Presentation Information

[2P10]In-situ observation of a Cu-Zn/Al2O3 catalyst during CO2 hydrogenation conditions using fluorescence-yield dispersive soft X-ray absorption spectroscopy

*Daiki Kanesada1, Kota Enomoto1, Fumitoshi Kumaki1,2, Ryo Toyoshima3, Yuki Tsujikawa2, Kaoruho Sakata2, Kenta Amemiya2, Hiroshi Kondoh1 (1. Keio University (Japan), 2. KEK-IMSS (Japan), 3. The University of Tokyo (Japan))
Methanol synthesis from CO2 hydrogenation is crucial for achieving carbon neutrality, but the active sites of Cu-Zn/Al2O3 catalysts remain controversial. In this study, the chemical state changes of copper were investigated by in-situ fluorescence-yield dispersive soft X-ray absorption spectroscopy (FY-DsXAS) under near-ambient-pressure CO2 and H2 gas conditions. The catalyst sample was pre-reduced by heating in a H2 atmosphere, turning the initial Cu2+ state into Cu0. Under a mixed gas of CO2 (5 Torr) and H2 (10 Torr), partial oxidation from Cu0 to Cu+ was observed from 200℃ to 275℃, whereas a reduction from Cu+ to Cu0 occurred from 275℃ to 300℃. A similar oxidation behavior was also observed under CO2 gas alone, indicating that this oxidation originates from the dissociation of CO2. Furthermore, this transient Cu+ formation was not observed during subsequent CO2 and H2 refill and re-heating. We will discuss this transient oxidation and the catalytic activity.

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