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Influence of CO on the Activation, O-Vacancy Formation, and Performance of Au/ZnO Catalysts in CO2 Hydrogenation to Methanol

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Knop-Gericke,  Axel
Research Department Schlögl, Max Planck Institute for Chemical Energy Conversion, Max Planck Society;

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Schlögl,  Robert
Research Department Schlögl, Max Planck Institute for Chemical Energy Conversion, Max Planck Society;

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Citation

Abdel-Mageed, A. M., Klyushin, A., Knop-Gericke, A., Schlögl, R., & Behm, R. J. (2019). Influence of CO on the Activation, O-Vacancy Formation, and Performance of Au/ZnO Catalysts in CO2 Hydrogenation to Methanol. The Journal of Physical Chemistry Letters, 10(13), 3645-3653. doi:10.1021/acs.jpclett.9b00925.


Cite as: http://hdl.handle.net/21.11116/0000-0005-A917-3
Abstract
The impact of CO on the activation and reaction characteristics of Au/ZnO catalysts in methanol synthesis from a CO2/H-2 mixture was studied by kinetic, near ambient pressure X-ray photoelectron spectroscopy and X-ray absorption spectroscopy at the 0 K-edge, together with in situ Foureir transform infrared measurements. Transient measurements under up to industrial reaction conditions (50 bar, 240 C) show a pronounced transient increase of the activity for methanol formation from CO2/H-2 after exposure to a CO/H-2 reaction gas mixture, while the steady-state activity is similar to that observed directly after oxidative pretreatment. For the reaction in CO/H-2, the much longer activation phase is accompanied by formation of CO2 due to reaction of CO with the ZnO catalyst support. This leads to O-vacancy formation on the support at an extent significantly higher than in CO2/H-2. The consequences of these findings on the mechanistic understanding of methanol formation from CO2/H-2 on Au/ZnO and for ZnO-supported catalysts in general are discussed.