The promotion of CO dissociation by molybdenum oxide overlayers on rhodium

Szenti, Imre; Bugyi, László

doi:10.1016/j.susc.2016.11.002

Cited by 5 publications

(2 citation statements)

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“…To characterize the binding of CO to the promoted Rh surface, Szenti et al performed temperature-programmed CO desorption measurements on 2D Rh-MoO x films. CO desorption occurred at a higher temperature on the Rh-MoO x surfaces, leading the authors to conclude that strongly bound CO species were present at the Rh-MoO x interface . On the other hand van den Berg et al suggested that hydrogenation was the rate-limiting step on Rh-MnO-MoO 2 /SiO 2 , and the increased activity was due to greater surface coverage of hydrogen at the expense of CO .…”

Section: Introductionmentioning

confidence: 99%

“…CO desorption occurred at a higher temperature on the Rh-MoO x surfaces, leading the authors to conclude that strongly bound CO species were present at the Rh-MoO x interface. 29 On the other hand van den Berg et al suggested that hydrogenation was the rate-limiting step on Rh-MnO-MoO 2 / SiO 2 , and the increased activity was due to greater surface coverage of hydrogen at the expense of CO. 30 In their study, however, the effects of MoO 2 were not isolated from MnO, which has been shown to significantly promote oxygenate production. 31−33 Recently, Zhang et al reported an increase in methanol production over Rh nanoparticles on a MoO 3modified silica support.…”

Section: Introductionmentioning

confidence: 99%

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Understanding Structure–Property Relationships of MoO₃-Promoted Rh Catalysts for Syngas Conversion to Alcohols

et al. 2019

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Rh-based catalysts have shown promise for the direct conversion of syngas to higher oxygenates. Although improvements in higher oxygenate yield have been achieved by combining Rh with metal oxide promoters, details of the structure of the promoted catalyst and the role of the promoter in enhancing catalytic performance are not well understood. In this work, we show that MoO 3 -promoted Rh nanoparticles form a novel catalyst structure in which Mo substitutes into the Rh surface, leading to both a 66-fold increase in turnover frequency and an enhancement in oxygenate yield. By applying a combination of atomically controlled synthesis, in situ characterization, and theoretical calculations, we gain an understanding of the promoter-Rh interactions that govern catalytic performance for MoO 3 -promoted Rh. We use atomic layer deposition to modify Rh nanoparticles with monolayer-precise amounts of MoO 3 , with a high degree of control over the structure of the catalyst. Through in situ X-ray absorption spectroscopy, we find that the atomic structure of the catalytic surface under reaction conditions consists of Mo−OH species substituted into the surface of the Rh nanoparticles. Using density functional theory calculations, we identify two roles of MoO 3 : first, the presence of Mo−OH in the catalyst surface enhances CO dissociation and also stabilizes a methanol synthesis pathway not present in the unpromoted catalyst; and second, hydrogen spillover from Mo−OH sites to adsorbed species on the Rh surface enhances hydrogenation rates of reaction intermediates.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Understanding Structure–Property Relationships of MoO₃-Promoted Rh Catalysts for Syngas Conversion to Alcohols

et al. 2019

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Reaction and Diffusion Paths of Water and Hydrogen on Rh Covered Black Titania

Szenti

Bugyi

2018

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Investigation of inherent differences between oxide supports in heterogeneous catalysis in the absence of structural variations

Yang

Bent

2017

Journal of Catalysis

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The promotion of CO dissociation by molybdenum oxide overlayers on rhodium

Cited by 5 publications

References 42 publications

Understanding Structure–Property Relationships of MoO₃-Promoted Rh Catalysts for Syngas Conversion to Alcohols

Understanding Structure–Property Relationships of MoO₃-Promoted Rh Catalysts for Syngas Conversion to Alcohols

Reaction and Diffusion Paths of Water and Hydrogen on Rh Covered Black Titania

Investigation of inherent differences between oxide supports in heterogeneous catalysis in the absence of structural variations

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The promotion of CO dissociation by molybdenum oxide overlayers on rhodium

Cited by 5 publications

References 42 publications

Understanding Structure–Property Relationships of MoO3-Promoted Rh Catalysts for Syngas Conversion to Alcohols

Understanding Structure–Property Relationships of MoO3-Promoted Rh Catalysts for Syngas Conversion to Alcohols

Reaction and Diffusion Paths of Water and Hydrogen on Rh Covered Black Titania

Investigation of inherent differences between oxide supports in heterogeneous catalysis in the absence of structural variations

Contact Info

Product

Resources

About

Understanding Structure–Property Relationships of MoO₃-Promoted Rh Catalysts for Syngas Conversion to Alcohols

Understanding Structure–Property Relationships of MoO₃-Promoted Rh Catalysts for Syngas Conversion to Alcohols