Confinement effects and acid strength in zeolites

Emanuele Grifoni, GiovanniMaria Piccini, Johannes A. Lercher, Vassiliki-Alexandra Glezakou (), Roger Rousseau () and Michele Parrinello ()
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Emanuele Grifoni: Department of Chemistry and Applied Biosciences, ETH Zurich, c/o USI Campus
GiovanniMaria Piccini: Department of Chemistry and Applied Biosciences, ETH Zurich, c/o USI Campus
Johannes A. Lercher: Pacific Northwest National Laboratory
Vassiliki-Alexandra Glezakou: Pacific Northwest National Laboratory
Roger Rousseau: Pacific Northwest National Laboratory
Michele Parrinello: Department of Chemistry and Applied Biosciences, ETH Zurich, c/o USI Campus

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract Chemical reactivity and sorption in zeolites are coupled to confinement and—to a lesser extent—to the acid strength of Brønsted acid sites (BAS). In presence of water the zeolite Brønsted acid sites eventually convert into hydronium ions. The gradual transition from zeolite Brønsted acid sites to hydronium ions in zeolites of varying pore size is examined by ab initio molecular dynamics combined with enhanced sampling based on Well-Tempered Metadynamics and a recently developed set of collective variables. While at low water content (1–2 water/BAS) the acidic protons prefer to be shared between zeolites and water, higher water contents (n > 2) invariably lead to solvation of the protons within a localized water cluster adjacent to the BAS. At low water loadings the standard free energy of the formed complexes is dominated by enthalpy and is associated with the acid strength of the BAS and the space around the site. Conversely, the entropy increases linearly with the concentration of waters in the pores, favors proton solvation and is independent of the pore size/shape.

Date: 2021
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DOI: 10.1038/s41467-021-22936-0

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