Proceedings of nanoGe Spring Meeting 2022 (NSM22)
DOI: https://doi.org/10.29363/nanoge.nsm.2022.350
Publication date: 7th February 2022
Effective large-scale CO2 conversion to fuels or value-added chemicals using renewable energies is critical to reduce our environmental impact [1]. To this end, better understanding of the CO2 mechanism is needed to develop efficient and selective catalysts that operates in water controlling H2 evolution. Covalent Organic Frameworks (COFs) are reticular materials, which can be used to combine the advantages of the well-defined molecular catalysts and the heterogeneous ones [2]. In this work, we present the first COF based on tricarbonyl Mn units (COFbpyMn), that by π-π stacking is attached to MWCNTs form electrocatalytic electrodes active for CO2 reduction in neutral water. The activity of the catalyst was evaluated by electrochemical techniques with good stability in aqueous solution. The COFbpyMn shows a low CO2RR onset potential (η = 190 mV) and high current densities (>12 mA·cm–2, at 550 mV overpotential) in water. TOFCO and TONCO values are as high as 1100 h–1 and 5800 (after 16 h), respectively, which are more than 10-fold higher than those obtained for the equivalent manganese-based molecular catalyst. The encapsulation of tricarbonyl Mn single-atom centers within the reticular covalent organic structure plays an important role by favouring the electrocatalytic CO2 reduction over competitive H2 evolution reaction. The spectroelectrochemical studies evidence the formation of five-coordinate species in the catalytic cycle for CO formation. The COF imposes mechanical constraints on the {fac-Mn(CO)3S} centers.
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