In situ observation of oscillatory redox dynamics of copper

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

doi:10.1038/s41467-020-17346-7

In situ observation of oscillatory redox dynamics of copper

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

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

40 Scopus citations

Abstract

How a catalyst behaves microscopically under reaction conditions, and what kinds of active sites 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 of hydrogen oxidation. Direct imaging combined with on-line mass spectroscopy shows that activity emerges near a phase boundary, where complex spatio-temporal dynamics are induced 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 and scanning photoemission microscopy, we reveal the relation between chemical and morphological dynamics and demonstrate that a static picture of active sites is insufficient to describe catalytic function of redox-active metal catalysts. The observed oscillatory redox dynamics provide a unique insight on phase-cooperation and a convenient and general mechanism for constant re-generation of transient active sites.

Original language	English
Article number	3554
Journal	Nature Communications
Volume	11
Issue number	1
DOIs	https://doi.org/10.1038/s41467-020-17346-7
State	Published - 1 Dec 2020

Bibliographical note

Publisher Copyright:
© 2020, The Author(s).

ASJC Scopus subject areas

General Chemistry
General Biochemistry, Genetics and Molecular Biology
General Physics and Astronomy

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title = "In situ observation of oscillatory redox dynamics of copper",

abstract = "How a catalyst behaves microscopically under reaction conditions, and what kinds of active sites 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 of hydrogen oxidation. Direct imaging combined with on-line mass spectroscopy shows that activity emerges near a phase boundary, where complex spatio-temporal dynamics are induced 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 and scanning photoemission microscopy, we reveal the relation between chemical and morphological dynamics and demonstrate that a static picture of active sites is insufficient to describe catalytic function of redox-active metal catalysts. The observed oscillatory redox dynamics provide a unique insight on phase-cooperation and a convenient and general mechanism for constant re-generation of transient active sites.",

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AU - Cao, Jing

AU - Rinaldi, Ali

AU - Plodinec, Milivoj

AU - Huang, Xing

AU - Willinger, Elena

AU - Hammud, Adnan

AU - Hieke, Stefan

AU - Beeg, Sebastian

AU - Gregoratti, Luca

AU - Colbea, Claudiu

AU - Schlögl, Robert

AU - Antonietti, Markus

AU - Greiner, Mark

AU - Willinger, Marc

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Y1 - 2020/12/1

N2 - How a catalyst behaves microscopically under reaction conditions, and what kinds of active sites 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 of hydrogen oxidation. Direct imaging combined with on-line mass spectroscopy shows that activity emerges near a phase boundary, where complex spatio-temporal dynamics are induced 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 and scanning photoemission microscopy, we reveal the relation between chemical and morphological dynamics and demonstrate that a static picture of active sites is insufficient to describe catalytic function of redox-active metal catalysts. The observed oscillatory redox dynamics provide a unique insight on phase-cooperation and a convenient and general mechanism for constant re-generation of transient active sites.

AB - How a catalyst behaves microscopically under reaction conditions, and what kinds of active sites 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 of hydrogen oxidation. Direct imaging combined with on-line mass spectroscopy shows that activity emerges near a phase boundary, where complex spatio-temporal dynamics are induced 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 and scanning photoemission microscopy, we reveal the relation between chemical and morphological dynamics and demonstrate that a static picture of active sites is insufficient to describe catalytic function of redox-active metal catalysts. The observed oscillatory redox dynamics provide a unique insight on phase-cooperation and a convenient and general mechanism for constant re-generation of transient active sites.

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JO - Nature Communications

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ER -

In situ observation of oscillatory redox dynamics of copper

Abstract

Bibliographical note

ASJC Scopus subject areas

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