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  Electrocatalytic CO2 Reduction on CuOx Nanocubes: Tracking the Evolution of Chemical State, Geometric Structure, and Catalytic Selectivity using Operando Spectroscopy

Möller, T., Scholten, F., Thanh, T. N., Sinev, I., Timoshenko, J., Wang, X., et al. (2020). Electrocatalytic CO2 Reduction on CuOx Nanocubes: Tracking the Evolution of Chemical State, Geometric Structure, and Catalytic Selectivity using Operando Spectroscopy. Angewandte Chemie International Edition, 59(41), 17974-17983. doi:10.1002/anie.202007136.

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 Creators:
Möller, Tim1, Author
Scholten, Fabian2, Author           
Thanh, Trung Ngo1, Author
Sinev, Ilya3, Author
Timoshenko, Janis2, Author           
Wang, Xingli1, Author
Jovanov, Zarko1, Author
Gliech, Manuel1, Author
Roldan Cuenya, Beatriz2, Author           
Varela, Ana Sofia4, Author
Strasser, Peter1, Author
Affiliations:
1The Electrochemical Energy, Catalysis, and Materials Science Laboratory, Department of Chemistry, Chemical Engineering Division, Technical University Berlin, Berlin, Germany, ou_persistent22              
2Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              
3Department of Physics, Ruhr-University Bochum, 44780 Bochum, Germany, ou_persistent22              
4Institute of Chemistry, National Autonomous University of Mexico, Mexico City, Mexico, ou_persistent22              

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 Abstract: The direct electrochemical conversion of carbon dioxide (CO2) into multi-carbon (C2+) products still faces
fundamental and technological challenges. While facet-controlled and oxide-derived Cu materials have
been touted as promising catalysts, their stability has remained problematic and poorly understood. The
present work uncovers changes in the chemical and morphological state of supported and unsupported Cu2O
nanocubes during operation in low-current H-Cells and in high-current Gas Diffusion Electrodes (GDEs)
using neutral pH buffer conditions. While unsupported nanocubes achieved a sustained C2+ faradaic
efficiency of around 60% for 40 h, the dispersion on a carbon support sharply shifted the selectivity pattern
towards C1 products. Operando XAS and time-resolved electron microscopy revealed the degradation of
the cubic shape and, in the presence of a carbon support, the formation of small Cu-seeds during the
surprisingly slow reduction of bulk Cu2O. Here, the initially (100)-rich facet structure has presumably no
controlling role on the catalytic selectivity, whereas the oxide-derived generation of under-coordinated
lattice defects, as revealed by the operando Cu-Cu coordination numbers, can support the high C2+ product
yields.

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Language(s): eng - English
 Dates: 2020-05-172020-07-022020-07-062020-10-05
 Publication Status: Issued
 Pages: 10
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/anie.202007136
 Degree: -

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Project name : OPERANDOCAT - In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects
Grant ID : 725915
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)

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Title: Angewandte Chemie International Edition
  Abbreviation : Angew. Chem., Int. Ed.
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: 10 Volume / Issue: 59 (41) Sequence Number: - Start / End Page: 17974 - 17983 Identifier: ISSN: 1433-7851
CoNE: https://pure.mpg.de/cone/journals/resource/1433-7851