The exploitation of molecular catalysts for CO 2 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 CO 2 electroreduction to CO, and immobilized on a carbon nanotubecoated gas diffusion electrode by using a noncovalent binding strategy. The as-prepared electrode is efficient, selective, and robust for electrocatalytic reduction of CO 2 to CO. Very high turnover numbers (ca. 61460) and turnover frequencies (ca. 4.27 s À 1) are enabled by the novel electrode material in organic solvent-water mixtures saturated with CO 2. This material provides an interesting platform for further improvement.
The development of molecular catalysts for CO2 electroreduction within electrolyzers requests their immobilization on the electrodes. While a variety of methods have been explored for the heterogenization of homogeneous complexes, a novel approach using a hierarchical porous carbon material, derived from a metal–organic framework, is reported as a support for the well‐known molecular catalyst [Re(bpy)(CO)3Cl] (bpy=2,2’‐bipyridine). This cathodic hybrid material, named Re@HPC (HPC=hierarchical porous carbon), has been tested for CO2 electroreduction using a mixture of an ionic liquid (1‐ethyl‐3‐methylimidazolium tetrafluoroborate, EMIM) and water as the electrolyte. Interestingly, it catalyzes the conversion of CO2 into a mixture of carbon monoxide and formic acid, with a selectivity that depends on the applied potential. The present study thus reveals that Re@HPC is a remarkable catalyst, enjoying excellent activity (turnover numbers for CO2 reduction of 7835 after 2 h at −1.95 V vs. Fc/Fc+ with a current density of 6 mA cm−2) and good stability. These results emphasize the advantages of integrating molecular catalysts onto such porous carbon materials for developing novel, stable and efficient, catalysts for CO2 reduction.
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