Chasing PtO  species in ceria supported platinum during CO oxidation extinction with correlative operando spectroscopic techniques

Di, Mengqiao; Simmance, Kerry; Schaëfer, Andreas; Feng, Yanyue; Hemmingsson, Felix; Skoglundh, Magnus; Bell, Tamsin; Thompsett, David; Jensen, Lucy Idowu Ajakaiye; Blomberg, Sara; Carlsson, Per-Anders

doi:10.1016/j.jcat.2022.03.022

Cited by 17 publications

(18 citation statements)

References 63 publications

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“…The reaction shows bistability and we include also the extinction results for the case of a CO pressure of 0.2 kPa. 17 The bistability window is about 40 and 25 °C for Pt/Al 2 O 3 and Pt/CeO 2 , respectively.…”

Section: ■ Results and Discussionmentioning

confidence: 97%

“…The diameter of Pt 34 is about 0.8 nm and comparable with the experimental average value, which has been measured to be 1 nm. 17 The particle exposes a Pt(100) microfacet to the oxide support. CeO 2 (111) is constructed with five O−Ce−O trilayers.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…The reaction order measurements are performed in a vertical fixed-bed powder reactor described elsewhere . The effluent gas is detected by a Fourier transform infrared spectrometer (MKS MultiGas 2030 FTIR).…”

Section: Experimental and Computational Methodsmentioning

confidence: 99%

“…The reaction order measurements are performed in a vertical fixedbed powder reactor described elsewhere. 17 The effluent gas is detected by a Fourier transform infrared spectrometer (MKS MultiGas 2030 FTIR). The catalyst sample is sieved, and the The catalyst performance is evaluated by using the reactor described above, and the effluent gas is analyzed by using a mass spectrometer (Hiden HPR-20) monitoring the m/e ratios 28 (CO), 32 (O 2 ), and 44 (CO 2 ).…”

Section: ■ Introductionmentioning

confidence: 99%

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Interface Reactions Dominate Low-Temperature CO Oxidation Activity over Pt/CeO₂

Bosio

Skoglundh

et al. 2022

J. Phys. Chem. C

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First-principles-based kinetic Monte Carlo simulations and kinetic experiments are used to explore CO oxidation over Pt/CeO2. The simulations compare CO oxidation over a ceria-supported ∼1 nm particle with simulations of a free-standing particle and Pt(111). The onset of the CO oxidation over ceria supported Pt is shifted to lower temperatures compared to the unsupported systems thanks to a Mars–van Krevelen mechanism at the Pt/CeO2 interface perimeter, which is not sensitive to CO poisoning. Both the Mars–van Krevelen mechanism and the conventional Langmuir–Hinshelwood mechanism over the Pt nanoparticle are contributing to the conversion after the reaction onset. The reaction orders in CO and O2 are compared experimentally for Pt/CeO2 and Pt/Al2O3. The reaction orders over Pt/CeO2 are close to zero for both CO and O2, whereas the corresponding reaction orders are −0.75 and 0.68 over Pt/Al2O3. The measured zero orders for Pt/CeO2 show the absence of CO/O2 site competition and underline the relevance of interface reactions. The measurements for Pt/Al2O3 indicate that the main reaction path for CO oxidation over Pt is a conventional Langmuir–Hinshelwood reaction. The results elucidate the interplay between condition-dependent reaction mechanisms for CO oxidation over Pt supported on reducible oxides.

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Section: ■ Results and Discussionmentioning

confidence: 97%

Section: ■ Results and Discussionmentioning

confidence: 99%

Section: Experimental and Computational Methodsmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Interface Reactions Dominate Low-Temperature CO Oxidation Activity over Pt/CeO₂

Bosio

Skoglundh

et al. 2022

J. Phys. Chem. C

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“…Carbon monoxide is a harmful pollutant [1][2][3], especially indoors or inside vehicle cabins, and many efforts have been devoted to oxidize CO to CO 2 at low temperatures. Au and Pt-based catalysts are particularly active at room temperature, and promoted by the presence of moisture [4][5][6].…”

Section: Introductionmentioning

confidence: 99%

Stability of Pt-Adsorbed CO on Catalysts for Room Temperature-Oxidation of CO

et al. 2022

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A large signal of gas-phase CO overlapping with those of adsorbates is often present when investigating catalysts by operando diffuse reflectance FT-IR spectroscopy. Physically removing CO(g) from the IR cell may lead to a fast decay of adsorbate signals. Our work shows that carbonyls adsorbed on metallic Pt sites fully vanished in less than 10 min at 30 °C upon removing CO(g) when redox supports were used. In contrast, a broad band assigned to CO adsorbed on oxidized Pt sites was stable. It was concluded that physically removing CO(g) at room temperature during IR analyses will most likely lead to changes in the distribution of CO(ads) and a misrepresentation of the Pt site speciation, misguiding the development of efficient low-temperature CO oxidation catalysts. A tentative representation of the nature of the Pt phases present depending on the feed composition is also proposed.

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Deposited PtGe Clusters as Active and Durable Catalysts for CO Oxidation**

Ugartemendia,

Mercero,

de Cózar

et al. 2024

ChemCatChem

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Control of CO emissions raises serious environmental concerns in the current chemical industry, as well as in nascent technologies based on hydrogen such as electrolyzers and fuel cells. Pt remains one of the state‐of‐art catalysts for the CO oxidation reaction, but suffers from CO self–poisoning. Recently, PtGe alloys were proposed as an excellent alternative to reduce CO poisoning. In this work we investigate the impact of Ge content on the CO oxidation kinetics of P4Gen subnanoclusters supported on MgO. Pt−Ge nanoalloys act as a bifunctional catalyst by displaying dual adsorption sites; i.e., CO is adsorbed on Pt whereas oxygen binds to Ge, forming an alternative oxygen source GeOx. Besides, Ge alloying modifies the electronic structure of Pt (ligand effects) and reduces the affinity to CO. In this way, the competition between CO and O2 adsorption and the overbinding of CO is alleviated, achieving a CO poisoning−free kinetic regime. Our calculations suggest that Pt4Ge3 is the optimal catalyst, evidencing that alloying composition is a parameter of extreme importance in nanocatalyst design. The work relies on global optimization search techniques to determine the accessibility of multiple structures at different conditions, mechanistic studies and microkinetic modelling

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Chasing PtO species in ceria supported platinum during CO oxidation extinction with correlative operando spectroscopic techniques

Cited by 17 publications

References 63 publications

Interface Reactions Dominate Low-Temperature CO Oxidation Activity over Pt/CeO₂

Interface Reactions Dominate Low-Temperature CO Oxidation Activity over Pt/CeO₂

Stability of Pt-Adsorbed CO on Catalysts for Room Temperature-Oxidation of CO

Deposited PtGe Clusters as Active and Durable Catalysts for CO Oxidation**

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Chasing PtO species in ceria supported platinum during CO oxidation extinction with correlative operando spectroscopic techniques

Cited by 17 publications

References 63 publications

Interface Reactions Dominate Low-Temperature CO Oxidation Activity over Pt/CeO2

Interface Reactions Dominate Low-Temperature CO Oxidation Activity over Pt/CeO2

Stability of Pt-Adsorbed CO on Catalysts for Room Temperature-Oxidation of CO

Deposited PtGe Clusters as Active and Durable Catalysts for CO Oxidation**

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Product

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Interface Reactions Dominate Low-Temperature CO Oxidation Activity over Pt/CeO₂

Interface Reactions Dominate Low-Temperature CO Oxidation Activity over Pt/CeO₂