Understanding the role of imidazolium-based ionic liquids in the electrochemical CO2 reduction reaction
Communications Chemistry, Electrocatalytic CO2 reduction (2023)
by Alessia Fortunati; Francesca Risplendi; Michele Re Fiorentin; Giancarlo Cicero; Emmanuele Parisi; Micaela Castellino; Elena Simone; Nunzio Russo; Simelys Hernández (Department of Applied Science and Technology, Politecnico di Torino); Boyan Iliev and Thomas J. S. Schubert (Iolitec Ioniq Liquids Technologies GmbH).
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.