Authors: Cuautli, C; Valente, JS; Conesa, JC; Ganduglia-Pirovano, MV; Ireta, J

J. Phys. Chem. C. vol: 123. page: 1932-7447.
Date: APR 11. 2019.
Doi: 10.1021/acs.jpcc.8b10935.

The layered double hydroxides (LDHs) containing Mg2+ Al3+, and OH- (MgAl-OH), commonly known as meixnerite, meixnerite-like, or activated LDH, act as catalyst in the cyanoethylation of alcohols, for which the catalytic activity depends on the LDH composition, particularly on the ratio R between the amount of Mg2+ and Al3+. It is known that MgAl-OH with R = 3 presents the largest catalytic activity when the reactants are methanol and acrylonitrile. To determine the molecular basis of such behavior, the adsorption of OH-, CH3O-, and H2O on the (001) surfaces of MgAl-OH with compositions R = 2, 3, and 3.5 is investigated using density functional theory. It is found that the peculiar catalytic activity of MgAl-OH in the methanol cyanoethylation reaction correlates with the capability of the MgAl-OH surface to stabilize CH3O–a process in which hydrogen bonding plays a crucial role-and the reactivity of the adsorbed CH3O- lone pairs..