Evidence of Hydronium Formation in Water–Chabazite Zeolite Using Inelastic Neutron Scattering Experiments and ab Initio Molecular Dynamics Simulations

A combined study of inelastic neutron scattering and ab initio molecular dynamics simulations has been performed in order to study the water–acid site interaction in zeolite chabazite with a ratio Si/Al = 16 that corresponds to 2 protons/uc with two different water coverages with the number of water molecules being lower and higher than that of proton sites. These results have provided a clear picture of the water–acid site interaction, and it has been demonstrated that there are two regimens of water adsorption, which depend on the water loading. (i) At low water coverage (water/acid site ∼0.5), the main interactions between water and the zeolitic acid sites are established through hydrogen bond and there is no proton transference to water. (ii) At relatively high water loading (water/acid site ∼3), the clustering of water molecules and hydronioum cations formed by the complete transference of the zeolitic proton to the water molecules has been observed. The formation of water–hydronium clusters interacting with oxygen atoms of the zeolite framework provides the stabilization energy needed for the protonation of water molecules confined in the cavities of chabazite. These results are the experimental evidence obtained from INS of proton transfer from the zeolitic acid site and the hydronium formation and are in agreement with a previous computational study ( Phys. Chem. Chem. Phys. 2009, 11, 1702−1712 ) and very recent solid state NMR spectroscopy studies ( J. Am. Chem. Soc. 2019, 141, 3444−3455 ). The inspection of the low energy bands (translational and optic modes) and librational bands of the experimental results allows obtaining information about the H-bond network of the hydronium–water cluster.