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

Shengnan Yue, C. S. Praveen, Alexander Klyushin, Alexey Fedorov, Masahiro Hashimoto, Qian Li, Travis Jones (), Panpan Liu, Wenqian Yu, Marc-Georg Willinger and Xing Huang ()
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Shengnan Yue: Fuzhou University
C. S. Praveen: Cochin University of Science and Technology
Alexander Klyushin: Lund University
Alexey Fedorov: ETH Zurich
Masahiro Hashimoto: allée de Giverny
Qian Li: Fuzhou University
Travis Jones: Los Alamos National Laboratory
Panpan Liu: Fuzhou University
Wenqian Yu: Fuzhou University
Marc-Georg Willinger: ETH Zurich
Xing Huang: Fuzhou University

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: 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) 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.

Date: 2024
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DOI: 10.1038/s41467-024-49134-y

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