Immobilization of a Molecular Re Complex on MOF-Derived Hierarchical Porous Carbon for CO2 Electroreduction in Water/Ionic Liquid Electrolyte
Domenico Grammatico a c, Huan Ngoc Tran b, Yun Li b, Silvia Pugliese a b, Laurent Billon c, Bao-Lian Su a, Marc Fontecave b
a Laboratory of Inorganic Materials Chemistry (CMI), University of Namur, France
b College de France, Place Marcelin Berthelot, 1175231 Paris Cedex 05, Paris, France
c EPCP, IPREM (UMR-5254), Université de Pau et des Pays de l'Adour, 2 avenue du Président Angot, 64053 Pau, Cedex, France
Proceedings of International Conference on Electrocatalysis for Energy Applications and Sustainable Chemicals (EcoCat)
Online, Spain, 2020 November 23rd - 25th
Organizers: Ward van der Stam, Marta Costa Figueiredo, Sixto Gimenez Julia, Núria López and Bastian Mei
Poster, Domenico Grammatico, 048
Publication date: 6th November 2020
ePoster: 

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.

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