Calculations of Product Selectivity in Electrochemical CO2 Reduction

Loading...
Thumbnail Image
Journal Title
Journal ISSN
Volume Title
A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
This publication is imported from Aalto University research portal.
View publication in the Research portal
View/Open full text file from the Research portal
Date
2018-06
Major/Subject
Mcode
Degree programme
Language
en
Pages
19
5240-5249
Series
ACS CATALYSIS, Volume 8, issue 6
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.
Description
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
Other note
Citation
Hussain, J, Jonsson, H & Skulason, E 2018, ' Calculations of Product Selectivity in Electrochemical CO2 Reduction ', ACS Catalysis, vol. 8, no. 6, pp. 5240-5249 . https://doi.org/10.1021/acscatal.7b03308