Articles producció científica> Química Física i Inorgànica

Design of Flame-Made ZnZrOx Catalysts for Sustainable Methanol Synthesis from CO2

  • Identification data

    Identifier: imarina:9293178
  • Authors:

    Araujo, TP
    Morales-Vidal, J
    Zou, TS
    Agrachev, M
    Verstraeten, S
    Willi, PO
    Grass, RN
    Jeschke, G
    Mitchell, S
    Lopez, N
    Perez-Ramirez, J
  • Others:

    Author, as appears in the article.: Araujo, TP; Morales-Vidal, J; Zou, TS; Agrachev, M; Verstraeten, S; Willi, PO; Grass, RN; Jeschke, G; Mitchell, S; Lopez, N; Perez-Ramirez, J
    Department: Química Física i Inorgànica
    URV's Author/s: Lopez Alonso, Nuria
    Keywords: Zro2 Znzrox catalysts Zirconia Total-energy calculations Sustainable methanol Surface region Points Phase-transformation Oxygen vacancies Hydrogenation High-temperature Flame spray pyrolysis Defects Co2 hydrogenation 1st-principles
    Abstract: Mixed zinc-zirconium oxides, ZnZrOx, are highly selective and stable catalysts for CO2 hydrogenation to methanol, a pivotal energy vector. However, their activity remains moderate, and descriptors to design improved systems are lacking. This work applies flame spray pyrolysis (FSP), a one-step and scalable method, to synthesize a series of ZnZrOx catalysts, and systematically compares them to coprecipitated (CP) analogs to establish deeper synthesis-structure-performance relationships. FSP systems (up to 5 mol%) generally display a threefold higher methanol productivity compared to their CP counterparts. In-depth characterization and theoretical simulations show that, unlike CP, FSP maximizes the surface area and formation of atomically dispersed Zn2+ sites incorporated in lattice positions within the ZrO2 surface, which is key to improving performance. Analysis by in situ electron paramagnetic resonance (EPR) spectroscopy reveals that the specific architecture of the flame-made catalyst markedly fosters the generation of oxygen vacancies. Together with surrounding Zn and Zr-O atoms, the oxygen vacancies create active ensembles that favor methanol formation through the formate path while suppressing undesired CO production, as confirmed by kinetic modeling. This study elucidates the nature of active sites and their working mechanism, pushing forward ZnZrOx-catalyzed methanol synthesis by providing a new benchmark for this cost-effective and earth-abundant catalyst family.
    Thematic Areas: Renewable energy, sustainability and the environment Physics, condensed matter Physics, applied Materials science, multidisciplinary Materials science (miscellaneous) Materials science (all) General materials science Energy & fuels Chemistry, physical
    licence for use: https://creativecommons.org/licenses/by/3.0/es/
    Author's mail: nuria.lopez@urv.cat
    Record's date: 2024-01-13
    Papper version: info:eu-repo/semantics/publishedVersion
    Link to the original source: https://onlinelibrary.wiley.com/doi/full/10.1002/aenm.202204122
    Papper original source: Advanced Energy Materials.
    APA: Araujo, TP; Morales-Vidal, J; Zou, TS; Agrachev, M; Verstraeten, S; Willi, PO; Grass, RN; Jeschke, G; Mitchell, S; Lopez, N; Perez-Ramirez, J (2023). Design of Flame-Made ZnZrOx Catalysts for Sustainable Methanol Synthesis from CO2. Advanced Energy Materials, (), -. DOI: 10.1002/aenm.202204122
    Licence document URL: http://repositori.urv.cat/ca/proteccio-de-dades/
    Article's DOI: 10.1002/aenm.202204122
    Entity: Universitat Rovira i Virgili
    Journal publication year: 2023
    Publication Type: Journal Publications
  • Keywords:

    Chemistry, Physical,Energy & Fuels,Materials Science (Miscellaneous),Materials Science, Multidisciplinary,Physics, Applied,Physics, Condensed Matter,Renewable Energy, Sustainability and the Environment
    Zro2
    Znzrox catalysts
    Zirconia
    Total-energy calculations
    Sustainable methanol
    Surface region
    Points
    Phase-transformation
    Oxygen vacancies
    Hydrogenation
    High-temperature
    Flame spray pyrolysis
    Defects
    Co2 hydrogenation
    1st-principles
    Renewable energy, sustainability and the environment
    Physics, condensed matter
    Physics, applied
    Materials science, multidisciplinary
    Materials science (miscellaneous)
    Materials science (all)
    General materials science
    Energy & fuels
    Chemistry, physical
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