Is Cu instability during the CO2 reduction reaction governed by the applied potential or the local CO concentration?

Patrick Wilde; Peter B. O'Mara; João R. C. Junqueira; Tsvetan Tarnev; Tania M. Benedetti; Corina Andronescu; Yen-Ting Chen; Richard D. Tilley; Wolfgang Schuhmann; J. Justin Gooding

doi:10.1039/D0SC05990K

Is Cu instability during the CO₂ reduction reaction governed by the applied potential or the local CO concentration?†

Patrick Wilde,

‡^a Peter B. O'Mara,

‡^b João R. C. Junqueira,

^a Tsvetan Tarnev,

^a Tania M. Benedetti,

^b Corina Andronescu,

^c Yen-Ting Chen,

^d Richard D. Tilley,

*^be Wolfgang Schuhmann

*^a and J. Justin Gooding

*^bf

Author affiliations

* Corresponding authors

^a Analytical Chemistry - Center for Electrochemical Sciences (CES), Faculty of Chemistry and Biochemistry, Ruhr-Universität Bochum, Universitätsstr. 150, D-44780 Bochum, Germany
E-mail: wolfgang.schuhmann@rub.de

^b School of Chemistry, Australian Centre for NanoMedicine, University of New South Wales, Sydney 2052, Australia
E-mail: justin.gooding@unsw.edu.au, r.tilley@unsw.edu.au

^c Chemical Technology III, Faculty of Chemistry and CENIDE, Center for Nanointegration University Duisburg Essen, Carl-Benz-Str. 199, D-47057 Duisburg, Germany

^d Center for Solvation Science (ZEMOS), Ruhr-Universität Bochum, Universitätsstr. 150, D-44780 Bochum, Germany

^e Electron Microscope Unit, Mark Wainwright Analytical Centre, University of New South Wales, Sydney 2052, Australia

^f Australian Research Council Centre of Excellence in Convergent Bio-Nano Science and Technology, University of New South Wales, Sydney 2052, Australia

Abstract

Cu-based catalysts have shown structural instability during the electrochemical CO₂ reduction reaction (CO₂RR). However, studies on monometallic Cu catalysts do not allow a nuanced differentiation between the contribution of the applied potential and the local concentration of CO as the reaction intermediate since both are inevitably linked. We first use bimetallic Ag-core/porous Cu-shell nanoparticles, which utilise nanoconfinement to generate high local CO concentrations at the Ag core at potentials at which the Cu shell is still inactive for the CO₂RR. Using operando liquid cell TEM in combination with ex situ TEM, we can unequivocally confirm that the local CO concentration is the main source for the Cu instability. The local CO concentration is then modulated by replacing the Ag-core with a Pd-core which further confirms the role of high local CO concentrations. Product quantification during CO₂RR reveals an inherent trade-off between stability, selectivity and activity in both systems.

This article is part of the themed collection: Editor’s Choice – Jinlong Gong

Chemical Science

Is Cu instability during the CO₂ reduction reaction governed by the applied potential or the local CO concentration?†

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Is Cu instability during the CO₂ reduction reaction governed by the applied potential or the local CO concentration?

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