Enhanced Catalytic Activity of Cobalt Porphyrin in CO2 Electroreduction upon Immobilization on Carbon Materials

In a comparative study of the electrocatalytic CO2 reduction, cobalt meso‐tetraphenylporphyrin (CoTPP) is used as a model molecular catalyst under both homogeneous and heterogeneous conditions. In the former case, employing N,N‐dimethylformamide as solvent, CoTPP performs poorly as an electrocatalys...

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Bibliographic Details
Published in:Angewandte Chemie 2017-06, Vol.129 (23), p.6568-6572
Main Authors: Hu, Xin‐Ming, Rønne, Magnus H., Pedersen, Steen U., Skrydstrup, Troels, Daasbjerg, Kim
Format: Article
Language:eng ; ger
Subjects:
Adsorption
Aqueous solutions
Carbon dioxide
Carbon nanotubes
Catalysts
Catalytic activity
Chemistry
CO2-Reduktion
Cobalt
Comparative studies
Dimethylformamide
Electrocatalysts
Elektrokatalyse
Heterogenkatalysatoren
Immobilisierung
Immobilization
Molekulare Katalysatoren
Nanotechnology
Nanotubes
Porphyrins
Selectivity
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Summary:In a comparative study of the electrocatalytic CO2 reduction, cobalt meso‐tetraphenylporphyrin (CoTPP) is used as a model molecular catalyst under both homogeneous and heterogeneous conditions. In the former case, employing N,N‐dimethylformamide as solvent, CoTPP performs poorly as an electrocatalyst giving low product selectivity in a slow reaction at a high overpotential. However, upon straightforward immobilization of CoTPP onto carbon nanotubes, a remarkable enhancement of the electrocatalytic abilities is seen with CO2 becoming selectively reduced to CO (>90 %) at a low overpotential in aqueous medium. This effect is ascribed to the particular environment created by the aqueous medium at the catalytic site of the immobilized catalyst that facilitates the adsorption and further reaction of CO2. This work highlights the significance of assessing an immobilized molecular catalyst from more than homogeneous measurements alone. Heterogen versus homogen: Wird Cobalt‐meso‐tetraphenylporphyrin (CoTTP) auf Kohlenstoffnanoröhren immobilisiert, resultiert eine bemerkenswert erhöhte katalytische Aktivität in der CO2‐Elektroreduktion, mit [CoITPP]− als der aktiven Spezies. Der hier beschriebene Ansatz zur Heterogenisierung ermöglicht die einfache Durchmusterung und Evaluierung molekularer Katalysatoren unter heterogenen Bedingungen.
ISSN:0044-8249
1521-3757
DOI:10.1002/ange.201701104