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The real-space imaging of small molecules is always challenging under theelectron microscopes, but highly demanded for investigating various nanoscaleinteractions, such as hydrogen bond and van der Waals (vdW) force. Especially,identifying the host-guest interactions in porous materials directly at themolecular level will bring a deeper insight into the behaviors of guestmolecules during the sorption, catalysis, gas separation and energy storage. Inthis 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 toidentify the host-guest vdW interactions. Based on these observations, werevealed that the PXs in one straight channel modified the channel geometrywith a coherent orientation. And the adjacent straight channels were deformedup to 8.8% along the different directions corresponding to three dominant PXconfigurations, resulting a negligible overall expansion of ZSM-5 lattices.Then, we could also image the disorder and desorption of PXs in ZSM-5 channelsduring the in situ heating. This work not only helped us to study thehost-guest vdW interactions and the sorption behaviors of PXs in ZSM-5, butalso provided an efficient tool for further imaging and studying othersingle-molecule behaviors under STEMs.

Real-Space Imaging of the Ordered Small Molecule Orientations in Porous Frameworks by Electron Microscopy