Functionalization of Carbon Nanotubes with Nickel Cyclam for the Electrochemical Reduction of CO2

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Abstract
The exploitation of molecular catalysts for CO2 electrolysis requires their immobilization on the cathode of the electrolyzer. As an illustration of this approach, a Ni‐cyclam complex with a cyclam derivative functionalized with a pyrene moiety is synthesized, found to be a selective catalyst for CO2 electroreduction to CO, and immobilized on a carbon nanotube‐coated gas diffusion electrode by using a noncovalent binding strategy. The as‐prepared electrode is efficient, selective, and robust for electrocatalytic reduction of CO2 to CO. Very high turnover numbers (ca. 61460) and turnover frequencies (ca. 4.27 s−1) are enabled by the novel electrode material in organic solvent‐water mixtures saturated with CO2. This material provides an interesting platform for further improvement.

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