What It Takes for Imidazolium Cations to Promote Electrochemical Reduction of CO2

Sobhan Neyrizi, Joep Kiewiet, Mark A. Hempenius, Guido Mul*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

25 Citations (Scopus)
161 Downloads (Pure)

Abstract

Imidazolium cations enhance the performance of several electrodes in converting CO2 to CO in non-aqueous media. In this publication, we elucidate the origin of the function of imidazolium cations when exposed to Au electrodes in anhydrous acetonitrile in CO2 atmosphere. We demonstrate that imidazolium cations lead to unprecedentedly low overpotentials for CO2 reduction to CO on Au, with ∼100% Faradaic efficiency. By modification of the N1 and N3 functionality of the imidazolium cation, we show a direct correlation between the performance in CO2 reduction and the C2-H acidity of the cation. Based on NMR analyses, DFT calculations, and isotopic labeling, showing an inverse kinetic isotope effect, we demonstrate that the mechanism involves a concerted proton-electron transfer to the electrode-adsorbed CO2 intermediate. The demonstrated mechanism provides guidelines for improvement in the energy efficiency of non-aqueous electrochemical CO2 reduction, by a tailored design of electrolyte cations.

Original languageEnglish
Pages (from-to)3439-3446
Number of pages8
JournalACS Energy Letters
Volume7
Issue number10
DOIs
Publication statusPublished - 14 Oct 2022

Keywords

  • UT-Hybrid-D

Fingerprint

Dive into the research topics of 'What It Takes for Imidazolium Cations to Promote Electrochemical Reduction of CO2'. Together they form a unique fingerprint.

Cite this