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Molecular cobalt corrole complex for the heterogeneous electrocatalytic reduction of carbon dioxide

 
: Gonglach, Sabine; Paul, Shounik; Haas, Michael; Pillwein, Felix; Sreekumar, S. Sreejith; Barman, Soumitra; De, Ratnadip; Müllegger, Stefan; Gerschel, Philipp; Apfel, Ulf-Peter; Coskun, Halime; Aljabour, Abdalaziz; Stadler, Philipp; Schöfberger, Wolfgang; Roy, Soumyajit

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Volltext urn:nbn:de:0011-n-5557675 (1.3 MByte PDF)
MD5 Fingerprint: 76d6bfa128029229e768eb4ffaa8e3e4
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Erstellt am: 5.9.2019


Nature Communications 10 (2019), Art. 3864, 10 S.
ISSN: 2041-1723
Englisch
Zeitschriftenaufsatz, Elektronische Publikation
Fraunhofer UMSICHT Oberhausen ()
carbon capture and storage; electrocatalysis; heterogeneous catalysis; materials for energy and catalysis; organometallic chemistry

Abstract
Electrochemical conversion of CO2 to alcohols is one of the most challenging methods of conversion and storage of electrical energy in the form of high-energy fuels. The challenge lies in the catalyst design to enable its real-life implementation. Herein, we demonstrate the synthesis and characterization of a cobalt(III) triphenylphosphine corrole complex, which contains three polyethylene glycol residues attached at the meso-phenyl groups. Electrondonation and therefore reduction of the cobalt from cobalt(III) to cobalt(I) is accompanied by removal of the axial ligand, thus resulting in a square-planar cobalt(I) complex. The cobalt(I) as an electron-rich supernucleophilic d8-configurated metal centre, where two electrons occupy and fill up the antibonding dz2 orbital. This orbital possesses high affinity towards electrophiles, allowing for such electronically configurated metals reactions with carbon dioxide. Herein, we report the potential dependent heterogeneous electroreduction of CO2 to ethanol or methanol of an immobilized cobalt A3-corrole catalyst system. In moderately acidic aqueous medium (pH = 6.0), the cobalt corrole modified carbon paper electrode exhibits a Faradaic Efficiency (FE%) of 48 % towards ethanol production.

: http://publica.fraunhofer.de/dokumente/N-555767.html