Periodic structural changes in Pd nanoparticles during oscillatory CO oxidation reaction

Tanmay Ghosh, Juan Manuel Arce-Ramos, Wen-Qing Li, Hongwei Yan, See Wee Chee, Alexander Genest and Utkur Mirsaidov ()
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Tanmay Ghosh: National University of Singapore
Juan Manuel Arce-Ramos: Agency for Science, Technology and Research
Wen-Qing Li: Agency for Science, Technology and Research
Hongwei Yan: National University of Singapore
See Wee Chee: National University of Singapore
Alexander Genest: Agency for Science, Technology and Research
Utkur Mirsaidov: National University of Singapore

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract Nanoparticle (NP) catalysts are ubiquitous in energy systems, chemical production, and reducing the environmental impact of many industrial processes. Under reactive environments, the availability of catalytically active sites on the NP surface is determined by its dynamic structure. However, atomic-scale insights into how a NP surface reconstructs under reaction conditions and the impact of the reconstruction on catalytic activity are still lacking. Using operando transmission electron microscopy, we show that Pd NPs exhibit periodic round–to–flat transitions altering their facets during CO oxidation reaction at atmospheric pressure and elevated temperatures. This restructuring causes spontaneous oscillations in the conversion of CO to CO2 under constant reaction conditions. Our study reveals that the oscillatory behavior stems from the CO-adsorption-mediated periodic restructuring of the nanocatalysts between high-index-faceted round and low-index-faceted flat shapes. These atomic-scale insights into the dynamic surface properties of NPs under reactive conditions play an important role in the design of high-performance catalysts.

Date: 2022
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DOI: 10.1038/s41467-022-33304-x

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