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Insights into Palladium Deactivation during Advanced Oxidation Processes
Verónica Pinos-Vélez1,2,3, Oscar Osegueda1,4, Dana Georgiana Crivoi1
1Chemical Engineering Department, Rovira i Virgili University, Av Paisos Catalans 26, 43007Tarragona, Spain.
Understanding catalyst deactivation is crucial. Small palladium (Pd) clusters and single atoms on corundum, prepared by impregnation, maintain activity during hydrogen cycles, unlike larger Pd nanoparticles.
Area of Science:
- Materials Science
- Catalysis
- Surface Chemistry
Background:
- Catalyst deactivation mechanisms are critical for developing efficient and durable catalysts.
- Palladium (Pd) supported on corundum (Al2O3) is a widely studied catalytic material.
Purpose of the Study:
- To investigate the behavior of Pd/corundum catalysts during hydrogen adsorption/desorption cycles.
- To elucidate the role of different Pd species (nanoparticles, clusters, single atoms) in catalyst deactivation.
Main Methods:
- Temperature-programmed desorption coupled with mass spectrometry (TPD-MS).
- Aberration-corrected transmission electron microscopy (AC-TEM).
- Preparation of Pd/corundum by impregnation and sputtering.
Main Results:
- Uniformly dispersed Pd nanoparticles were observed in both preparation methods.
- Single atoms and small Pd clusters were exclusively found in materials prepared by impregnation.
- Larger Pd nanoparticles (>2 nm) transformed into a Pd/PdHₓ core-shell structure upon hydrogen exposure.
- Pd nanoparticles <2 nm and single atoms remained unchanged.
Conclusions:
- The long-term activity of Pd/corundum catalysts prepared by impregnation is attributed to the stability of small Pd clusters and single atoms.
- Understanding the deactivation of larger Pd nanoparticles is key to improving catalyst longevity.
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