Abstract
The controlled electrochemical reduction of carbon dioxide to value added chemicals is an important strategy in terms of renewable energy technologies. Therefore, the development of efficient and stable catalysts in an aqueous environment is of great importance. In this context, we focused on synthesizing and studying a molecular MnIII‐corrole complex, which is modified on the three meso‐positions with polyethylene glycol moieties for direct and selective production of acetic acid from CO2. Electrochemical reduction of MnIII leads to an electroactive MnII species, which binds CO2 and stabilizes the reduced intermediates. This catalyst allows to electrochemically reduce CO2 to acetic acid in a moderate acidic aqueous medium (pH 6) with a selectivity of 63 % and a turn over frequency (TOF) of 8.25 h−1, when immobilized on a carbon paper (CP) electrode. In terms of high selectivity towards acetate, we propose the formation and reduction of an oxalate type intermediate, stabilized at the MnIII‐corrole center.
Highlights
The growing consumption of fuels led to a drastic increase of the CO2 level in the atmosphere (33.1 Gt of CO2 in 2018[1])
Owing to its solubility in acetonitrile and insolubility in water heterogenization over different platforms like carbon paper (CP), indium doped tin oxide (ITO) and glassy carbon (GC) leads to facile fabrication of electrodes via drop casting, which are stable in aqueous solution
To demonstrate the charge transfer occurring between Mn-corrole and CO2, we have reduced MnIII-corrole typically by the addition of KC8 in dry acetonitrile solution
Summary
The growing consumption of fuels led to a drastic increase of the CO2 level in the atmosphere (33.1 Gt of CO2 in 2018[1]). The Heterogeneous Electrochemistry with Mn-Corrole Towards CO2 Reduction formation of the C2 product acetate is favored with a substantial increase in its FE (40 to 63 %, Table 1, Figure S14A).
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