Calculations of Product Selectivity in Electrochemical CO2 Reduction

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A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
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Date

2018-06

Department

Department of Applied Physics

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Language

en

Pages

19
5240-5249

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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.

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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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DOI

10.1021/acscatal.7b03308

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

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https://urn.fi/URN:NBN:fi:aalto-201809044940

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[article-cris] Perustieteiden korkeakoulu / SCI