Computational study of electrochemical CO2 reduction at transition metal electrodes

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Journal Title
Journal ISSN
Volume Title
A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
Date
2015
Major/Subject
Mcode
Degree programme
Language
en
Pages
7
1865-1871
Series
PROCEDIA COMPUTER SCIENCE, Volume 51
Abstract
A detailed understanding of the mechanism of electrochemical reduction of CO2 to form hydrocarbons can help design improved catalysts for this important reaction. Density functional theory calculations were used here to model the various elementary steps in this reaction on transition metal surfaces, in particular Cu(111) and Pt(111). The minimum energy paths for sequential protonation by either Tafel or Heyrovsky mechanism were calculated using the nudged elastic band method for applied potentials comparable to those used in experimental studies, ranging from -0.7 V to -1.7 V. A detailed mechanism for CO2 reduction on Cu(111) has been identified where the highest activation energy is 0.5 eV at -1.3 V vs. RHE. On Pt(111), a different mechanism is found to be optimal but it involves a higher barrier, 0.7 eV at -1.0 V vs. RHE. Hydrogen production is then a faster reaction with activation energy of only 0.3 eV on Pt(111) at the same potential, while on Cu(111) hydrogen production has an activation energy of 0.9 eV at -1.3 V. These results are consistent with experimental findings where copper electrodes are found to lead to relatively high yield of CH4 while H2 forms almost exclusively at platinum electrodes.
Description
Keywords
Density functional theory, Electrocatalysis, Electrochemical reduction of carbon dioxide, Nudged elastic band
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Citation
Hussain , J , Skúlason , E & Jónsson , H 2015 , ' Computational study of electrochemical CO 2 reduction at transition metal electrodes ' , PROCEDIA COMPUTER SCIENCE , vol. 51 , pp. 1865-1871 . https://doi.org/10.1016/j.procs.2015.05.419