Reduction of Carbon Dioxide to Formate at Low Overpotential Using a Superbase Ionic Liquid

A new low‐energy pathway is reported for the electrochemical reduction of CO2 to formate and syngas at low overpotentials, utilizing a reactive ionic liquid as the solvent. The superbasic tetraalkyl phosphonium ionic liquid [P66614][124Triz] is able to chemisorb CO2 through equimolar binding of CO2...

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Bibliographic Details
Published in:Angewandte Chemie 2015-11, Vol.127 (47), p.14370-14374
Main Authors: Hollingsworth, Nathan, Taylor, S. F. Rebecca, Galante, Miguel T., Jacquemin, Johan, Longo, Claudia, Holt, Katherine B., de Leeuw, Nora H., Hardacre, Christopher
Format: Article
Language:eng ; ger
Subjects:
Carbon dioxide
Carbon monoxide
Chemical reduction
Chemisorption
Chemistry
CO2‐Reduktion
Electrochemistry
Electrodes
Elektrolyse
Formates
Formiat
Ionic liquids
Ionische Flüssigkeiten
Ions
Reduction
Solvents
Superbasen
Synthesis gas
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Summary:A new low‐energy pathway is reported for the electrochemical reduction of CO2 to formate and syngas at low overpotentials, utilizing a reactive ionic liquid as the solvent. The superbasic tetraalkyl phosphonium ionic liquid [P66614][124Triz] is able to chemisorb CO2 through equimolar binding of CO2 with the 1,2,4‐triazole anion. This chemisorbed CO2 can be reduced at silver electrodes at overpotentials as low as 0.17 V, forming formate. In contrast, physically absorbed CO2 within the same ionic liquid or in ionic liquids where chemisorption is impossible (such as [P66614][NTf2]) undergoes reduction at significantly increased overpotentials, producing only CO as the product. [P66614][124Triz], eine bei Raumtemperatur flüssige ionische Verbindung (RTIL), öffnet einen alternativen energetisch günstigen Pfad für die Umwandlung von CO2 in Formiat. Hier senkt die chemische Bindung von CO2 an das RTIL‐Anion, durch die CO2 nicht mehr linear, sondern gebogen vorliegt, erstmals die Aktivierungsenergie für die elektrochemische CO2‐Reduktion.
ISSN:0044-8249
1521-3757
DOI:10.1002/ange.201507629