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Ionic liquids (ILs) in electrocatalysis have attracted a lot of attention from the seminal work of Rosen et al. [1] where they achieved a relevant overpotential decrease for CO2 reduction reaction (CO2RR) on a silver electrode. Moreover, ILs have been proposed as organic promoters for enhancing the catalytic activity by modifying the electrostatic properties at the electrochemical interface. Then, electrolyte engineering has become a powerful way to impact on the stability of reaction intermediates and control reaction selectivity.   The role of different ILs as simultaneous supporting electrolyte and co-catalyst in acetonitrile for CO2 electroreduction in the presence of a model molecular catalyst [Re(bpy)(CO)3Cl] is presented here. [2] In particular, the nature of the cation, anion and cation alkyl chain is varied by a choice of 5 different ILs, including imidazolium and pyrrolidinium cations and their results are compared to conventional benchmark supporting electrolyte. Under catalytic conditions an overpotential diminution of 0.33 V for CO2 to CO conversion is achieved in the presence of ILs. Finally, a mechanistic explanation is provided to justify this behaviour. [1] Rosen, B.A.; Salehi-Khojin, A.; Thorson, M.R.; Zhu, W.; Whipple, D.T.; Kenis, P.J.A.; Masel, R.I. Science 2011, 334 (6056), 643. [2] Vichou, E.; Xu-Li, Y.; Gomez-Mingot, M.; Fontecave, M.; Sánchez-Sánchez, C.M. J. Phys. Chem. C 2020, 124, 23764.

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