Fleury Guillaume, Steele Julian A, Gerber Iann C, Jolibois F, Puech P, Muraoka Koki, Keoh Sye Hoe, Chaikittisilp Watcharop, Okubo Tatsuya, Roeffaers Maarten B J
Department of Microbial and Molecular Systems, Centre for Surface Chemistry and Catalysis (COK) , KU Leuven , Celestijnenlaan 200F , 3001 Leuven , Belgium.
LPCNO , Université Fédérale de Toulouse Midi-Pyrénées, INSA, CNRS, UPS, CNRS , 135 av. de Rangueil , F-31077 Toulouse , France.
J Phys Chem Lett. 2018 Apr 5;9(7):1778-1782. doi: 10.1021/acs.jpclett.8b00399. Epub 2018 Mar 26.
The direct synthesis of hierarchically intergrown silicalite-1 can be achieved using a specific diquaternary ammonium agent. However, the location of these molecules in the zeolite framework, which is critical to understand the formation of the material, remains unclear. Where traditional characterization tools have previously failed, herein we use polarized stimulated Raman scattering (SRS) microscopy to resolve molecular organization inside few-micron-sized crystals. Through a combination of experiment and first-principles calculations, our investigation reveals the preferential location of the templating agent inside the linear pores of the MFI framework. Besides illustrating the attractiveness of SRS microscopy in the field of material science to study and spatially resolve local molecular distribution as well as orientation, these results can be exploited in the design of new templating agents for the preparation of hierarchical zeolites.
使用特定的双季铵试剂可以实现分级共生硅沸石-1的直接合成。然而，这些分子在沸石骨架中的位置对于理解材料的形成至关重要，但仍不清楚。在传统表征工具先前失效的情况下，我们在此使用偏振受激拉曼散射（SRS）显微镜来解析几微米大小晶体内部的分子组织。通过实验和第一性原理计算相结合，我们的研究揭示了模板剂在MFI骨架线性孔内的优先位置。除了说明SRS显微镜在材料科学领域研究和空间解析局部分子分布及取向方面的吸引力外，这些结果还可用于设计新型模板剂以制备分级沸石。
