Morphology and mechanism of highly selective Cu(II) oxide nanosheet catalysts for carbon dioxide electroreduction

Xingli Wang, Katharina Klingan, Malte Klingenhof, Tim Möller, Jorge Ferreira de Araújo, Isaac Martens, Alexander Bagger, Shan Jiang, Jan Rossmeisl, Holger Dau and Peter Strasser ()
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Xingli Wang: Technical University Berlin
Katharina Klingan: Free University of Berlin
Malte Klingenhof: Technical University Berlin
Tim Möller: Technical University Berlin
Jorge Ferreira de Araújo: Technical University Berlin
Isaac Martens: European Synchrotron Radiation Facility (ESRF)
Alexander Bagger: University of Copenhagen
Shan Jiang: Free University of Berlin
Jan Rossmeisl: University of Copenhagen
Holger Dau: Free University of Berlin
Peter Strasser: Technical University Berlin

Nature Communications, 2021, vol. 12, issue 1, 1-12

Abstract: Abstract Cu oxides catalyze the electrochemical carbon dioxide reduction reaction (CO2RR) to hydrocarbons and oxygenates with favorable selectivity. Among them, the shape-controlled Cu oxide cubes have been most widely studied. In contrast, we report on novel 2-dimensional (2D) Cu(II) oxide nanosheet (CuO NS) catalysts with high C2+ products, selectivities (> 400 mA cm−2) in gas diffusion electrodes (GDE) at industrially relevant currents and neutral pH. Under applied bias, the (001)-orientated CuO NS slowly evolve into highly branched, metallic Cu0 dendrites that appear as a general dominant morphology under electrolyte flow conditions, as attested by operando X-ray absorption spectroscopy and in situ electrochemical transmission electron microscopy (TEM). Millisecond-resolved differential electrochemical mass spectrometry (DEMS) track a previously unavailable set of product onset potentials. While the close mechanistic relation between CO and C2H4 was thereby confirmed, the DEMS data help uncover an unexpected mechanistic link between CH4 and ethanol. We demonstrate evidence that adsorbed methyl species, *CH3, serve as common intermediates of both CH3H and CH3CH2OH and possibly of other CH3-R products via a previously overlooked pathway at (110) steps adjacent to (100) terraces at larger overpotentials. Our mechanistic conclusions challenge and refine our current mechanistic understanding of the CO2 electrolysis on Cu catalysts.

Date: 2021
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DOI: 10.1038/s41467-021-20961-7

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