Oxygen Chemisorption, Formation, and Thermal Stability of Pt Oxides on Pt Nanoparticles Supported on SiO<sub>2</sub>/Si(001): Size Effects

Ono, Luis K.; Croy, Jason R.; Heinrich, Helge; Cuenya, Beatriz Roldán

doi:10.1021/jp204743q

Cited by 122 publications

(168 citation statements)

References 84 publications

(149 reference statements)

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“…Thus, we assume that the bulk oxides formed from the smaller nanoparticles whereas the larger paticles underwent the oxygen-induced shape changes discussed earlier. Such a size-dependent oxidation behaviour was also reported for other nanoparticle systems 54,76,77 .…”

Section: Pt Bulk Oxide Formationsupporting

confidence: 80%

“…Not much is known about the structure of completely oxidized Pt nanoparticles either. In a recent study combining atomic force microscopy (AFM), transmission electron microscopy (TEM), XPS and thermal programmed desorption (TPD) the size dependence of Pt nanoparticles with respect to bulk oxide formation and the thermal stability of the resulting Pt oxides was investigated 54 . It was concluded that oxide formation was more favorable on smaller particles.…”

Section: Introductionmentioning

confidence: 99%

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In Situ Oxidation Study of Pt Nanoparticles on MgO(001)

et al. 2013

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Noble metal nanoparticles supported by oxide carriers are widely employed in heterogeneous catalysis. In order to improve catalyst efficiency it is important to understand oxidation processes on the atomic scale. Here we studied oxygen-induced shape changes of Pt nanoparticles on MgO(001) by means of in-situ surface x-ray diffraction (SXRD) and x-ray reflectivity measurements (XRR). The x-ray results on the particle morphology were complemented by transmission electron microscopy (TEM) studies. The samples were prepared by means of physical vapor deposition and differed in average particle size and lateral particle size distribution. The oxygen-induced particle shape changes were found to be independent of particle size * To whom correspondence should be addressed † Max-Planck-Institut für Intelligente Systeme (former Max-Planck-Institut für Metallforschung), Heisenbergstr. and were characterized by the emergence of higher indexed facets. We propose a particle sizedependent oxidation behavior with a kinetically hindered bulk oxide formation. The formed bulk oxide structures were concluded to be (110)-oriented Pt 3 O 4 and a modified structure of (0001)-oriented α-PtO 2 . CO exposure of the oxidized particles did not lead to a shape change reversibility.

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Section: Pt Bulk Oxide Formationsupporting

confidence: 80%

Section: Introductionmentioning

confidence: 99%

In Situ Oxidation Study of Pt Nanoparticles on MgO(001)

et al. 2013

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“…20,38 There is a dominant Pt 4f 7/2 peak at 73.9 eV arising from PtO 2 , and a minor contribution at 72.3 eV due to Pt 2+ (PtO), but no detectable Pt 0 . When comparing two samples with different average NP size distributions, the largest initial content of PtO 2 species was observed for the smaller NPs: sample S2 comprises 83% PtO 2 and 17% PtO, versus 68% PtO 2 and 32% PtO for sample S1.…”

Section: Resultsmentioning

confidence: 99%

“…The polymer shells were then removed using an ultrahigh vacuum oxygen plasma source (SPECS, GmbH), which leaves behind oxidized platinum NPs. 20,38 2.2. Sample Characterization.…”

Section: Methodsmentioning

confidence: 99%

“…This phenomenon, which limits the degree to which catalysts can be dispersed, possibly arises from the stronger binding of oxygen to smaller NPs. 20,21 In particular, higher surface concentrations of chemisorbed OH, O, or PtO x species may hinder the reduction of O 2 . 21,22 Knowledge of the chemical state of Pt under oxidizing conditions is needed for an understanding of the degradation of fuel cell performance during long-term operation, due primarily to the loss of electrocatalytic surface area at the cathode at high potentials.…”

Section: Introductionmentioning

confidence: 99%

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Electrochemical Oxidation of Size-Selected Pt Nanoparticles Studied Using in Situ High-Energy-Resolution X-ray Absorption Spectroscopy

Merte

Behafarid

Miller³

et al. 2012

ACS Catal.

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109

133

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High-energy-resolution fluorescence-detected Xray absorption spectroscopy (HERFD-XAS) has been applied to study the chemical state of ∼1.2 nm size-selected Pt nanoparticles (NPs) in an electrochemical environment under potential control. Spectral features due to chemisorbed hydrogen, chemisorbed O/ OH, and platinum oxides can be distinguished with increasing potential. Pt electro-oxidation follows two competitive pathways involving both oxide formation and Pt dissolution.

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Dewetting of Pt Nanoparticles Boosts Electrocatalytic Hydrogen Evolution Due to Electronic Metal‐Support Interaction

Harsha,

Sharma,

Dierner

et al. 2024

Adv Funct Materials

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Solid‐state dewetting is the heat‐induced agglomeration of thin metal films into defined nanoparticles (NPs). Dewetted Pt nanoparticles are investigated on F‐doped SnO2 (FTO) substrates as model binder‐free electrodes for the hydrogen evolution reaction (HER). Dewetting of Pt films into particles exposes the FTO substrate and the metal/support (Pt‐FTO) contact line. Despite the decrease in Pt electrochemical surface area (ECSA) upon dewetting, dewetted NPs show a >3‐fold increase in ECSA‐normalized HER activity compared to as‐deposited nanocrystalline Pt films. Electrodes designed with dewetted Pt NPs of different sizes show that the HER activity does not only correlate with the ECSA but also increases with increasing the Pt‐FTO contact line length. The smaller the NPs, the larger the Pt‐FTO contact line, and the higher the activity. This effect is ascribed to electronic metal‐support interaction (EMSI), due to electron transfer from FTO to Pt. It is proposed that EMSI effects alter the electronic structure of Pt sites near the Pt‐FTO contact line, facilitating the H2 evolution kinetics. When NPs are a few nm‐sized, a large mass fraction of Pt is affected by EMSI, resulting in a further increase of HER activity compared to NPs ≥10 nm despite the lower ECSA.

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Oxygen Chemisorption, Formation, and Thermal Stability of Pt Oxides on Pt Nanoparticles Supported on SiO₂/Si(001): Size Effects

Cited by 122 publications

References 84 publications

In Situ Oxidation Study of Pt Nanoparticles on MgO(001)

In Situ Oxidation Study of Pt Nanoparticles on MgO(001)

Electrochemical Oxidation of Size-Selected Pt Nanoparticles Studied Using in Situ High-Energy-Resolution X-ray Absorption Spectroscopy

Dewetting of Pt Nanoparticles Boosts Electrocatalytic Hydrogen Evolution Due to Electronic Metal‐Support Interaction

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Oxygen Chemisorption, Formation, and Thermal Stability of Pt Oxides on Pt Nanoparticles Supported on SiO2/Si(001): Size Effects

Cited by 122 publications

References 84 publications

In Situ Oxidation Study of Pt Nanoparticles on MgO(001)

In Situ Oxidation Study of Pt Nanoparticles on MgO(001)

Electrochemical Oxidation of Size-Selected Pt Nanoparticles Studied Using in Situ High-Energy-Resolution X-ray Absorption Spectroscopy

Dewetting of Pt Nanoparticles Boosts Electrocatalytic Hydrogen Evolution Due to Electronic Metal‐Support Interaction

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Oxygen Chemisorption, Formation, and Thermal Stability of Pt Oxides on Pt Nanoparticles Supported on SiO₂/Si(001): Size Effects