APSUSC-D-20-06693_R2-2020 08 09 accepted version.pdf (1.11 MB)
Insights into ethanol electro-oxidation over solvated Pt(1 0 0): Origin of selectivity and kinetics revealed by DFT
journal contribution
posted on 2020-08-17, 08:34 authored by Tian Sheng, Chuang Qiu, Xiao Lin, Wen-Feng LinWen-Feng Lin, Shi-Gang SunThe use of ethanol fuel in direct ethanol fuel cells has been hindered by the slow kinetics of anodic ethanol electro-oxidation reactions over Pt catalysts. We employ ab initio molecular dynamics simulations and thermodynamic integrations on the solvated Pt(1 0 0) model electrode surface with explicit water molecules, to systematically investigate the ethanol electrocatalytic oxidation mechanisms including partial oxidation to acetic acid and complete oxidation to CO2. We find that the ethanol decomposition rate does not limit the overall efficiency of the ethanol electro-oxidation reaction. However, the slow oxidation kinetics of surface intermediates to final products, due to the bonding between intermediates and the Pt surface being too strong, is the main obstacle. We suggest that weakening the surface affinity towards adsorption of the intermediates such as CO, for example by engineering the surface structures (e.g. via alloying), could improve the overall catalytic effeciency for ethanol electro-oxidation reaction.
Funding
National Natural Science Foundation of China (21903001)
Natural Science Foundation of Anhui Province (1908085QB58)
EPSRC (EP/I013229/1)
Royal Society and the Newton Fund (NAF\R1\191294)
History
School
- Aeronautical, Automotive, Chemical and Materials Engineering
Department
- Chemical Engineering
Published in
Applied Surface ScienceVolume
533Publisher
Elsevier BVVersion
- AM (Accepted Manuscript)
Rights holder
© Elsevier B.V.Publisher statement
This paper was accepted for publication in the journal Applied Surface Science and the definitive published version is available at https://doi.org/10.1016/j.apsusc.2020.147505.Acceptance date
2020-08-09Publication date
2020-08-11Copyright date
2020ISSN
0169-4332Publisher version
Language
- en
Depositor
Prof Wen Feng Lin. Deposit date: 14 August 2020Article number
147505Usage metrics
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