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What It Takes for Imidazolium Cations to Promote Electrochemical Reduction of CO2.
| Content Provider | Europe PMC |
|---|---|
| Author | Neyrizi, Sobhan Kiewiet, Joep Hempenius, Mark A. Mul, Guido |
| Copyright Year | 2022 |
| Abstract | Imidazolium cations enhance the performance of severalelectrodesin converting CO2 to CO in non-aqueous media. In this publication,we elucidate the origin of the function of imidazolium cations whenexposed to Au electrodes in anhydrous acetonitrile in CO2 atmosphere. We demonstrate that imidazolium cations lead to unprecedentedlylow 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 showa direct correlation between the performance in CO2 reductionand the C2–H acidity of the cation. Based on NMRanalyses, DFT calculations, and isotopic labeling, showing an inversekinetic isotope effect, we demonstrate that the mechanism involvesa concerted proton–electron transfer to the electrode-adsorbedCO2 intermediate. The demonstrated mechanism provides guidelinesfor improvement in the energy efficiency of non-aqueous electrochemicalCO2 reduction, by a tailored design of electrolyte cations. |
| Related Links | https://europepmc.org/backend/ptpmcrender.fcgi?accid=PMC9578038&blobtype=pdf |
| Journal | ACS Energy Letters [ACS Energy Lett] |
| Volume Number | 7 |
| DOI | 10.1021/acsenergylett.2c01372 |
| PubMed Central reference number | PMC9578038 |
| Issue Number | 10 |
| PubMed reference number | 36277133 |
| e-ISSN | 23808195 |
| Language | English |
| Publisher | American Chemical Society |
| Publisher Date | 2022-09-15 |
| Access Restriction | Open |
| Rights License | Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). © 2022 The Authors. Published by American Chemical Society |
| Content Type | Text |
| Resource Type | Article |
| Subject | Chemistry Energy Engineering and Power Technology Renewable Energy, Sustainability and the Environment Materials Chemistry Fuel Technology |