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Carbon subsurface traffic jam as driver for methane oxidation activity and selectivity on palladium surfaces

Küst, Ulrike LU orcid ; Jones, Rosemary LU ; Prumbs, Julia LU ; Namar, Alessandro ; Scardamaglia, Mattia LU ; Shavorskiy, Andrey LU and Knudsen, Jan LU (2025) In Nature Communications 16(1).
Abstract

Separating how surface and subsurface species affect catalytic function is a challenging task in heterogeneous catalysis, particularly when deposition and segregation take place at reaction conditions. Here, we report on an operando approach to establish surface/subsurface/function correlations. Using temperature modulations we oscillate carbon deposition and segregation over a Pd catalyst. Catalytic composition and function are monitored during methane oxidation showing that the surface coverage of carbon drives partial oxidation to CO, while subsurface carbon controls the overall methane turnover. Also, we show that a carbon traffic jam in the subsurface leads to a shifting selectivity from H2 to H2O formation,... (More)

Separating how surface and subsurface species affect catalytic function is a challenging task in heterogeneous catalysis, particularly when deposition and segregation take place at reaction conditions. Here, we report on an operando approach to establish surface/subsurface/function correlations. Using temperature modulations we oscillate carbon deposition and segregation over a Pd catalyst. Catalytic composition and function are monitored during methane oxidation showing that the surface coverage of carbon drives partial oxidation to CO, while subsurface carbon controls the overall methane turnover. Also, we show that a carbon traffic jam in the subsurface leads to a shifting selectivity from H2 to H2O formation, highlighting the importance of the catalyst subsurface for the catalytic reaction.

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Please use this url to cite or link to this publication:
author
; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Nature Communications
volume
16
issue
1
article number
7755
publisher
Nature Publishing Group
external identifiers
  • pmid:40835836
  • scopus:105013799925
ISSN
2041-1723
DOI
10.1038/s41467-025-63088-9
language
English
LU publication?
yes
id
26916b13-0b2d-4127-8917-cf1027f5ef51
date added to LUP
2025-10-03 12:14:42
date last changed
2025-10-17 14:08:30
@article{26916b13-0b2d-4127-8917-cf1027f5ef51,
  abstract     = {{<p>Separating how surface and subsurface species affect catalytic function is a challenging task in heterogeneous catalysis, particularly when deposition and segregation take place at reaction conditions. Here, we report on an operando approach to establish surface/subsurface/function correlations. Using temperature modulations we oscillate carbon deposition and segregation over a Pd catalyst. Catalytic composition and function are monitored during methane oxidation showing that the surface coverage of carbon drives partial oxidation to CO, while subsurface carbon controls the overall methane turnover. Also, we show that a carbon traffic jam in the subsurface leads to a shifting selectivity from H<sub>2</sub> to H<sub>2</sub>O formation, highlighting the importance of the catalyst subsurface for the catalytic reaction.</p>}},
  author       = {{Küst, Ulrike and Jones, Rosemary and Prumbs, Julia and Namar, Alessandro and Scardamaglia, Mattia and Shavorskiy, Andrey and Knudsen, Jan}},
  issn         = {{2041-1723}},
  language     = {{eng}},
  number       = {{1}},
  publisher    = {{Nature Publishing Group}},
  series       = {{Nature Communications}},
  title        = {{Carbon subsurface traffic jam as driver for methane oxidation activity and selectivity on palladium surfaces}},
  url          = {{http://dx.doi.org/10.1038/s41467-025-63088-9}},
  doi          = {{10.1038/s41467-025-63088-9}},
  volume       = {{16}},
  year         = {{2025}},
}