论文标题
通过电子显微镜在多孔框架中有序小分子取向的真实空间成像
Real-Space Imaging of the Ordered Small Molecule Orientations in Porous Frameworks by Electron Microscopy
论文作者
论文摘要
在电子显微镜下,小分子的真实空间成像始终具有挑战性,但是高度要求研究各种纳米级相互作用,例如氢键和范德华(VDW)力。尤其是,直接在分子水平上识别多孔材料中的宿主 - 球相互作用将使您对在吸附,催化,气体分离和能量存储期间的客体分子行为有更深入的了解。在这项工作中,我们通过扫描透射电子显微镜(STEM)通过集成差异相比(IDPC)技术直接解决了在ZSM-5框架中吸附在ZSM-5框架中的有序构型,以识别宿主GUEST VDW相互作用。基于这些观察结果,我们揭示了一个直道中的PXS以连贯的方向修改了通道几何形状。并将相邻的直道沿不同方向变形至8.8%,对应于三种主要的PX构型,从而导致ZSM-5晶格的总体膨胀可忽略不计。然后,我们还可以在原位加热期间成像ZSM-5通道中PX的障碍和解吸。这项工作不仅有助于我们研究ZSM-5中PXS的宿主-Guest VDW相互作用以及PX的吸附行为,而且还提供了一种有效的工具,用于进一步成像和研究茎下其他单分子行为。
The real-space imaging of small molecules is always challenging under the electron microscopes, but highly demanded for investigating various nanoscale interactions, such as hydrogen bond and van der Waals (vdW) force. Especially, identifying the host-guest interactions in porous materials directly at the molecular level will bring a deeper insight into the behaviors of guest molecules during the sorption, catalysis, gas separation and energy storage. In this work, we directly resolved the ordered configurations of p-xylenes (PXs) adsorbed in ZSM-5 frameworks by the scanning transmission electron microscopy (STEM) with the integrated differential phase contrast (iDPC) technique to identify the host-guest vdW interactions. Based on these observations, we revealed that the PXs in one straight channel modified the channel geometry with a coherent orientation. And the adjacent straight channels were deformed up to 8.8% along the different directions corresponding to three dominant PX configurations, resulting a negligible overall expansion of ZSM-5 lattices. Then, we could also image the disorder and desorption of PXs in ZSM-5 channels during the in situ heating. This work not only helped us to study the host-guest vdW interactions and the sorption behaviors of PXs in ZSM-5, but also provided an efficient tool for further imaging and studying other single-molecule behaviors under STEMs.