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Please use this identifier to cite or link to this item: https://dspace.lboro.ac.uk/2134/20292

Title: Insight into CO activation over Cu(100) under electrochemical conditions
Authors: Sheng, Tian
Wang, Dong
Lin, Wen-Feng
Hu, P.
Sun, Shi-Gang
Keywords: CO2
Copper electrode
Density functional theory
Ab initio molecular dynamics
Issue Date: 2016
Publisher: Crown Copyright © Published by Elsevier Ltd.
Citation: SHENG, T. ... et al., 2016. Insight into CO Activation over Cu(100) under Electrochemical Conditions. Electrochimica Acta, 190, pp.446-454.
Abstract: The reduction of CO2 on copper electrodes has attracted great attentions in the last decades, since it provides a sustainable approach for energy restore. During the CO2 reduction process, the electron transfer to COads is experimentally suggested to be the crucial step. In this work, we examine two possible pathways in CO activation, i.e. to generate COHads and CHOads, respectively, by performing the state-of-the-art constrained ab initio molecular dynamics simulations on the charged Cu(100) electrode under aqueous conditions, which is close to the realistic electrochemical condition. The free energy profile in the formation of COHads via the coupled proton and electron transfer is plotted. Furthermore, by Bader charge analyses, a linear relationship between C-O bond distance and the negative charge in CO fragment is unveiled. The formation of CHOads is identified to be a surface catalytic reaction, which requires the adsorption of H atom on the surface first. By comparing these two pathways, we demonstrate that kinetically the formation of COHads is more favored than that of CHOads, while CHOads is thermodynamically more stable. This work reveals that CO activation via COHads intermediate is an important pathway in electrocatalysis, which could provide some insights into CO2 electroreduction over Cu electrodes.
Description: Closed access until 7 Jan 2017.
Sponsor: Financial supports from the NSFC (21361140374, 21321062, 21333003 and 21573183) are acknowledged.
Version: Accepted for publication
DOI: 10.1016/j.electacta.2016.01.037
URI: https://dspace.lboro.ac.uk/2134/20292
Publisher Link: http://dx.doi.org/10.1016/j.electacta.2016.01.037
ISSN: 0013-4686
Appears in Collections:Closed Access (Chemical Engineering)

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