Temperature dependence of CO oxidation on Rh(111) by adsorbed oxygen

Turano, Marie E.; Farber, Rachael G.; Hildebrandt, George; Killelea, Daniel R.

doi:10.1016/j.susc.2020.121573

Cited by 6 publications

(4 citation statements)

References 39 publications

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“…Therefore, extensive studies [4][5][6] have been conducted on the detailed process of CO oxidation to understand the relationship between CO oxidation activity and the morphology, the electronic properties of the catalyst, so as to design more efficient catalysts. Noble metals like Rh [7][8][9] and Pd [10][11][12] show excellent catalytic activities on converting CO to CO 2 , but the high prices and limited reserves, as well as the demand of high temperature for ideal efficiency impede their large-scale industrialization.…”

Section: Introductionmentioning

confidence: 99%

A theoretical study of the improved CO oxidation on WC supported Au monolayer by Cu doping

Chang¹,

Zhang²,

Yang³

2023

Phys. Scr.

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Metal monolayer supported on tungsten carbides have received considerable attention in the field of catalysis, while the adsorption properties of reactants need to be optimized to improve the catalytic activity further. Alloy monolayers on tungsten carbides can deliver different geometric and electronic characters from pure metal layers, owing to the change in local environments. Herein, using the first-principles calculations, the CO oxidation processes on the supported CuAu alloy monolayer on tungsten carbide are systematically investigated and compared with that on pure metal monolayers. It is found that introducing Cu dopant in Au monolayer will elevate the d-band center of the formed alloy monolayer and thus enhancing the adsorption of reactants around the Cu atom, which is caused by the charge redistribution. Especially, the unbalanced interaction strength between Cu-O and Au-O promotes the rotation and migration of oxygen atom to interact with the C atom of CO, which lowers the energy barriers for the formation and dissociation of OOCO intermediate. The oxidation of CO by an atomic O with the largest energy barrier of 0.27 eV along the Langmuir-Hinshelwood pathway is identified as the rate determining step, which is superior or comparable to the reported CO oxidation catalysts. The significance of alloy monolayer on tungsten carbides are further highlighted by comparing the adsorption energy and reaction barrier of rate-limiting step on the pure metal monolayers. This work is insightful for the rational design of highly efficient catalysts based on alloy systems.

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Section: Introductionmentioning

confidence: 99%

A theoretical study of the improved CO oxidation on WC supported Au monolayer by Cu doping

Chang¹,

Zhang²,

Yang³

2023

Phys. Scr.

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“…Dosing Rh(111) with O2 at room temperature, oxygen readily dissociates and saturates at an oxygen surface-coverage (O) of 0.5 monolayers (ML, 1 ML = 1.6 × 10 15 atoms cm -2 ) [16] in a (2 × 1)-O adlayer. [17] At these modest temperatures and low pressures, the rate of sub-surface oxygen formation is low. In contrast, when exposing Rh(111) to AO at elevated temperatures, sub-surface oxygen as well as single-layer RhO2 surface oxide domains are created in addition to the (2 × 1)-O adlayer.…”

Section: A Introductionmentioning

confidence: 99%

Velocity map images of desorbing oxygen from sub-surface states of Rh(111)

Dorst

Güthoff

Schauermann

et al. 2022

Phys. Chem. Chem. Phys.

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“…For example, a trilayer surface oxide forms on Rh under conditions similar to those for Ir and Pd, and the oxide trilayer has been hypothesized to form on Ru, although this has yet to be experimentally observed. − Additionally, O 2 readily dissociates on these surfaces, forming adlayers of known structure and composition . While O 2 dissociates into O ad on Rh(111) and saturates at an oxygen coverage (θ O ) of 0.5 monolayers (ML, 1.6 × 10 15 O cm –2 ) in a (2 × 1)-O adlayer, the rate of O sub formation from O ad is slow . Furthermore, high pressures of molecular oxygen are necessary to form high oxygen phases and O sub . , In order to generate higher amounts of O sub , gas-phase atomic oxygen (AO) is used because it is much more likely to be absorbed.…”

mentioning

confidence: 99%

“…23−25 Additionally, O 2 readily dissociates on these surfaces, forming adlayers of known structure and composition. 6 While O 2 dissociates into O ad on Rh(111) and saturates at an oxygen coverage (θ O ) of 0.5 monolayers (ML, 1.6 × 10 15 O cm −2 ) 26 in a (2 × 1)-O adlayer, the rate of O sub formation from O ad is slow. 17 Furthermore, high pressures of molecular oxygen are necessary to form high oxygen phases and O sub .…”

mentioning

confidence: 99%

Emergence of Subsurface Oxygen on Rh(111)

Turano

Jamka

Gillum

et al. 2021

J. Phys. Chem. Lett.

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Oxygen atoms on transition metal surfaces are highly mobile under the demanding pressures and temperatures typically employed for heterogeneously catalyzed oxidation reactions. This mobility allows for rapid surface diffusion of oxygen atoms, as well as absorption into the subsurface and reemergence to the surface, resulting in variable reactivity. Subsurface oxygen atoms play a unique role in the chemistry of oxidized metal catalysts, yet little is known about how subsurface oxygen is formed or returns to the surface. Furthermore, if oxygen diffusion between the surface and subsurface is mediated by defects, there will be localized changes in the surface chemistry due to the elevated oxygen concentration near the emergence sites. We observed that oxygen atoms emerge preferentially along the boundary between surface phases and that subsurface oxygen is depleted before the surface oxide decomposes.

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Temperature dependence of CO oxidation on Rh(111) by adsorbed oxygen

Cited by 6 publications

References 39 publications

A theoretical study of the improved CO oxidation on WC supported Au monolayer by Cu doping

A theoretical study of the improved CO oxidation on WC supported Au monolayer by Cu doping

Velocity map images of desorbing oxygen from sub-surface states of Rh(111)

Emergence of Subsurface Oxygen on Rh(111)

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