Dataset Information

Understanding the role of imidazolium-based ionic liquids in the electrochemical CO₂ reduction reaction.

ABSTRACT: The development of efficient CO₂ capture and utilization technologies driven by renewable energy sources is mandatory to reduce the impact of climate change. Herein, seven imidazolium-based ionic liquids (ILs) with different anions and cations were tested as catholytes for the CO₂ electrocatalytic reduction to CO over Ag electrode. Relevant activity and stability, but different selectivities for CO₂ reduction or the side H₂ evolution were observed. Density functional theory results show that depending on the IL anions the CO₂ is captured or converted. Acetate anions (being strong Lewis bases) enhance CO₂ capture and H₂ evolution, while fluorinated anions (being weaker Lewis bases) favour the CO₂ electroreduction. Differently from the hydrolytically unstable 1-butyl-3-methylimidazolium tetrafluoroborate, 1-Butyl-3-Methylimidazolium Triflate was the most promising IL, showing the highest Faradaic efficiency to CO (>95%), and up to 8 h of stable operation at high current rates (-20 mA & -60 mA), which opens the way for a prospective process scale-up.

SUBMITTER: Fortunati A

PROVIDER: S-EPMC10148827 | biostudies-literature | 2023 Apr

REPOSITORIES: biostudies-literature

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Understanding the role of imidazolium-based ionic liquids in the electrochemical CO2 reduction reaction.

Fortunati Alessia A Risplendi Francesca F Re Fiorentin Michele M Cicero Giancarlo G Parisi Emmanuele E Castellino Micaela M Simone Elena E Iliev Boyan B Schubert Thomas J S TJS Russo Nunzio N Hernández Simelys S

Communications chemistry 20230429 1

The development of efficient CO2 capture and utilization technologies driven by renewable energy sources is mandatory to reduce the impact of climate change. Herein, seven imidazolium-based ionic liquids (ILs) with different anions and cations were tested as catholytes for the CO2 electrocatalytic reduction to CO over Ag electrode. Relevant activity and stability, but different selectivities for CO2 reduction or the side H2 evolution were observed. Den ...[more]

PMID: 37120643

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Project description:Carbon capture and sequestration are the major applied techniques for mitigating CO2 emission. The marked affinity of carbon dioxide to react with amino groups is well known, and the amine scrubbing process is the most widespread technology. Among various compounds and solutions containing amine groups, in biodegradability and biocompatibility perspectives, amino acid ionic liquids (AAILs) are a very promising class of materials having good CO2 absorption capacity. The reaction of amines with CO2 follows a multi-step mechanism where the initial pathway is the formation of the C-N bond between the NH2 group and CO2. The added product has a zwitterionic character and can rearrange to give a carbamic derivative. These steps of the mechanism have been investigated in the present study by quantum mechanical methods by considering three ILs where amino acid anions are coupled with choline cations. Glycinate, L-phenylalanilate and L-prolinate anions have been compared with the aim of examining if different local structural properties of the amine group can affect some fundamental steps of the CO2 absorption mechanism. All reaction pathways have been studied by DFT methods considering, first, isolated anions in a vacuum as well as in a liquid continuum environment. Subsequently, the role of specific interactions of the anion with a choline cation has been investigated, analyzing the mechanism of the amine-CO2 reaction, including different coupling anion-cation structures. The overall reaction is exothermic for the three anions in all models adopted; however, the presence of the solvent, described by a continuum medium as well as by models, including specific cation- -anion interactions, modifies the values of the reaction energies of each step. In particular, both reaction steps, the addition of CO2 to form the zwitterionic complex and its subsequent rearrangement, are affected by the presence of the solvent. The reaction enthalpies for the three systems are indeed found comparable in the models, including solvent effects.

Dataset Information

Understanding the role of imidazolium-based ionic liquids in the electrochemical CO₂ reduction reaction.

Publications

Understanding the role of imidazolium-based ionic liquids in the electrochemical CO<sub>2</sub> reduction reaction.

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