The AIMD simulations employed MOLOPT Gaussian double-zeta (DZVP-SR) basis sets for all elements. These calculations were performed in the NVT ensemble, fixing the unit cell parameters to the optimized values obtained in the structure optimizations. Depending on the size of the unit cell, supercells were used for some zeolites (see Supporting Information), resulting in least four fluoride anions per simulation box (six in the case of CHA). The AIMD simulations, which were performed for temperatures of 298 K, 373 K, and 473 K, used a Nosé-Hoover thermostat with a timestep of 0.5 fs and a time constant of 50 fs. Four separate trajectories were computed for each zeolite at each temperature, with every trajectory consisting of an equilibration phase of 5,000 steps (2.5 ps) and a production phase of 15,000 steps (7.5 ps). Root mean square displacements (RMSDs) of fluoride anions as well as AIMD average structures were calculated using the VMD code, version 1.9. Radial distribution functions (RDFs) of selected pairs of elements were computed with a customized code provided by Gloria Tabacchi (Università degli Studi dell'Insubria). All RDFs shown throughout this article correspond to averages over four trajectories. Structure visualizations were prepared with VESTA.