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

Nathan Hollingsworth; S. F. Rebecca Taylor; Miguel T. Galante; Johan Jacquemin; Claudia Longo; Katherine B. Holt; Nora H. de Leeuw; Christopher Hardacre

doi:10.1002/anie.201507629

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

Nathan Hollingsworth, S. F. Rebecca Taylor, Miguel T. Galante, Johan Jacquemin, Claudia Longo, Katherine B. Holt, Nora H. de Leeuw, Christopher Hardacre

School of Chemistry and Chemical Engineering

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Abstract

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.

Original language	English
Pages (from-to)	14164
Number of pages	6
Journal	Angewandte Chemie International Edition
Volume	54
Issue number	47
Early online date	22 Sept 2015
DOIs	https://doi.org/10.1002/anie.201507629
Publication status	Published - 2015

Keywords

CO2 reduction, electrolysis, formate, ionic liquids, superbases

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10.1002/anie.201507629

Reduction of Carbon Dioxide to Formate at Low Overpotential using a Superbase Ionic Liquid
2015 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the Creative Commons Attribution License, (https://creativecommons.org/licenses/by/4.0/), which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
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title = "Reduction of Carbon Dioxide to Formate at Low Overpotential using a Superbase Ionic Liquid",

abstract = "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.",

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year = "2015",

doi = "10.1002/anie.201507629",

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T1 - Reduction of Carbon Dioxide to Formate at Low Overpotential using a Superbase Ionic Liquid

AU - Hollingsworth, Nathan

AU - Taylor, S. F. Rebecca

AU - Galante, Miguel T.

AU - Jacquemin, Johan

AU - Longo, Claudia

AU - Holt, Katherine B.

AU - de Leeuw, Nora H.

AU - Hardacre, Christopher

PY - 2015

Y1 - 2015

N2 - 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.

AB - 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.

KW - CO2 reduction, electrolysis, formate, ionic liquids, superbases

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DO - 10.1002/anie.201507629

M3 - Article

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JF - Angewandte Chemie International Edition

IS - 47

ER -

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

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