Boosting the Activity of Pd Single Atoms by Tuning Their Local Environment on Ceria for Methane Combustion.

Angew Chem Int Ed Engl

Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.

Published: January 2023

AI Article Synopsis

  • - Supported Pd single atom catalysts (SACs) show promise for methane combustion, but there are mixed opinions on their efficiency and durability.
  • - Researchers found that pre-treating ceria before adding Pd changes the catalyst's electronic and structural properties, leading to a unique anchor site for Pd single atoms.
  • - This modified Pd shows significantly improved activity for methane oxidation, with reduced reaction temperatures and much higher turnover rates, attributed to its specific local structure that enhances oxygen delivery and reaction intermediary breakdown.

Article Abstract

Supported Pd single atom catalysts (SACs) have triggered great research interest in methane combustion yet with contradicting views on their activity and stability. Here, we show that the Pd SAs can take different electronic structure and atomic geometry on ceria support, resulting in different catalytic properties. By a simple thermal pretreatment to ceria prior to Pd deposition, a unique anchoring site is created. The Pd SA, taking this site, can be activated to Pd (0<δ<2) that has greatly enhanced activity for methane oxidation: T lowered by up to 130 °C and almost 10 times higher turnover frequency compared to the untreated catalyst. The enhanced activity of Pd site is related to its oxygen-deficient local structure and elongated interacting distance with ceria, leading to enhanced capability in delivering reactive oxygen species and decomposing reaction intermediates. This work provides insights into designing highly efficient Pd SACs for oxidation reactions.

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http://dx.doi.org/10.1002/anie.202217323DOI Listing

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