Calculations of Product Selectivity in Electrochemical CO2 Reduction

Javed Hussain, Hannes Jonsson, Egill Skulason*

*Corresponding author for this work

Research output: Contribution to journalArticleScientificpeer-review

49 Citations (Scopus)
262 Downloads (Pure)

Abstract

CO2 can be reduced electrochemically to form valuable chemicals such as hydrocarbons and alcohols using copper electrodes, whereas the other metal electrodes tested so far mainly form CO or formate, or only the side product, H-2. Accurate modeling of electrochemical reaction rates including the complex environment of an electrical double layer in the presence of an applied electrical potential is challenging. We show here that calculated rates, obtained using a combination of density functional and rate theory, are in close agreement with available experimental data on the formation of the various products on several metal electrodes and over a range in applied potential, thus demonstrating the applicability of the theoretical methodology. The results explain why copper electrodes give a significant yield of hydrocarbons and alcohols, and why methane, ethylene, and ethanol are formed in electroreduction rather than methanol, which is the main product when H-2 gas reacts with CO2 on copper catalyst. The insight obtained from the calculations is used to develop criteria for identifying new and improved catalysts for electrochemical CO2 reduction.

Original languageEnglish
Pages (from-to)5240-5249
Number of pages19
JournalACS Catalysis
Volume8
Issue number6
DOIs
Publication statusPublished - Jun 2018
MoE publication typeA1 Journal article-refereed

Keywords

  • reaction mechanism
  • electrochemical CO2 reduction reaction
  • electrocatalysis
  • density functional theory calculations
  • selectivity
  • DENSITY-FUNCTIONAL THEORY
  • TRANSITION-METAL ELECTRODES
  • HYDROGEN-EVOLUTION REACTION
  • INITIO MOLECULAR-DYNAMICS
  • SOLID-LIQUID INTERFACE
  • CARBON-DIOXIDE
  • COPPER ELECTRODES
  • AB-INITIO
  • ELECTROCATALYTIC CONVERSION
  • OXYGEN REDUCTION

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