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Ethylene Epoxidation at the Phase Transition of Copper Oxides

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Greiner,  Mark
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Jones,  Travis
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Klyushin,  Alexander
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Knop-Gericke,  Axel
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Schlögl,  Robert
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Citation

Greiner, M., Jones, T., Klyushin, A., Knop-Gericke, A., & Schlögl, R. (2017). Ethylene Epoxidation at the Phase Transition of Copper Oxides. Journal of the American Chemical Society, 139(34), 11825-11832. doi:10.1021/jacs.7b05004.


Cite as: https://hdl.handle.net/11858/00-001M-0000-002D-D6BA-B
Abstract
Catalytic materials tend to be metastable. When a material becomes metastable close to a thermodynamic phase transition it can exhibit unique catalytic behavior. Using in situ photoemission spectroscopy and online product analysis, we have found that close to the Cu2O−CuO phase transition there is a boost in activity for a kinetically driven reaction, ethylene epoxidation, giving rise to a 20-fold selectivity enhancement relative to the selectivity observed far from the phase transition. By tuning conditions toward low oxygen chemical potential, this metastable state and the resulting enhanced selectivity can be sustained. Using density functional theory, we find that metastable O precursors to the CuO phase can account for the selectivity enhancements near the phase transition.