ₂¹⁷中¹⁷ O的掺入得到了证实O进入分子筛框架。将大分子三甲基膦和吡啶（动力学直径比SAPO-34的孔径大得多）封装到CHA腔中，巩固了水诱导的动态过程。因此，提供了对分子筛在水中动力学特性的新见解。基于这些发现的“瓶中装船”策略也为精细的酸度识别开辟了新领域，并进一步促进了形状选择催化。

更新日期：2020-07-24

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