Methane complete and partial oxidation catalyzed by Pt-doped CeO2

Tang, Wei; Hu, Zhenpeng; Wang, Miaojun; Stucky, Galen D.; Metiu, Horia; McFarland, Eric W.

doi:10.1016/j.jcat.2010.05.005

Cited by 208 publications

(212 citation statements)

References 47 publications

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“…18 Such a promotional effect on the creation of vacancies on the support surface adjacent to the metal single atoms was also suggested by Metiu and co-workers and has been intensively studied in various single-atombased catalysts. 43,53,54 …”

Section: 4353à55mentioning

confidence: 99%

Single-Atom Catalysts: A New Frontier in Heterogeneous Catalysis

et al. 2013

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Supported metal nanostructures are the most widely used type of heterogeneous catalyst in industrial processes. The size of metal particles is a key factor in determining the performance of such catalysts. In particular, because low-coordinated metal atoms often function as the catalytically active sites, the specific activity per metal atom usually increases with decreasing size of the metal particles. However, the surface free energy of metals increases significantly with decreasing particle size, promoting aggregation of small clusters. Using an appropriate support material that strongly interacts with the metal species prevents this aggregation, creating stable, finely dispersed metal clusters with a high catalytic activity, an approach industry has used for a long time. Nevertheless, practical supported metal catalysts are inhomogeneous and usually consist of a mixture of sizes from nanoparticles to subnanometer clusters. Such heterogeneity not only reduces the metal atom efficiency but also frequently leads to undesired side reactions. It also makes it extremely difficult, if not impossible, to uniquely identify and control the active sites of interest.The ultimate small-size limit for metal particles is the single-atom catalyst (SAC), which contains isolated metal atoms singly dispersed on supports. SACs maximize the efficiency of metal atom use, which is particularly important for supported noble metal catalysts. Moreover, with well-defined and uniform single-atom dispersion, SACs offer great potential for achieving high activity and selectivity.In this Account, we highlight recent advances in preparation, characterization, and catalytic performance of SACs, with a focus on single atoms anchored to metal oxides, metal surfaces, and graphene. We discuss experimental and theoretical studies for a variety of reactions, including oxidation, water gas shift, and hydrogenation. We describe advances in understanding the spatial arrangements and electronic properties of single atoms, as well as their interactions with the support. Single metal atoms on support surfaces provide a unique opportunity to tune active sites and optimize the activity, selectivity, and stability of heterogeneous catalysts, offering the potential for applications in a variety of industrial chemical reactions.

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Section: 4353à55mentioning

confidence: 99%

Single-Atom Catalysts: A New Frontier in Heterogeneous Catalysis

et al. 2013

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“…In ref. 45, Pt doped ceria (111) was studied with DFT + U in conjunction with experimental characterisation of this catalyst. The modelling was able to provide insights into the experimental findings.…”

Section: Q2mentioning

confidence: 99%

“…4 we show the atomic structure of the bare CeO 2 (111) and (110) surfaces. 45,46 The (111) surface has 7 coordinate surface Ce and 3 coordinate surface oxygen, with Ce-O distances slightly shortened over the bulk oxide, at 2.36 Å . In the surface layer, the (110) surface has 6 coordinate Ce and surface oxygen are 3 coordinate, with surface Ce-O distances of 2.32 Å .…”

Section: Modelling the Interaction Of Mg With The (111) And (110) Surmentioning

confidence: 99%

On the interaction of Mg with the (111) and (110) surfaces of ceria

Nolan

Lykhach

Tsud

et al. 2012

Phys. Chem. Chem. Phys.

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Access to the full text of the published version may require a subscription. Please note that, in the typefaces we use, an italic vee looks like this: n, and a Greek nu looks like this: n. RightsWe will publish articles on the web as soon as possible after receiving your corrections; no late corrections will be made.Please return your final corrections, where possible within 48 hours of receipt, by e-mail to: pccp@rsc.org.Reprints-Electronic (PDF) reprints will be provided free of charge to the corresponding author. The catalytic activity of cerium dioxide can be modified by deposition of alkaline earth oxide layers or nanoparticles or by substitutional doping of metal cations at the Ce site in ceria. In order to understand the effect of Mg oxide deposition and doping, a combination of experiment and first principles simulations is a powerful tool. In this paper, we examine the interaction of Mg with the ceria (111) surface using both angle resolved X-ray (ARXPS) and resonant (RPES) photoelectron spectroscopy measurements and density functional theory (DFT) corrected for onsite Coulomb interactions (DFT + U). With DFT + U, we also examine the interaction of Mg with the ceria (110) (111) surface. The combined results provide a basis for deeper insights into the catalytic behaviour of ceria-based mixed oxide catalysts.

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“…[13][14][15][16] Over recent years, a great deal of work has examined how the reactivity of ceria in oxidation reactions can be enhanced. [17][18][19][20][21][22][23][24][25][26][27][28][29][30][31] In CO oxidation, which occurs by the Mars van Krevelen mechanism (CO removes lattice oxygen from CeO 2 and this oxygen is returned from the atmosphere or from reduction of NO x species), the key step is the removal of oxygen from ceria. Thus, enhancing oxygen vacancy formation, by making its energy cost lower, can be of benefit by lowering the reaction temperature and improving the oxidative power of ceria.…”

Section: Introductionmentioning

confidence: 99%

Modifying ceria (111) with a TiO2 nanocluster for enhanced reactivity

Nolan

2013

The Journal of Chemical Physics

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Modification of ceria catalysts is of great interest for oxidation reactions such as oxidative dehydrogenation of alcohols. Improving the reactivity of ceria based catalysts for these reactions means that they can be run at lower temperatures and density functional theory (DFT) simulations of new structures and compositions are proving valuable in the development of these catalysts. In this paper, we have used DFT+U (DFT corrected for on-site Coulomb interactions) to examine the reactivity of a novel modification of ceria, namely, modifying with TiO2, using the example of a Ti2O4 species adsorbed on the ceria (111) surface. The oxygen vacancy formation energy in the Ti2O4–CeO2 system is significantly reduced over the bare ceria surfaces, which together with previous work on ceria-titania indicates that the presence of the interface favours oxygen vacancy formation. The energy gain upon hydrogenation of the catalyst, which is the rate determining step in oxidative dehydrogenation, further points to the improved oxidation power of this catalyst structure.

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Methane complete and partial oxidation catalyzed by Pt-doped CeO2

Cited by 208 publications

References 47 publications

Single-Atom Catalysts: A New Frontier in Heterogeneous Catalysis

Single-Atom Catalysts: A New Frontier in Heterogeneous Catalysis

On the interaction of Mg with the (111) and (110) surfaces of ceria

Modifying ceria (111) with a TiO2 nanocluster for enhanced reactivity

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