CO2 activation at Au(110)–water interfaces: An ab initio molecular dynamics study

Xueping Qin, Tejs Vegge, Heine Anton Hansen*

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

The electrochemical reduction of CO2 into valuable chemicals under mild conditions has become a promising technology for energy storage and conversion in the past few years, receiving much attention from theoretical researchers investigating the reaction mechanisms. However, most of the previous simulations are related to the key intermediates of *COOH and *CO using the computational hydrogen electrode approach under vacuum conditions, and the details of the CO2 activation are usually ignored due to the model simplicity. Here, we study the CO2 activation at the Au–water interfaces by considering the dynamics of an explicit water solvent, where both regular ab initio molecular dynamics and constrained ab initio molecular dynamics simulations are carried out to explore the CO2 adsorption/desorption reactions from the atomic level. By introducing K+ cations into Au(110)–water interfacial models, an electrochemical environment under reducing potentials is constructed, where the reaction free energy (0.26 eV) and activation energy (0.61 eV) are obtained for CO2 adsorption based on the thermodynamic integration. Moreover, the Bader charge analysis demonstrates that CO2 adsorption is activated by the first-electron transfer, forming the adsorbed CO2− anion initiating the overall catalytic reaction.
Original languageEnglish
Article number134703
JournalJournal of Chemical Physics
Volume155
Issue number13
Number of pages8
ISSN0021-9606
DOIs
Publication statusPublished - 2021

Fingerprint

Dive into the research topics of 'CO<sub>2</sub> activation at Au(110)–water interfaces: An ab initio molecular dynamics study'. Together they form a unique fingerprint.

Cite this