2026-05-17T13:59:58Z https://archive.materialscloud.org/oai2d

oai:materialscloud.org:2034 2023-12-20T13:00:18Z openaire_data community-mcarchive

Fernández Villanueva, Estefanía Ganduglia Pirovano, María Verónica Fernández Villanueva, Estefanía Lustemberg, Pablo Germán Zhao, Minjie Soriano, Jose Concepción, Patricia Ganduglia Pirovano, María Verónica 2023-12-20 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. The computational evidence has been experimentally validated by comparing the catalytic performance of the Cu-MgO-Al₂O₃ catalyst with hydroxyl groups against 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 the understanding of the underlying mechanisms and provide valuable insights for optimizing methanol synthesis processes. application/gzip text/plain text/markdown https://doi.org/10.24435/materialscloud:tz-pn oai:materialscloud.org:2034 mcid:2023.197 eng Materials Cloud https://doi.org/10.1021/jacs.3c10685 https://archive.materialscloud.org/communities/mcarchive https://doi.org/10.24435/materialscloud:89-an info:eu-repo/semantics/openAccess Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode Computational chemistry Heterogeneous catalysis CO2 hydrogenation Methanol Copper MgO DFT Water and Cu⁺ synergy in selective CO₂ hydrogenation to methanol over Cu/MgO catalysts info:eu-repo/semantics/other