In situ observation of oscillatory redox dynamics of copper

Cao, Jing; Rinaldi, Ali; Plodinec, Milivoj; Huang, Xing; Willinger, Elena; Hammud, Adnan; Hieke, Stefan; Beeg, Sebastian; Gregoratti, Luca; Colbea, Claudiu; Schlögl, Robert; Antonietti, Markus; Greiner, Mark; Willinger, Marc Georg

doi:10.1038/s41467-020-17346-7

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In situ observation of oscillatory redox dynamics of copper

MPS-Authors

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Cao, Jing
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons200441

Plodinec, Milivoj
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons39194

Huang, Xing
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Scientific Center for Optical and Electron Microscopy, ScopeMETH Zürich;

/persons/resource/persons49292

Willinger, Elena
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Scientific Center for Optical and Electron Microscopy, ScopeMETH Zürich;

/persons/resource/persons188971

Hammud, Adnan
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons22071

Schlögl, Robert
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Max Planck Institute for Chemical Energy Conversion;

/persons/resource/persons22243

Willinger, Marc Georg
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Scientific Center for Optical and Electron Microscopy, ScopeMETH Zürich;
Max-Planck-Institute of Colloids andInterfaces, Department of Colloid Chemistry;

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s41467-020-17346-7.pdf
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引用

Cao, J., Rinaldi, A., Plodinec, M., Huang, X., Willinger, E., Hammud, A., Hieke, S., Beeg, S., Gregoratti, L., Colbea, C., Schlögl, R., Antonietti, M., Greiner, M., & Willinger, M. G. (2020). In situ observation of oscillatory redox dynamics of copper. Nature Communications, 11:. doi:10.1038/s41467-020-17346-7.

引用: https://hdl.handle.net/21.11116/0000-0006-CA06-0

要旨

How a catalyst behaves microscopically under reaction conditions, and what kinds of activesites transiently exist on its surface, is still very much a mystery to the scientific community.Here we present an in situ study on the red-ox behaviour of copper in the model reaction ofhydrogen oxidation. Direct imaging combined with on-line mass spectroscopy shows thatactivity emerges near a phase boundary, where complex spatio-temporal dynamics areinduced by the competing action of simultaneously present oxidizing and reducing agents.Using a combination of in situ imaging with in situ X-ray absorption spectroscopy andscanning photoemission microscopy, we reveal the relation between chemical and mor-phological dynamics and demonstrate that a static picture of active sites is insufficient todescribe catalytic function of redox-active metal catalysts. The observed oscillatory redoxdynamics provide a unique insight on phase-cooperation and a convenient and generalmechanism for constant re-generation of transient active sites.