Methanol-Mediated Hydrogen Transfer Reactions at Surface Lewis Acid Sites of H-SSZ-13

Lewis acid sites (LAS) at the CHA(001) and CHA(101) surfaces are investigated regarding their activity for MeOH-mediated hydrogen transfer reactions from MeOH to alkenes, yielding alkanes and formaldehyde. Direct MeOH decomposition to formaldehyde and hydrogen is also investigated. Furthermore, the coupling of the produced olefins with formaldehyde to dienes and H${}_2$O via the Prins reaction is studied. The reactivity of LAS for these reactions is compared to that of bulk Brønsted acid sites (BAS) and surface BAS. Periodic density functional theory (DFT) is used in connection with DLPNO-CCSD(T) calculations on cluster models. Hydrogen transfer reactions are found to be often more favorable on LAS, while both LAS and BAS have similar activity for Prins reactions.