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<p>The use of redox active metal oxides to support noble metals is critical in the design of highly-active CO oxidation catalysts for gas emissions control. Unfortunately, supports promoting the activity, such as CeO<sub>2</sub>, tend also to promote acute catalyst deactivation by turning highly-active metallic Pt clusters into less-active PtO<sub>x</sub> species, under practical reaction conditions (high-temperature and/or the excess of O<sub>2</sub>). This leads to a problematic activity/stability tradeoff where Pt/CeO<sub>2</sub> catalysts, highly-active, and Pt on non-reducible supports, highly stable, are bookends. Herein, we report a method to trap Pt at V-shaped pockets/stepped sites of CeO<sub>2</sub> that break this undesired correlation by showing both high activity and stability in the CO oxidation reaction. XAS, CO-DRIFT, XPS, HAADF-STEM, and DFT are used to infer that the generation of low order metallic Pt clusters connected to two crystallographic planes of the support is key to inhibit (deactivating) re-oxidation paths of the metal, as a result of the high-energy required to form disordered/distorted PtO<sub>x</sub> ensembles at these positions. This new material allows, thus, to operate outside the commonly observed, limiting, activity/stability tradeoff.</p>

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Overcoming activity/stability tradeoffs in CO oxidation catalysis by Pt/CeO2

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年8月12日

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  • Benjamin Bohigues,
  • Sergio Rojas-Buzo,
  • Davide Salusso,
  • Yu Xia,
  • Avelino Corma,
  • Silvia Bordiga,
  • Mercedes Boronat,
  • Tom Willhammar,
  • Manuel Moliner,
  • Pedro Serna

摘要

The use of redox active metal oxides to support noble metals is critical in the design of highly-active CO oxidation catalysts for gas emissions control. Unfortunately, supports promoting the activity, such as CeO2, tend also to promote acute catalyst deactivation by turning highly-active metallic Pt clusters into less-active PtOx species, under practical reaction conditions (high-temperature and/or the excess of O2). This leads to a problematic activity/stability tradeoff where Pt/CeO2 catalysts, highly-active, and Pt on non-reducible supports, highly stable, are bookends. Herein, we report a method to trap Pt at V-shaped pockets/stepped sites of CeO2 that break this undesired correlation by showing both high activity and stability in the CO oxidation reaction. XAS, CO-DRIFT, XPS, HAADF-STEM, and DFT are used to infer that the generation of low order metallic Pt clusters connected to two crystallographic planes of the support is key to inhibit (deactivating) re-oxidation paths of the metal, as a result of the high-energy required to form disordered/distorted PtOx ensembles at these positions. This new material allows, thus, to operate outside the commonly observed, limiting, activity/stability tradeoff.