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

Nathan Hollingsworth; 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, Rebecca Taylor, Miguel T. Galante, Johan Jacquemin, Claudia Longo, Katherine B. Holt, Nora H. De Leeuw, Christopher Hardacre^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

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)	14164-14168
Number of pages	5
Journal	Angewandte Chemie - International Edition
Volume	54
Issue number	47
DOIs	https://doi.org/10.1002/anie.201507629
Publication status	Published - 10 Nov 2015

Keywords

CO reduction
electrolysis
formate
ionic liquids
superbases

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1002/anie.201507629

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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.",

keywords = "CO reduction, electrolysis, formate, ionic liquids, superbases",

author = "Nathan Hollingsworth and Rebecca Taylor and Galante, {Miguel T.} and Johan Jacquemin and Claudia Longo and Holt, {Katherine B.} and {De Leeuw}, {Nora H.} and Christopher Hardacre",

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doi = "10.1002/anie.201507629",

language = "English",

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TY - JOUR

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

AU - Hollingsworth, Nathan

AU - Taylor, Rebecca

AU - Galante, Miguel T.

AU - Jacquemin, Johan

AU - Longo, Claudia

AU - Holt, Katherine B.

AU - De Leeuw, Nora H.

AU - Hardacre, Christopher

PY - 2015/11/10

Y1 - 2015/11/10

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 - CO reduction

KW - electrolysis

KW - formate

KW - ionic liquids

KW - superbases

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U2 - 10.1002/anie.201507629

DO - 10.1002/anie.201507629

M3 - Article

SN - 1433-7851

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EP - 14168

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 47

ER -

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

Abstract

Keywords

UN SDGs

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