Publication date: 6th November 2020
Electroreduction of CO2 is one of the ways to valorise CO2 as a source of carbon. 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, mainly introducing functionalities to the molecular catalysts, we here report a novel approach using a hierarchical porous carbon material, derived from a Metal Organic Framework, as a support for the well-known molecular catalyst [Re(bpy)(CO)3Cl] (bpy = 2,2’-bipyridine). This cathodic hybrid material, named Re@HPC, 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 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 if compared to other hybrid solid electrode where [Re(bpy)(CO)3Cl] has been immobilized.These results emphasize the advantages of integrating molecular catalysts onto such porous carbon materials for developing novel, stable and efficient, catalysts for CO2 reduction.
Acknowledgments for the financial support from the European
School on Artificial Leaf: Electrodes & Devices (eSCALED). This
work is part of the eSCALED project which has received funding
from the European’s Union’s Horizon 2020 research and innovation
programme under the Marie Sklodowska-Curie grant agreement
No 765376.