The electrochemical reduction of CO2 to value-added products is hindered by its thermodynamic stability and by the large energy required to chemically activate the molecule. With this respect, forcing CO2 in a non-linear geometry would induce an internal electron charge rearrangement which would facilitate further electrochemical transformations. In this work, we achieved this goal through the design of a dual function electro-organocatalyst, which exploits the ability of the imidazolate (Im-) lone pair to bind CO2 via nucleophilic attack and then electrochemically reduce it. To give structural stability to the Im- based catalyst, the imidazoles species are incorporated into a solid structure, namely ZIF-8. Once activated by the organic Im- ligand, CO2 is electrochemically reduced to CO when a bias is applied to ZIF-8. The catalyst proposed in our study was first devised by computer aided design based on Density functional Theory simulations and then realized in laboratory. Our results demonstrate that ZIF-8 supported on conductive CNTs presents surface Im- active sites which convert CO2 into CO with a high faradaic efficiency (70.4 %) at −1.2 V vs reversible hydrogen electrode, by combining chemical activation with electrochemical catalysis.

Imidazole-imidazolate pair as organo-electrocatalyst for CO2 reduction on ZIF-8 material / Sassone, D.; Bocchini, S.; Fontana, M.; Salvini, C.; Cicero, G.; Re Fiorentin, M.; Risplendi, F.; Latini, G.; Amin Farkhondehfal, M.; Pirri, F.; Zeng, J.. - In: APPLIED ENERGY. - ISSN 0306-2619. - ELETTRONICO. - 324:(2022), p. 119743. [10.1016/j.apenergy.2022.119743]

Imidazole-imidazolate pair as organo-electrocatalyst for CO2 reduction on ZIF-8 material

Sassone D.;Bocchini S.;Fontana M.;Salvini C.;Cicero G.;Re Fiorentin M.;Risplendi F.;Latini G.;Amin Farkhondehfal M.;Pirri F.;Zeng J.
2022

Abstract

The electrochemical reduction of CO2 to value-added products is hindered by its thermodynamic stability and by the large energy required to chemically activate the molecule. With this respect, forcing CO2 in a non-linear geometry would induce an internal electron charge rearrangement which would facilitate further electrochemical transformations. In this work, we achieved this goal through the design of a dual function electro-organocatalyst, which exploits the ability of the imidazolate (Im-) lone pair to bind CO2 via nucleophilic attack and then electrochemically reduce it. To give structural stability to the Im- based catalyst, the imidazoles species are incorporated into a solid structure, namely ZIF-8. Once activated by the organic Im- ligand, CO2 is electrochemically reduced to CO when a bias is applied to ZIF-8. The catalyst proposed in our study was first devised by computer aided design based on Density functional Theory simulations and then realized in laboratory. Our results demonstrate that ZIF-8 supported on conductive CNTs presents surface Im- active sites which convert CO2 into CO with a high faradaic efficiency (70.4 %) at −1.2 V vs reversible hydrogen electrode, by combining chemical activation with electrochemical catalysis.
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11583/2971426