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 2020 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. application/pdf https://sonar.ch/global/documents/185642 eng info:eu-repo/semantics/altIdentifier/doi/10.1038/s41467-020-17346-7 info:eu-repo/semantics/altIdentifier/pmid/32678088 info:eu-repo/semantics/openAccess Nature communications. - 2020 General Biochemistry, Genetics and Molecular Biology General Physics and Astronomy General Chemistry In situ observation of oscillatory redox dynamics of copper. http://purl.org/coar/resource_type/c_6501