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Redox dynamics and surface structures of an active palladium catalyst during methane oxidation

Yue, Shengnan ; Praveen, C. S. ; Klyushin, Alexander LU ; Fedorov, Alexey ; Hashimoto, Masahiro ; Li, Qian ; Jones, Travis ; Liu, Panpan ; Yu, Wenqian and Willinger, Marc Georg , et al. (2024) In Nature Communications 15(1).
Abstract

Catalysts based on palladium are among the most effective in the complete oxidation of methane. Despite extensive studies and notable advances, the nature of their catalytically active species and conceivable structural dynamics remains only partially understood. Here, we combine operando transmission electron microscopy (TEM) with near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) and density functional theory (DFT) calculations to investigate the active state and catalytic function of Pd nanoparticles (NPs) under methane oxidation conditions. We show that the particle size, phase composition and dynamics respond appreciably to changes in the gas-phase chemical potential. In combination with mass spectrometry (MS)... (More)

Catalysts based on palladium are among the most effective in the complete oxidation of methane. Despite extensive studies and notable advances, the nature of their catalytically active species and conceivable structural dynamics remains only partially understood. Here, we combine operando transmission electron microscopy (TEM) with near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) and density functional theory (DFT) calculations to investigate the active state and catalytic function of Pd nanoparticles (NPs) under methane oxidation conditions. We show that the particle size, phase composition and dynamics respond appreciably to changes in the gas-phase chemical potential. In combination with mass spectrometry (MS) conducted simultaneously with in situ observations, we uncover that the catalytically active state exhibits phase coexistence and oscillatory phase transitions between Pd and PdO. Aided by DFT calculations, we provide a rationale for the observed redox dynamics and demonstrate that the emergence of catalytic activity is related to the dynamic interplay between coexisting phases, with the resulting strained PdO having more favorable energetics for methane oxidation.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Nature Communications
volume
15
issue
1
article number
4678
publisher
Nature Publishing Group
external identifiers
  • scopus:85195017686
  • pmid:38824167
ISSN
2041-1723
DOI
10.1038/s41467-024-49134-y
language
English
LU publication?
yes
id
6191299b-e33a-439a-99be-6b663641f95c
date added to LUP
2024-07-02 13:40:37
date last changed
2024-10-09 02:07:31
@article{6191299b-e33a-439a-99be-6b663641f95c,
  abstract     = {{<p>Catalysts based on palladium are among the most effective in the complete oxidation of methane. Despite extensive studies and notable advances, the nature of their catalytically active species and conceivable structural dynamics remains only partially understood. Here, we combine operando transmission electron microscopy (TEM) with near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) and density functional theory (DFT) calculations to investigate the active state and catalytic function of Pd nanoparticles (NPs) under methane oxidation conditions. We show that the particle size, phase composition and dynamics respond appreciably to changes in the gas-phase chemical potential. In combination with mass spectrometry (MS) conducted simultaneously with in situ observations, we uncover that the catalytically active state exhibits phase coexistence and oscillatory phase transitions between Pd and PdO. Aided by DFT calculations, we provide a rationale for the observed redox dynamics and demonstrate that the emergence of catalytic activity is related to the dynamic interplay between coexisting phases, with the resulting strained PdO having more favorable energetics for methane oxidation.</p>}},
  author       = {{Yue, Shengnan and Praveen, C. S. and Klyushin, Alexander and Fedorov, Alexey and Hashimoto, Masahiro and Li, Qian and Jones, Travis and Liu, Panpan and Yu, Wenqian and Willinger, Marc Georg and Huang, Xing}},
  issn         = {{2041-1723}},
  language     = {{eng}},
  number       = {{1}},
  publisher    = {{Nature Publishing Group}},
  series       = {{Nature Communications}},
  title        = {{Redox dynamics and surface structures of an active palladium catalyst during methane oxidation}},
  url          = {{http://dx.doi.org/10.1038/s41467-024-49134-y}},
  doi          = {{10.1038/s41467-024-49134-y}},
  volume       = {{15}},
  year         = {{2024}},
}