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In Situ Dispersion of Palladium on TiO2 During Reverse Water-Gas Shift Reaction: Formation of Atomically Dispersed Palladium.

Nicholas C NelsonLinxiao ChenDebora Motta MeiraLibor KovarikJános Szanyi
Published in: Angewandte Chemie (International ed. in English) (2020)
The application of single-atom catalysts (SACs) to high-temperature hydrogenation requires materials that thermodynamically favor metal atom isolation over cluster formation. We demonstrate that Pd can be predominantly dispersed as isolated atoms onto TiO2 during the reverse water-gas shift (rWGS) reaction at 400 °C. Achieving atomic dispersion requires an artificial increase of the absolute TiO2 surface area by an order of magnitude and can be accomplished by physically mixing a precatalyst (Pd/TiO2 ) with neat TiO2 prior to the rWGS reaction. The in situ dispersion of Pd was reflected through a continuous increase of rWGS activity over 92 h and supported by kinetic analysis, infrared and X-ray absorption spectroscopies and scanning transmission electron microscopy. The thermodynamic stability of Pd under high-temperature rWGS conditions is associated with Pd-Ti coordination, which manifests upon O-vacancy formation, and the artificial increase in TiO2 surface area.
Keyphrases
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