Promoting Selective CO2 Electroreduction to Formic Acid in Acidic Medium with Low Potassium Concentrations under High CO2 Pressure

Abstract Electrocatalytic CO2 reduction reaction (CO2RR) offers a sustainable pathway for the production of chemicals and fuels. Acidic electrolysis has been shown to be a promising strategy in order to avoid CO2 loss via the formation (bi)carbonate during reaction. Previous studies have been carrie...

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Main Authors: Florian Lhostis, Ngoc‐Huan Tran, Gwenaëlle Rousse, Sandrine Zanna, Nicolas Menguy, Marc Fontecave
Format: Article
Language:English
Published: Wiley-VCH 2024-04-01
Series:ChemElectroChem
Subjects:
Online Access:https://doi.org/10.1002/celc.202300799
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author Florian Lhostis
Ngoc‐Huan Tran
Gwenaëlle Rousse
Sandrine Zanna
Nicolas Menguy
Marc Fontecave
author_facet Florian Lhostis
Ngoc‐Huan Tran
Gwenaëlle Rousse
Sandrine Zanna
Nicolas Menguy
Marc Fontecave
author_sort Florian Lhostis
collection DOAJ
description Abstract Electrocatalytic CO2 reduction reaction (CO2RR) offers a sustainable pathway for the production of chemicals and fuels. Acidic electrolysis has been shown to be a promising strategy in order to avoid CO2 loss via the formation (bi)carbonate during reaction. Previous studies have been carried out in ambient CO2 pressure systems and have stressed the importance of adding high concentration of alkali cation (K+) in the catholyte to inhibit the hydrogen evolution reaction (HER) and achieve higher selectivity of CO2RR. Herein, CO2 reduction to HCOOH was performed in strong acid (pH 1) using a dendritic bismuth catalyst in a home‐designed high‐pressure electrochemical cell. At a CO2 pressure of 30 bar, we could achieve a high Faradaic efficiency of 100 % at 100 mA cm−2 at a KCl concentration of 3.0 M. With this first system that combines high pressure of CO2 and highly acidic catholyte, we show that pressurization offers an appropriate strategy to limit both HER and K+ dependence. Indeed we obtained a Faradaic efficiency of 34 % in the absence of K+ cations and 75–80 % in the presence of 1.0 M KCl under an applied current density of 100 mA cm−2.
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spelling doaj.art-83ff402f282d4d0aa6b8a565b3f5c9d12024-04-04T17:37:37ZengWiley-VCHChemElectroChem2196-02162024-04-01117n/an/a10.1002/celc.202300799Promoting Selective CO2 Electroreduction to Formic Acid in Acidic Medium with Low Potassium Concentrations under High CO2 PressureFlorian Lhostis0Ngoc‐Huan Tran1Gwenaëlle Rousse2Sandrine Zanna3Nicolas Menguy4Marc Fontecave5Laboratoire de Chimie des Processus Biologiques CNRS UMR 8229 Collège de France Sorbonne Université 11 Place Marcelin Berthelot 75231 Paris Cedex 05 FranceLaboratoire de Chimie des Processus Biologiques CNRS UMR 8229 Collège de France Sorbonne Université 11 Place Marcelin Berthelot 75231 Paris Cedex 05 FranceLaboratoire de Chimie du Solide et Energie FRE 3677 Collège de France Université Pierre et Marie Curie 11 Place Marcelin Berthelot 75231 Paris Cedex 05 FranceChimie ParisTech PSL Research University CNRS Institut de Recherche de Chimie Paris (IRCP) 11 rue Pierre et Marie Curie 75005 Paris FranceSorbonne Université UMR CNRS 7590 Institut de Minéralogie de Physique des Matériaux et de Cosmochimie 75005 Paris FranceLaboratoire de Chimie des Processus Biologiques CNRS UMR 8229 Collège de France Sorbonne Université 11 Place Marcelin Berthelot 75231 Paris Cedex 05 FranceAbstract Electrocatalytic CO2 reduction reaction (CO2RR) offers a sustainable pathway for the production of chemicals and fuels. Acidic electrolysis has been shown to be a promising strategy in order to avoid CO2 loss via the formation (bi)carbonate during reaction. Previous studies have been carried out in ambient CO2 pressure systems and have stressed the importance of adding high concentration of alkali cation (K+) in the catholyte to inhibit the hydrogen evolution reaction (HER) and achieve higher selectivity of CO2RR. Herein, CO2 reduction to HCOOH was performed in strong acid (pH 1) using a dendritic bismuth catalyst in a home‐designed high‐pressure electrochemical cell. At a CO2 pressure of 30 bar, we could achieve a high Faradaic efficiency of 100 % at 100 mA cm−2 at a KCl concentration of 3.0 M. With this first system that combines high pressure of CO2 and highly acidic catholyte, we show that pressurization offers an appropriate strategy to limit both HER and K+ dependence. Indeed we obtained a Faradaic efficiency of 34 % in the absence of K+ cations and 75–80 % in the presence of 1.0 M KCl under an applied current density of 100 mA cm−2.https://doi.org/10.1002/celc.202300799Bi-based electrocatalystsCO2 electroreductionacidic electrolyteFormic acidHigh pressure cell
spellingShingle Florian Lhostis
Ngoc‐Huan Tran
Gwenaëlle Rousse
Sandrine Zanna
Nicolas Menguy
Marc Fontecave
Promoting Selective CO2 Electroreduction to Formic Acid in Acidic Medium with Low Potassium Concentrations under High CO2 Pressure
ChemElectroChem
Bi-based electrocatalysts
CO2 electroreduction
acidic electrolyte
Formic acid
High pressure cell
title Promoting Selective CO2 Electroreduction to Formic Acid in Acidic Medium with Low Potassium Concentrations under High CO2 Pressure
title_full Promoting Selective CO2 Electroreduction to Formic Acid in Acidic Medium with Low Potassium Concentrations under High CO2 Pressure
title_fullStr Promoting Selective CO2 Electroreduction to Formic Acid in Acidic Medium with Low Potassium Concentrations under High CO2 Pressure
title_full_unstemmed Promoting Selective CO2 Electroreduction to Formic Acid in Acidic Medium with Low Potassium Concentrations under High CO2 Pressure
title_short Promoting Selective CO2 Electroreduction to Formic Acid in Acidic Medium with Low Potassium Concentrations under High CO2 Pressure
title_sort promoting selective co2 electroreduction to formic acid in acidic medium with low potassium concentrations under high co2 pressure
topic Bi-based electrocatalysts
CO2 electroreduction
acidic electrolyte
Formic acid
High pressure cell
url https://doi.org/10.1002/celc.202300799
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