Hydrogen spillover on cerium-based catalysts

Виканова, К. В.; Редина, Е. А.; Кustov, Leonid М.

doi:10.1007/s11172-022-3567-2

Cited by 5 publications

(2 citation statements)

References 75 publications

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“…The addition of PGMs to CeO 2 has been proposed to introduce an additional H 2 reaction pathway on CeO 2 through homolytic H 2 activation on the metal and subsequent H-spillover to CeO 2 , forming 2 OH ads – and 2 Ce 3+ simultaneously (eq ). ,,, normalP normalt + normalH 2 + 2 normalO 2 − + 2 normalC normale 4 + → normalP normalt + 2 normalO normalH normala normald normals − + 2 normalC normale 3 + …”

Section: Resultsmentioning

confidence: 99%

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How Pt Influences H₂ Reactions on High Surface-Area Pt/CeO₂ Powder Catalyst Surfaces

Lee

Tieu

Finzel

et al. 2023

JACS Au

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The addition of platinum-group metals (PGMs, e.g., Pt) to CeO2 is used in heterogeneous catalysis to promote the rate of redox surface reactions. Well-defined model system studies have shown that PGMs facilitate H2 dissociation, H-spillover onto CeO2 surfaces, and CeO2 surface reduction. However, it remains unclear how the heterogeneous structures and interfaces that exist on powder catalysts influence the mechanistic picture of PGM-promoted H2 reactions on CeO2 surfaces developed from model system studies. Here, controlled catalyst synthesis, temperature-programmed reduction (TPR), in situ infrared spectroscopy (IR), and in situ electron energy loss spectroscopy (EELS) were used to interrogate the mechanisms of how Pt nanoclusters and single atoms influence H2 reactions on high-surface area Pt/CeO2 powder catalysts. TPR showed that Pt promotes H2 consumption rates on Pt/CeO2 even when Pt exists on a small fraction of CeO2 particles, suggesting that H-spillover proceeds far from Pt–CeO2 interfaces and across CeO2–CeO2 particle interfaces. IR and EELS measurements provided evidence that Pt changes the mechanism of H2 activation and the rate limiting step for Ce3+, oxygen vacancy, and water formation as compared to pure CeO2. As a result, higher-saturation surface hydroxyl coverages can be achieved on Pt/CeO2 compared to pure CeO2. Further, Ce3+ formed by spillover-H from Pt is heterogeneously distributed and localized at and around interparticle CeO2–CeO2 boundaries, while activated H2 on pure CeO2 results in homogeneously distributed Ce3+. Ce3+ localization at and around CeO2–CeO2 boundaries for Pt/CeO2 is accompanied by surface reconstruction that enables faster rates of H2 consumption. This study reconciles the materials gap between model structures and powder catalysts for H2 reactions with Pt/CeO2 and highlights how the spatial heterogeneity of powder catalysts dictates the influence of Pt on H2 reactions at CeO2 surfaces.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

How Pt Influences H₂ Reactions on High Surface-Area Pt/CeO₂ Powder Catalyst Surfaces

Lee

Tieu

Finzel

et al. 2023

JACS Au

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Hydrogen transfer from the anthracene oil of coal tar: thermal reaction with α-methylstyrene

Krasikova,

Pervova,

Andreikov

et al. 2023

Russ Chem Bull

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Effect of preparation method on active sites variation for catalytic oxidation of toluene over Pt/MCM-48

Tang

Yang

et al. 2023

Applied Catalysis A: General

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Hydrogen spillover on cerium-based catalysts

Cited by 5 publications

References 75 publications

How Pt Influences H₂ Reactions on High Surface-Area Pt/CeO₂ Powder Catalyst Surfaces

How Pt Influences H₂ Reactions on High Surface-Area Pt/CeO₂ Powder Catalyst Surfaces

Hydrogen transfer from the anthracene oil of coal tar: thermal reaction with α-methylstyrene

Effect of preparation method on active sites variation for catalytic oxidation of toluene over Pt/MCM-48

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Hydrogen spillover on cerium-based catalysts

Cited by 5 publications

References 75 publications

How Pt Influences H2 Reactions on High Surface-Area Pt/CeO2 Powder Catalyst Surfaces

How Pt Influences H2 Reactions on High Surface-Area Pt/CeO2 Powder Catalyst Surfaces

Hydrogen transfer from the anthracene oil of coal tar: thermal reaction with α-methylstyrene

Effect of preparation method on active sites variation for catalytic oxidation of toluene over Pt/MCM-48

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Product

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How Pt Influences H₂ Reactions on High Surface-Area Pt/CeO₂ Powder Catalyst Surfaces

How Pt Influences H₂ Reactions on High Surface-Area Pt/CeO₂ Powder Catalyst Surfaces