Ubiquitous Presence of Intermolecular CH…O Hydrogen Bonds in As‐synthesized Host‐Guest Zeolite Materials

Abstract CH⋅⋅⋅O hydrogen bonds (HBs) are ubiquituous in silica zeolite crystals hosting cationic Organic Structure Directing agents (OSDAs). This new finding is notably supported by a correlation between experimental C−O distances and COSi angles’ distributions of two series 19 11 available structures. The enables to asses the directionality CH…O intermolecular interactions extrapolate geometrical model for bonded moeities. DFT−D3 calculations on representative structures further confirmed presence these HBs their geometry basis H−O distances, CHO angles electron density. reported insights demonstrate also particularities terms charge distribution electrostatic potentials. Further, multiple bonding evidenced OSDAs zeolites’ channels cages, opening perspectives study zeolite‐OSDA host‐guest interactions.