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

Daniele Sassone, Sergio Bocchini, Marco Fontana, Clara Salvini, Giancarlo Cicero, Michele Re Fiorentin, Francesca Risplendi, Giulio Latini, M. Amin Farkhondehfal, Fabrizio Pirri and Juqin Zeng

Applied Energy, 2022, vol. 324, issue C, No S0306261922010303

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.

Keywords: Molecular catalysis; Electrochemistry; CO2 activation; Imidazole; Modelling-guided synthesis; ZIF-8; DFT; Mechanism (search for similar items in EconPapers)
Date: 2022
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DOI: 10.1016/j.apenergy.2022.119743

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