APSUSC-D-20-06693_R2-2020 08 09 accepted version.pdf (1.11 MB)
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Insights into ethanol electro-oxidation over solvated Pt(1 0 0): Origin of selectivity and kinetics revealed by DFT

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journal contribution
posted on 17.08.2020, 08:34 by Tian Sheng, Chuang Qiu, Xiao Lin, Wen-Feng LinWen-Feng Lin, Shi-Gang Sun
The 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 Science

Volume

533

Publisher

Elsevier BV

Version

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

09/08/2020

Publication date

2020-08-11

Copyright date

2020

ISSN

0169-4332

Language

en

Depositor

Prof Wen Feng Lin. Deposit date: 14 August 2020

Article number

147505