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CO methanation on ruthenium flat and stepped surfaces: Key role of H-transfers and entropy revealed by ab initio molecular dynamics


Foppa, Lucas; Iannuzzi, Marcella; Copéret, Christophe; Comas-Vives, Aleix (2019). CO methanation on ruthenium flat and stepped surfaces: Key role of H-transfers and entropy revealed by ab initio molecular dynamics. Journal of Catalysis, 371:270-275.

Abstract

The methanation reaction converting CO into CH4 at ca. 400 °C is proposed to take place on uncoordinated surface sites (e.g. step-edges) of Ru catalysts because of the higher measured reactivity of stepped vs. flat single crystal metal surfaces. However, the reaction mechanisms occurring at step-edges remain unclear due to the limitations in modelling high temperatures processes by the common evaluation of potential energy surfaces by density functional theory calculations. Here, we show using ab initio molecular dynamics simulations on CO-covered Ru flat and stepped surfaces models at 400 °C that hydrogen-transfers favoured at elevated temperatures are crucial for both CO activation and CHx (x = 1, 2, 3) hydrogenation steps of the methanation reaction, especially at step-edges.

Abstract

The methanation reaction converting CO into CH4 at ca. 400 °C is proposed to take place on uncoordinated surface sites (e.g. step-edges) of Ru catalysts because of the higher measured reactivity of stepped vs. flat single crystal metal surfaces. However, the reaction mechanisms occurring at step-edges remain unclear due to the limitations in modelling high temperatures processes by the common evaluation of potential energy surfaces by density functional theory calculations. Here, we show using ab initio molecular dynamics simulations on CO-covered Ru flat and stepped surfaces models at 400 °C that hydrogen-transfers favoured at elevated temperatures are crucial for both CO activation and CHx (x = 1, 2, 3) hydrogenation steps of the methanation reaction, especially at step-edges.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:570 Life sciences; biology
610 Medicine & health
Uncontrolled Keywords:Physical and Theoretical Chemistry, Catalysis
Language:English
Date:1 March 2019
Deposited On:20 Mar 2019 15:28
Last Modified:20 Mar 2019 15:28
Publisher:Elsevier
ISSN:0021-9517
OA Status:Closed
Publisher DOI:https://doi.org/10.1016/j.jcat.2019.02.008

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