posted on 2024-01-11, 14:06authored byEstefanía Fernández-Villanueva, Pablo G. Lustemberg, Minjie Zhao, Jose Soriano Rodriguez, Patricia Concepción, M. Verónica Ganduglia-Pirovano
The CO2 hydrogenation reaction to produce
methanol holds
great significance as it contributes to achieving a CO2-neutral economy. Previous research identified isolated Cu+ species doping the oxide surface of a Cu-MgO-Al2O3-mixed oxide derived from a hydrotalcite precursor as the
active site in CO2 hydrogenation, stabilizing monodentate
formate species as a crucial intermediate in methanol synthesis. In
this work, we present a molecular-level understanding of how surface
water and hydroxyl groups play a crucial role in facilitating spontaneous
CO2 activation at Cu+ sites and the formation
of monodentate formate species. Computational evidence has been experimentally
validated by comparing the catalytic performance of the Cu-MgO-Al2O3 catalyst with hydroxyl groups against that of
its hydrophobic counterpart, where hydroxyl groups are blocked using
an esterification method. Our work highlights the synergistic effect
between doped Cu+ ions and adjacent hydroxyl groups, both
of which serve as key parameters in regulating methanol production
via CO2 hydrogenation. By elucidating the specific roles
of these components, we contribute to advancing our understanding
of the underlying mechanisms and provide valuable insights for optimizing
methanol synthesis processes.