Stroboscopic operando spectroscopy of the dynamics in heterogeneous catalysis by event-averaging

Jan Knudsen, Tamires Gallo, Virgínia Boix, Marie Døvre Strømsheim, Giulio D’Acunto, Christopher Goodwin, Harald Wallander, Suyun Zhu, Markus Soldemo, Patrick Lömker, Filippo Cavalca, Mattia Scardamaglia, David Degerman, Anders Nilsson, Peter Amann, Andrey Shavorskiy, Joachim Schnadt

Forskningsoutput: TidskriftsbidragArtikel i vetenskaplig tidskriftPeer review

Sammanfattning

Heterogeneous catalyst surfaces are dynamic entities that respond rapidly to changes in their local gas environment, and the dynamics of the response is a decisive factor for the catalysts’ action and activity. Few probes are able to map catalyst structure and local gas environment simultaneously under reaction conditions at the timescales of the dynamic changes. Here we use the CO oxidation reaction and a Pd(100) model catalyst to demonstrate how such studies can be performed by time-resolved ambient pressure photoelectron spectroscopy. Central elements of the method are cyclic gas pulsing and software-based event-averaging by image recognition of spectral features. A key finding is that at 3.2 mbar total pressure a metallic, predominantly CO-covered metallic surface turns highly active for a few seconds once the O2:CO ratio becomes high enough to lift the CO poisoning effect before mass transport limitations triggers formation of a √5 oxide.

Originalspråkengelska
Artikelnummer6117
TidskriftNature Communications
Volym12
Utgåva1
DOI
StatusPublished - 2021 dec

Bibliografisk information

Publisher Copyright:
© 2021, The Author(s).

Ämnesklassifikation (UKÄ)

  • Atom- och molekylfysik och optik
  • Annan kemiteknik

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