Structure Sensitivity of Oxidative Dehydrogenation of Cyclohexane over FeOx and Au/Fe3O4 Nanocrystals

Goergen, Simone; Yin, Chunrong; Yang, Ming; Lee, B.; Lee, S.; Wang, C.; Wu, Peng; Boucher, Matthew B.; Kwon, Gihan; Seifert, Söenke; Winans, Randall E.; Vajda, Štefan; Flytzani‐Stephanopoulos, Maria

doi:10.1021/cs3007582

Cited by 29 publications

(22 citation statements)

References 51 publications

(90 reference statements)

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“…The oxidized clusters may consist of smaller subunits detected by GISAXS. 41 Indeed, a grainy structure of the shells can be seen in TEM images (see below in Figure 6). Another explanation may be a coreÀshell structure with sizes corresponding to the outer and the inner diameter of the particles, respectively.…”

Section: Articlementioning

confidence: 96%

Pronounced Size Dependence in Structure and Morphology of Gas-Phase Produced, Partially Oxidized Cobalt Nanoparticles under Catalytic Reaction Conditions

Bartling

Yin²,

Barke

et al. 2015

ACS Nano

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It is generally accepted that optimal particle sizes are key for efficient nanocatalysis. Much less attention is paid to the role of morphology and atomic arrangement during catalytic reactions. Here, we unravel the structural, stoichiometric, and morphological evolution of gas-phase produced and partially oxidized cobalt nanoparticles in a broad size range. Particles with diameters between 1.4 and 22 nm generated in cluster sources are size selected and deposited on amorphous alumina (Al2O3) and ultrananocrystalline diamond (UNCD) films. A combination of different techniques is employed to monitor particle properties at the stages of production, exposure to ambient conditions, and catalytic reaction, in this case, the oxidative dehydrogenation of cyclohexane at elevated temperatures. A pronounced size dependence is found, naturally classifying the particles into three size regimes. While small and intermediate clusters essentially retain their compact morphology, large particles transform into hollow spheres due to the nanoscale Kirkendall effect. Depending on the substrate, an isotropic (Al2O3) or anisotropic (UNCD) Kirkendall effect is observed. The latter results in dramatic lateral size changes. Our results shed light on the interplay between chemical reactions and the catalyst's structure and provide an approach to tailor the cobalt oxide phase composition required for specific catalytic schemes.

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Section: Articlementioning

confidence: 96%

Pronounced Size Dependence in Structure and Morphology of Gas-Phase Produced, Partially Oxidized Cobalt Nanoparticles under Catalytic Reaction Conditions

Bartling

Yin²,

Barke

et al. 2015

ACS Nano

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“…This process rendered am ixture of benzene and cyclohexene, with the highest benzene selectivity being 85 %a t350 8C. [100]…”

Section: Gold Impregnationmentioning

confidence: 98%

ChemInform Abstract: Magnetite and Metal‐Impregnated Magnetite Catalysts in Organic Synthesis: A Very Old Concept with New Promising Perspectives

2016

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“…Goergen et al . investigated the oxidative dehydrogenation of cyclohexane over the FeO x octahedrons and nanocubes comprising the (1 1 1) and (1 0 0) facet, respectively, and the Au/(1 1 1) and Au/(1 0 0) interfaces.…”

Section: Metal Oxide Substrates Metal/oxide Interfaces and Their Camentioning

confidence: 99%

Surface/Interfacial Catalysis of (Metal)/Oxide System: Structure and Performance Control

2018

ChemCatChem

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Surface/interfacial catalysis on a series of oxide substrates and metal/oxide interfaces has been reviewed. Special attention has been paid to those systems in which the oxide substrates are structurally defined with certain exposed facets, and the metal assembling is well controlled with desired particle size and narrow particle size distribution. The distinct catalytic behaviors over the selected systems have been discussed in line with their specific surface/interfacial structure features as well as other surface properties. The tactics and cations how to build up the novel metal/oxide interfacial structures are provided, and the guideline for extended reaction exploration is also suggested. Success in structure and performance control on these important systems is highly valuable for designing more selective and efficient catalyst in practical applications.

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Structure Sensitivity of Oxidative Dehydrogenation of Cyclohexane over FeO_x and Au/Fe₃O₄ Nanocrystals

Cited by 29 publications

References 51 publications

Pronounced Size Dependence in Structure and Morphology of Gas-Phase Produced, Partially Oxidized Cobalt Nanoparticles under Catalytic Reaction Conditions

Pronounced Size Dependence in Structure and Morphology of Gas-Phase Produced, Partially Oxidized Cobalt Nanoparticles under Catalytic Reaction Conditions

ChemInform Abstract: Magnetite and Metal‐Impregnated Magnetite Catalysts in Organic Synthesis: A Very Old Concept with New Promising Perspectives

Surface/Interfacial Catalysis of (Metal)/Oxide System: Structure and Performance Control

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