Methanol decomposition on low index and stepped CeO 2 surfaces from GGA+ U

Reimers, W.; Branda, María Marta

doi:10.1016/j.apsusc.2016.10.154

Cited by 8 publications

(2 citation statements)

References 40 publications

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“…Reimers and Branda 22 found that the dehydrogenation of methoxy groups to formaldehyde on ceria is the ratedetermining step, and the formation of formyl species is facilitated only on the stepped surface. Mullins et al 23 found that surface oxygen vacancies on ceria are not required for the primary interaction with methanol.…”

Section: ■ Introductionmentioning

confidence: 99%

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Nickel-Decorated Mesoporous Iron–Cerium Mixed Oxides: Microstructure and Catalytic Activity in Methanol Decomposition

Tsoncheva

Rosmini

Mihaylov

et al. 2021

ACS Appl. Mater. Interfaces

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Nickel-decorated mesoporous cerium−iron oxide composites were synthesized by a combination of incipient wetness impregnation and templateassisted hydrothermal techniques. The effects of the Fe/Ce ratio and the calcination temperature of cerium−iron oxides on the phase composition, texture, structure, and redox properties of the composites were studied by a combination of N 2 physisorption, XRD, high-resolution transmission electron microscopy, SEM, Mossbauer, Raman, XPS, ultraviolet−visible and FTIR spectroscopies, H 2temperature-programmed reduction, and total oxidation of ethyl acetate as a catalytic test. The combined physicochemical characterization and in situ FTIR investigation of methanol decomposition was used for a proper understanding of the microstructure of the Ni/FeCe oxide composites and the mechanism of the reaction occurring on them. The complex role of the FeCe support in the stabilization of highly dispersed Ni particles, the generation of surface intermediates, and the impact of the support phase transformation under the reaction medium are discussed.

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Section: ■ Introductionmentioning

confidence: 99%

“…Typically, the Ni/Ce ratio (Table 4) was higher than the expected one, which did not confirm the reported 22 encapsulation of Ni species in ceria. The surface concentration of Ni ions was close to the theoretical one only for the supports with a relatively low Fe/Ce ratio (Table 4).…”

Section: ■ Introductionmentioning

confidence: 99%

Nickel-Decorated Mesoporous Iron–Cerium Mixed Oxides: Microstructure and Catalytic Activity in Methanol Decomposition

Tsoncheva

Rosmini

Mihaylov

et al. 2021

ACS Appl. Mater. Interfaces

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Catalytic Activities of Low‐Coordinated Ce for Methane Conversion

Zhou

Gong

2021

ChemCatChem

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In heterogeneous catalysis, the catalytic activity of an active center strongly correlates with its coordination number. In this work, density functional theory calculations corrected by on‐site Coulomb interactions were conducted to investigate the catalytic performances of the CeO4‐terminated reconstructed CeO2(100) (CeO4‐t) and the Ca‐doped CeO4‐t surfaces. The undoped CeO4‐t surface contains single 4‐fold coordinated Ce (Ce4c) sites on its top surface layer, and the Ca‐doped CeO4‐t surface can expose even lower‐coordinated 3‐fold Ce (Ce3c) sites. We found that the empty 4f states of the single Ce3c sites on the Ca‐doped CeO4‐t surface have much lower energies than that of the single Ce4c sites on the undoped CeO4‐t surface, which can effectively boost the reduction of Ce4+ to Ce3+. We further studied the selective oxidation of CH4 to CH3OH on the two surfaces and found that the isolated nature combined with the strong electron‐reservoir character of the single Ce3c site makes it highly desirable for the selective activation of the first C−H bond of CH4, while the subsequent C−H bond cleavage step is less affected by such low‐coordinated Ce and the CH3OH formation becomes more facile on the Ca‐doped CeO4‐t surface, giving rise to the high activity and selectivity of the Ca‐doped CeO4‐t surface toward the selective oxidation of CH4 to CH3OH.

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