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Ultraefficient homogeneous catalyst for the CO2-to-CO electrochemical conversion.


ABSTRACT: A very efficient electrogenerated Fe(0) porphyrin catalyst was obtained by substituting in tetraphenylporphyrin two of the opposite phenyl rings by ortho-, ortho'-phenol groups while the other two are perfluorinated. It proves to be an excellent catalyst of the CO2-to-CO conversion as to selectivity (the CO faradaic yield is nearly quantitative), overpotential, and turnover frequency. Benchmarking with other catalysts, through catalytic Tafel plots, shows that it is the most efficient, to the best of our knowledge, homogeneous molecular catalyst of the CO2-to-CO conversion at present. Comparison with another Fe(0) tetraphenylporphyrin bearing eight ortho-, ortho'-phenol functionalities launches a general strategy where changes in substituents will be designed so as to optimize the operational combination of all catalyst elements of merit.

SUBMITTER: Costentin C 

PROVIDER: S-EPMC4210317 | biostudies-literature | 2014 Oct

REPOSITORIES: biostudies-literature

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Ultraefficient homogeneous catalyst for the CO2-to-CO electrochemical conversion.

Costentin Cyrille C   Passard Guillaume G   Robert Marc M   Savéant Jean-Michel JM  

Proceedings of the National Academy of Sciences of the United States of America 20141006 42


A very efficient electrogenerated Fe(0) porphyrin catalyst was obtained by substituting in tetraphenylporphyrin two of the opposite phenyl rings by ortho-, ortho'-phenol groups while the other two are perfluorinated. It proves to be an excellent catalyst of the CO2-to-CO conversion as to selectivity (the CO faradaic yield is nearly quantitative), overpotential, and turnover frequency. Benchmarking with other catalysts, through catalytic Tafel plots, shows that it is the most efficient, to the be  ...[more]

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