A kinetic Monte Carlo/UBI-QEP model of O2 adsorption on fcc (111) metal surfaces

Abramova, L. A.; Zeigarnik, Andrew V.; Baranov, S. P.; Shustorovich, Evgeny

doi:10.1016/j.susc.2004.06.205

Cited by 11 publications

(5 citation statements)

References 24 publications

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“…This tailing indicates that O 2 interaction includes various reversible surface steps. According to theoretical and experimental studies performed on different Rh − and Pt − crystal surfaces, O 2 adsorbs reversibly and dissociatively via a molecularly adsorbed oxygen species.…”

Section: Resultsmentioning

confidence: 99%

Partial Oxidation of Methane to Syngas Over γ-Al₂O₃-Supported Rh Nanoparticles: Kinetic and Mechanistic Origins of Size Effect on Selectivity and Activity

2014

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A series of supported Rh/γ-Al 2 O 3 catalysts with an overall metal loading of 0.005 wt % was synthesized by impregnation of γ-Al 2 O 3 with a toluene solution containing colloidally prepared well-defined (1.1, 2.5, 2.9, 3.7, and 5.5 nm) Rh nanoparticles (NP). The size of NP was not found to change after their deposition on γ-Al 2 O 3 and even after performing partial oxidation of methane (POM) to synthesis gas at 1073 K for 160 h on stream. Apparent CO formation turnover rates and CO selectivity strongly decrease with an increase in this size. Contrarily, the overall scheme of POM is size-independent, i.e. CO and H 2 are mainly formed through reforming reactions of CH 4 with CO 2 and H 2 O at least under conditions of complete oxygen conversion. The size effect on the activity and selectivity was related to the kinetics of interaction of CH 4 , O 2 , and CO 2 with Rh/γ-Al 2 O 3 as concluded from our microkinetic analysis of corresponding transient experiments in the temporal analysis of products reactor. The rate constants of CH 4 , O 2 , and CO 2 activation decrease with an increase in the size of supported Rh NP thus influencing both primary (methane combustion) and secondary (reforming of methane) pathways within the course of POM.

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Section: Resultsmentioning

confidence: 99%

Partial Oxidation of Methane to Syngas Over γ-Al₂O₃-Supported Rh Nanoparticles: Kinetic and Mechanistic Origins of Size Effect on Selectivity and Activity

2014

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“…The UBI-QEP approach is relatively simple, yet it offers a reasonable way of estimating the activation barriers. Therefore, different groups have applied this method to the activation barrier of the O 2 dissociation process on Ni(111), 18) the CHN 2 dissociation process on Fe, Ni, Pd, and Cu, 19) the CO and H 2 O combination process on Cu, 20) and so on. In the present study, we apply the UBI-QEP technique to estimate the activation barrier for the dissociation of H 2 O.…”

Section: Methodsmentioning

confidence: 99%

CO Oxidation Process on Pt-M(111) Alloys (M=Ru, Sn): An <I>ab initio</I> Study

Oka

Mizuseki

2007

Mater. Trans.

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Direct Methanol Fuel Cell (DMFC) have attracted attention in recent years because they are very energy-efficient. However, there is a serious problem in that Pt, which is the usual anode electrocatalyst, is poisoned by CO. Therefore, it is very important to develop new materials for use as electrocatalysts that exhibit good tolerance to CO. The aim of this study is to examine the mechanism of H 2 O dissociation and of the CO+OH combination reactions in the CO oxidation process by calculating the adsorption energies and the activation barriers. In the case of PtRu alloys, the activation barrier for the H 2 O dissociation reaction is almost the same as it is for pure Pt. The activation barrier for the CO+OH combination reaction on the Pt-Ru alloy is larger than that on pure Pt. Nevertheless, the adsorption energy of H 2 O is larger than that on pure Pt. On the other hand, the activation barrier and adsorption energies of H 2 O on the Pt-Sn alloy are very close to the corresponding values on pure Pt. Moreover, the activation barrier for the CO+OH combination reaction on the Pt-Sn alloy is lower than that on pure Pt.

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“…Zhdanov proposed that the reactant coverage is not first order in the O 2 reaction. Abramova et al [97] studied the O 2 adsorption on fcc(111) metals by kMC. By taken into account seven elementary steps, they report the total oxygen coverage profile in terms of σ (charge density) and sticking probability reporting a strong coverage dependency in the pre-exponential factor.…”

Section: Another Common Kmc Algorithm Used Is the Variablementioning

confidence: 99%

Performance and degradation of Proton Exchange Membrane Fuel Cells: State of the art in modeling from atomistic to system scale

Jahnke

Futter

Latz

et al. 2016

Journal of Power Sources

207

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Proton Exchange Membrane Fuel Cells (PEMFC) are energy efficient and environmentally friendly alternatives to conventional energy conversion systems in many yet emerging applications. In order to enable prediction of their performance and durability, it is crucial to gain a deeper understanding of the relevant operation phenomena, e.g., electrochemistry, transport phenomena, thermodynamics as well as the mechanisms leading to the degradation of cell components. Achieving the goal of providing predictive tools to model PEMFC performance, durability and degradation is a challenging task requiring the development of detailed and realistic models reaching from the atomic/molecular scale over the meso scale of structures and materials up to components, stack and system level. In addition an appropriate way of coupling the different scales is required. This review provides a comprehensive overview of the state of the art in modeling of PEMFC, covering all relevant scales from atomistic up to system level as well as the coupling between these scales. Furthermore, it focuses on the modeling of PEMFC degradation mechanisms and on the coupling between performance and degradation models.

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A kinetic Monte Carlo/UBI-QEP model of O2 adsorption on fcc (111) metal surfaces

Cited by 11 publications

References 24 publications

Partial Oxidation of Methane to Syngas Over γ-Al₂O₃-Supported Rh Nanoparticles: Kinetic and Mechanistic Origins of Size Effect on Selectivity and Activity

Partial Oxidation of Methane to Syngas Over γ-Al₂O₃-Supported Rh Nanoparticles: Kinetic and Mechanistic Origins of Size Effect on Selectivity and Activity

CO Oxidation Process on Pt-M(111) Alloys (M=Ru, Sn): An <I>ab initio</I> Study

Performance and degradation of Proton Exchange Membrane Fuel Cells: State of the art in modeling from atomistic to system scale

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A kinetic Monte Carlo/UBI-QEP model of O2 adsorption on fcc (111) metal surfaces

Cited by 11 publications

References 24 publications

Partial Oxidation of Methane to Syngas Over γ-Al2O3-Supported Rh Nanoparticles: Kinetic and Mechanistic Origins of Size Effect on Selectivity and Activity

Partial Oxidation of Methane to Syngas Over γ-Al2O3-Supported Rh Nanoparticles: Kinetic and Mechanistic Origins of Size Effect on Selectivity and Activity

CO Oxidation Process on Pt-M(111) Alloys (M=Ru, Sn): An <I>ab initio</I> Study

Performance and degradation of Proton Exchange Membrane Fuel Cells: State of the art in modeling from atomistic to system scale

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Product

Resources

About

Partial Oxidation of Methane to Syngas Over γ-Al₂O₃-Supported Rh Nanoparticles: Kinetic and Mechanistic Origins of Size Effect on Selectivity and Activity

Partial Oxidation of Methane to Syngas Over γ-Al₂O₃-Supported Rh Nanoparticles: Kinetic and Mechanistic Origins of Size Effect on Selectivity and Activity