Corrigendum to “Methane oxidation on Pd–Ceria: A DFT study of the mechanism over Pd Ce1−O2, Pd, and PdO” [J. Catal. 2781 (2011) 16–25]

Mayernick, Adam D.; Janik, Michael J.

doi:10.1016/j.jcat.2011.12.001

Cited by 26 publications

(41 citation statements)

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“…In the electronic aspect, it was shown by charge density analysis that the electrons transferred from the Pd phase form Ce 3+ , and the electrons subsequently transfer to the adsorbed O 2 , leading to active oxygen species. Additionally, it was demonstrated that the charge transfer predominantly takes place in the bottom layer of Pd in direct contact with the support, indicating that charge transfer occurs at the interface between metal phase and oxide support …”

Section: Strategy To Improve Co Oxidation By Controlling the Interactmentioning

confidence: 99%

Design of Ceria Catalysts for Low‐Temperature CO Oxidation

et al. 2019

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A catalyst active to carbon monoxide (CO) oxidation at low temperature is essential for environmental conservation, saving fuel and improvement of the quality of human life. Rational design of CO oxidation catalyst on the basis of comprehensive understanding of physicochemical properties of catalytic materials, rather than simply searching for the catalyst based on trial‐and‐error, is a promising approach to meet the increasingly stringent regulations. This review covers metal‐doped and ‐loaded system based on CeO2 catalysts as strategies to significantly improve CO oxidation activity at low temperature. When incorporated into CeO2 lattice, active metals significantly lower the oxygen vacancy formation energy (Evf) of the catalyst surface, resulting in high catalytic activities at low temperature. When the active metals are loaded on the CeO2 surface, many active sites could be acquired by increasing the dispersion, and the catalytic activity can be dramatically improved by newly introducing the interfacial sites between the metals and the CeO2 support. Doping the support could further improve this loaded system in terms of specific surface area, oxygen vacancy formation, and spillover effects. In this review, based on this knowledge, we propose a rational design approach to a robust low‐temperature CO oxidation catalysts. The desirable CO oxidation catalysts identified from the interplay between theoretical and experimental approaches would ultimately improve the quality of human life, and create potential economic benefits by alleviating air pollution.

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Section: Strategy To Improve Co Oxidation By Controlling the Interactmentioning

confidence: 99%

Design of Ceria Catalysts for Low‐Temperature CO Oxidation

et al. 2019

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“…Radical intermediates on oxide surfaces are ubiquitous in catalytic oxidation of alkanes and alkenes [55][56][57][58][59] ; yet this chemistry frequently involves C-H scission barriers >1 eV and thus requires high temperatures (>300 o C) in order to achieve appreciable reaction rates. The low barrier in the C-OH scission signifies that radicals can also mediate heterogeneous catalytic processes involving reduction, potentially at much lower temperatures (<200 o C).…”

Section: C-o Bond Hydrogenolysis Active Sitementioning

confidence: 99%

Conjugation-Driven “Reverse Mars–van Krevelen”-Type Radical Mechanism for Low-Temperature C–O Bond Activation

Mironenko

Vlachos

2016

J. Am. Chem. Soc.

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C-O bond activation on monofunctional catalysts (metals, carbides, and oxides) is challenging due to activity constraints imposed by energy scaling relationships. Yet, contrary to predictions, recently discovered multifunctional metal/metal oxide catalysts (e.g., Rh/ReOx, Rh/MoOx, Ir/VOx) demonstrate unusually high C-O scission activity at moderate temperatures. Herein, we use extensive density functional theory calculations, first-principles microkinetic modeling, and electronic structure analysis to elucidate the metal/metal oxide synergy in the Ru/RuO2 catalyst, which enables up to 76% yield of the C-O scission product (2-methyl furan) in catalytic transfer hydrogenolysis of furfural at low temperatures. Our key mechanistic finding is a facile radical-mediated C-O bond activation on RuO2 oxygen vacancies, which directly leads to a weakly bound final product. This is the first time the radical reduction mechanism is reported in heterogeneous catalysis at temperatures <200 °C. We attribute the unique catalytic properties to the formation of a conjugation-stabilized furfuryl radical upon C-O bond scission, the strong hydroxyl affinity of oxygen vacancies due to the metallic character of RuO2, and the acid-base heterogeneity of the oxide surface. The conjugation-driven radical-assisted C-O bond scission applies to any catalytic surface that preserves the π-electron system of the reactant and leads to C-O selectivity enhancement, with notable examples including Cu, H-covered Pd, self-assembled monolayers on Pd, and oxygen-covered Mo2C. Furthermore, we reveal the cooperativity of active sites in multifunctional catalysts. The mechanism is fully consistent with kinetic studies and isotopic labeling experiments, and the insights gained might prove useful more broadly in overcoming activity constraints induced by energy scaling relationships.

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“…The promotion is likely linked to the change of palladium species [13,14], indicating the important role of Ce x Zr 1Àx O 2 in methanol oxidation. Especially, a huge improvement has been observed over Ce 0.3 Zr 0.7 O 2 -containing catalyst.…”

Section: Catalytic Methanol Oxidationmentioning

confidence: 99%