Estefanía Fernández Villanueva^1,2*, Pablo Germán Lustemberg¹, Minjie Zhao³, Jose Soriano³, Patricia Concepción³, María Verónica Ganduglia Pirovano^1*

1 Instituto de Catálisis y Petroleoquímica – Consejo Superior de Investigaciones Científicas (ICP – CSIC), Calle de Marie Curie 2, 28049 Madrid, Spain

2 Universitat Politècnica de València (UPV), Camí de Vera s/n, 46022 Valencia, Spain

3 Instituto de Tecnología Química, Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC) Avenida de los Naranjos s/n, 46022 Valencia, Spain.

* Corresponding authors emails: e.fernandez@icp.csic.es, vgp@icp.csic.es

DOI10.24435/materialscloud:tz-pn [version v1]

Publication date: Dec 20, 2023

How to cite this record

Estefanía Fernández Villanueva, Pablo Germán Lustemberg, Minjie Zhao, Jose Soriano, Patricia Concepción, María Verónica Ganduglia Pirovano, Water and Cu⁺ synergy in selective CO₂ hydrogenation to methanol over Cu/MgO catalysts, Materials Cloud Archive 2023.197 (2023), https://doi.org/10.24435/materialscloud:tz-pn

Description

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.

Materials Cloud sections using this data

Files

File name	Size	Description
Structures.tar.gz MD5md5:b096e3e4938284716ab69a4ddb0312ff	333.7 MiB	INCAR, KPOINTS, CONTCAR and OUTCAR files for the structures reported in the paper entitled "Water and Cu+ synergy in selective CO2 hydrogenation to methanol over Cu/MgO catalysts" by Estefanía Fernández Villanueva, Pablo Germán Lustemberg, Minjie Zhao, Jose Soriano, Patricia Concepción, M. Verónica Ganduglia-Pirovano.
README.txt MD5md5:30fd6b8df4f87189367d525959c382da	2.5 KiB	"README.txt" file describing the contents of the "Structures.tar.gz" file

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External references

Keywords

Computational chemistry Heterogeneous catalysis CO2 hydrogenation Methanol Copper MgO DFT