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

Sabrina Gonglach, Shounik Paul, Michael Haas, Felix Pillwein, Sreekumar S. Sreejith, Soumitra Barman, Ratnadip De, Stefan Müllegger, Philipp Gerschel, Ulf-Peter Apfel, Halime Coskun, Abdalaziz Aljabour, Philipp Stadler, Wolfgang Schöfberger () and Soumyajit Roy ()
Additional contact information
Sabrina Gonglach: Institute of Organic Chemistry, Johannes Kepler University Linz
Shounik Paul: Eco-Friendly Applied Materials Laboratory (EFAML), Materials Science Centre, Department of Chemical Sciences, Mohanpur Campus, Indian Institute of Science Education and Research
Michael Haas: Institute of Organic Chemistry, Johannes Kepler University Linz
Felix Pillwein: Institute of Organic Chemistry, Johannes Kepler University Linz
Sreekumar S. Sreejith: Eco-Friendly Applied Materials Laboratory (EFAML), Materials Science Centre, Department of Chemical Sciences, Mohanpur Campus, Indian Institute of Science Education and Research
Soumitra Barman: Eco-Friendly Applied Materials Laboratory (EFAML), Materials Science Centre, Department of Chemical Sciences, Mohanpur Campus, Indian Institute of Science Education and Research
Ratnadip De: Eco-Friendly Applied Materials Laboratory (EFAML), Materials Science Centre, Department of Chemical Sciences, Mohanpur Campus, Indian Institute of Science Education and Research
Stefan Müllegger: Institute of Semiconductor and Solid State Physics, Johannes Kepler University Linz
Philipp Gerschel: Inorganic Chemistry I, Ruhr-Universität Bochum NC 3/74
Ulf-Peter Apfel: Inorganic Chemistry I, Ruhr-Universität Bochum NC 3/74
Halime Coskun: Institute of Physical Chemistry and Linz Institute of Organic Solar Cells, Johannes Kepler University Linz
Abdalaziz Aljabour: Institute of Physical Chemistry and Linz Institute of Organic Solar Cells, Johannes Kepler University Linz
Philipp Stadler: Institute of Physical Chemistry and Linz Institute of Organic Solar Cells, Johannes Kepler University Linz
Wolfgang Schöfberger: Institute of Organic Chemistry, Johannes Kepler University Linz
Soumyajit Roy: Eco-Friendly Applied Materials Laboratory (EFAML), Materials Science Centre, Department of Chemical Sciences, Mohanpur Campus, Indian Institute of Science Education and Research

Nature Communications, 2019, vol. 10, issue 1, 1-10

Abstract: 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. Electron-donation 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.

Date: 2019
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DOI: 10.1038/s41467-019-11868-5

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