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Enhanced Methanol Synthesis from CO2 Hydrogenation Achieved by Tuning the Cu-ZnO Interaction in ZnO/Cu2O Nanocube Catalysts Supported on ZrO2 and SiO2

MPS-Authors
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Kordus,  David       
Interface Science, Fritz Haber Institute, Max Planck Society;

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Widrinna,  Simon
Interface Science, Fritz Haber Institute, Max Planck Society;

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Timoshenko,  Janis       
Interface Science, Fritz Haber Institute, Max Planck Society;

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Lopez-Luna,  Mauricio       
Interface Science, Fritz Haber Institute, Max Planck Society;

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Rettenmaier,  Clara       
Interface Science, Fritz Haber Institute, Max Planck Society;

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Chee,  See Wee       
Interface Science, Fritz Haber Institute, Max Planck Society;

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Ortega,  Eduardo
Interface Science, Fritz Haber Institute, Max Planck Society;

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Karslıoğlu,  Osman
Interface Science, Fritz Haber Institute, Max Planck Society;

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Kühl,  Stefanie
Interface Science, Fritz Haber Institute, Max Planck Society;

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Roldan Cuenya,  Beatriz       
Interface Science, Fritz Haber Institute, Max Planck Society;

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引用

Kordus, D., Widrinna, S., Timoshenko, J., Lopez-Luna, M., Rettenmaier, C., Chee, S. W., Ortega, E., Karslıoğlu, O., Kühl, S., & Roldan Cuenya, B. (2024). Enhanced Methanol Synthesis from CO2 Hydrogenation Achieved by Tuning the Cu-ZnO Interaction in ZnO/Cu2O Nanocube Catalysts Supported on ZrO2 and SiO2. Journal of the American Chemical Society, 146(12), 8677-8687. doi:10.1021/jacs.4c01077.


引用: https://hdl.handle.net/21.11116/0000-000E-7EB3-B
要旨
The nature of the Cu–Zn interaction and especially the role of Zn in Cu/ZnO catalysts used for methanol synthesis from CO2 hydrogenation are still debated. Migration of Zn onto the Cu surface during reaction results in a Cu–ZnO interface, which is crucial for the catalytic activity. However, whether a Cu–Zn alloy or a Cu–ZnO structure is formed and the transformation of this interface under working conditions demand further investigation. Here, ZnO/Cu2O core–shell cubic nanoparticles with various ZnO shell thicknesses, supported on SiO2 or ZrO2 were prepared to create an intimate contact between Cu and ZnO. The evolution of the catalyst’s structure and composition during and after the CO2 hydrogenation reaction were investigated by means of operando spectroscopy, diffraction, and ex situ microscopy methods. The Zn loading has a direct effect on the oxidation state of Zn, which, in turn, affects the catalytic performance. High Zn loadings, resulting in a stable ZnO catalyst shell, lead to increased methanol production when compared to Zn-free particles. Low Zn loadings, in contrast, leading to the presence of metallic Zn species during reaction, showed no significant improvement over the bare Cu particles. Therefore, our work highlights that there is a minimum content of Zn (or optimum ZnO shell thickness) needed to activate the Cu catalyst. Furthermore, in order to minimize catalyst deactivation, the Zn species must be present as ZnOx and not metallic Zn or Cu–Zn alloy, which is undesirably formed during the reaction when the precatalyst ZnO overlayer is too thin.