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Probing CO₂ Reduction Pathways for Copper Catalysis Using an Ionic Liquid as a Chemical Trapping Agent

Zhang, Gui‐Rong ; Straub, Sascha‐Dominic ; Shen, Liu‐Liu ; Hermans, Yannick ; Schmatz, Patrick ; Reichert, Andreas M. ; Hofmann, Jan P. ; Katsounaros, Ioannis ; Etzold, Bastian J. M. (2021):
Probing CO₂ Reduction Pathways for Copper Catalysis Using an Ionic Liquid as a Chemical Trapping Agent. (Publisher's Version)
In: Angewandte Chemie International Edition, 59 (41), pp. 18095-18102. Wiley, ISSN 1433-7851, e-ISSN 1521-3773,
DOI: 10.26083/tuprints-00019357,
[Article]

Abstract

The key to fully leveraging the potential of the electrochemical CO₂ reduction reaction (CO2RR) to achieve a sustainable solar-power-based economy is the developmentof high-performance electrocatalysts. The development process relies heavily on trial and error methods due to poormechanistic understanding of the reaction. Demonstrated here is that ionic liquids (ILs) can be employed as achemical trapping agent to probe CO2RR mechanistic pathways. This method is implemented by introducing a small amount of an IL([BMIm][NTf₂]) to a copper foam catalyst, on which a wide range of CO2RR products,including formate, CO, alcohols, and hydrocarbons, can be produced. The IL can selectively suppress the formation of ethylene, ethanol and n-propanol while having little impact on others. Thus, reaction networks leading to various products can be disentangled. The results shed new light on the mechanistic understanding of the CO2RR, and provide guidelines for modulating the CO2RR properties. Chemical trapping using an IL adds to the toolbox to deduce the mechanistic understanding of electrocatalysis and could be applied to other reactions as well.

Item Type: Article
Erschienen: 2021
Creators: Zhang, Gui‐Rong ; Straub, Sascha‐Dominic ; Shen, Liu‐Liu ; Hermans, Yannick ; Schmatz, Patrick ; Reichert, Andreas M. ; Hofmann, Jan P. ; Katsounaros, Ioannis ; Etzold, Bastian J. M.
Origin: Secondary publication service
Status: Publisher's Version
Title: Probing CO₂ Reduction Pathways for Copper Catalysis Using an Ionic Liquid as a Chemical Trapping Agent
Language: English
Abstract:

The key to fully leveraging the potential of the electrochemical CO₂ reduction reaction (CO2RR) to achieve a sustainable solar-power-based economy is the developmentof high-performance electrocatalysts. The development process relies heavily on trial and error methods due to poormechanistic understanding of the reaction. Demonstrated here is that ionic liquids (ILs) can be employed as achemical trapping agent to probe CO2RR mechanistic pathways. This method is implemented by introducing a small amount of an IL([BMIm][NTf₂]) to a copper foam catalyst, on which a wide range of CO2RR products,including formate, CO, alcohols, and hydrocarbons, can be produced. The IL can selectively suppress the formation of ethylene, ethanol and n-propanol while having little impact on others. Thus, reaction networks leading to various products can be disentangled. The results shed new light on the mechanistic understanding of the CO2RR, and provide guidelines for modulating the CO2RR properties. Chemical trapping using an IL adds to the toolbox to deduce the mechanistic understanding of electrocatalysis and could be applied to other reactions as well.

Journal or Publication Title: Angewandte Chemie International Edition
Journal volume: 59
Number: 41
Publisher: Wiley
Divisions: 11 Department of Materials and Earth Sciences
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences > Material Science > Surface Science
07 Department of Chemistry
07 Department of Chemistry > Fachgebiet Technische Chemie
07 Department of Chemistry > Fachgebiet Technische Chemie > Technische Chemie I
Date Deposited: 26 Aug 2021 12:19
DOI: 10.26083/tuprints-00019357
Official URL: https://tuprints.ulb.tu-darmstadt.de/19357
URN: urn:nbn:de:tuda-tuprints-193578
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