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  4. Solution-based Cu+ transient species mediate the reconstruction of copper electrocatalysts for CO2 reduction
 
research article

Solution-based Cu+ transient species mediate the reconstruction of copper electrocatalysts for CO2 reduction

Vavra, Jan  
•
Ramona, Gaetan P. L.
•
Dattila, Federico
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January 3, 2024
Nature Catalysis

Understanding metal surface reconstruction is of the utmost importance in electrocatalysis, as this phenomenon directly affects the nature of available active sites. However, its dynamic nature renders surface reconstruction notoriously difficult to study. Here, we report on the intermediates that drive the rearrangement of copper catalysts for the electrochemical CO2 reduction reaction (CO2RR). Online MS and UV-vis absorption spectroscopy data are consistent with a dissolution-redeposition process, as previously demonstrated by in situ electron microscopy. The data indicate that the soluble transient species contain copper in the +1 oxidation state. Density functional theory identifies copper-adsorbate complexes that can exist in solution under operating conditions. Copper carbonyls and oxalates are suggested as the major reaction-specific species driving copper reconstruction during CO2RR. This work motivates future methodological studies to enable the direct detection of these compounds and strategies that specifically target them to improve the catalyst operational stability.

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Type
research article
DOI
10.1038/s41929-023-01070-8
Web of Science ID

WOS:001135867900002

Author(s)
Vavra, Jan  
Ramona, Gaetan P. L.
Dattila, Federico
Kormanyos, Attila
Priamushko, Tatiana
Albertini, Petru Pasquale  
Loiudice, Anna  
Cherevko, Serhiy
Lopez, Nuria
Buonsanti, Raffaella  
Date Issued

2024-01-03

Publisher

Nature Portfolio

Published in
Nature Catalysis
Volume

7

Issue

1

Start page

89

End page

97

Subjects

Physical Sciences

•

Surface Reconstruction

•

Carbon-Dioxide

•

Dissolution

•

Cu(111)

•

Electroreduction

•

Electrodes

•

Ensembles

•

Operando

•

Cu(100)

•

Metals

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LNCE  
FunderGrant Number

SNSF NCCR Catalysis Grant 180544

Ecole Normale Superieure Paris Saclay

NCCR Catalysis, National Centre of Competence in Research - Swiss National Science Foundation

180544

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Available on Infoscience
February 20, 2024
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/204882
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