Triangulation of Guest Species in Porous Frameworks Using Solid-State NMR Spectroscopy and Quantum Chemical Calculations

F and its sensitivity to its surrounding environment enable the site-specific characterization of host-guest interactions. When combined with density functional theory calculations and numerical simulations, structurally realistic adsorption models can be evaluated against experimentally derived spatial constraints. Results indicate specific binding of 3-fluoropyridine to bridging hydroxyl Bro̷nsted acid sites and Lewis acid sites at defects, with stabilizing orientations governed by hydrogen bonding and π···π interactions. This work establishes an experimental-computational approach applicable to porous frameworks, offering molecular-level insights into adsorption structures relevant to material design for enhanced and tailored functionality.