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  Identifying structure-selectivity correlations in the electrochemical reduction of CO2: comparison of well-ordered atomically-clean and chemically-etched Cu single crystal surfaces

Scholten, F., Nguyen, K.-L.-C., Bruce, J. P., Heyde, M., & Roldan Cuenya, B. (2021). Identifying structure-selectivity correlations in the electrochemical reduction of CO2: comparison of well-ordered atomically-clean and chemically-etched Cu single crystal surfaces. Angewandte Chemie, 133(35), 19318-19324. doi:10.1002/ange.202103102.

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ange.202103102.pdf (Publisher version), 2MB
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 Creators:
Scholten, Fabian1, Author              
Nguyen, Khanh-Ly Claudia1, Author              
Bruce, Jared P.1, Author              
Heyde, Markus1, Author              
Roldan Cuenya, Beatriz1, Author              
Affiliations:
1Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              

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 Abstract: Despite significant theoretical efforts, the identification of the active sites for the electrochemical reduction of CO2 (CO2RR) to specific chemical products has remained elusive. This is partially due to insufficient experimental data gathered on clean and atomically well-ordered electrode surfaces. Here, ultrahigh vacuum based preparation methods and surface science characterization techniques are used together with gas chromatography to demonstrate that subtle changes in the preparation of well-oriented Cu(100) and Cu(111) single crystal surfaces drastically affect their CO2RR selectivity. Copper single crystals with clean, flat, and atomically ordered surfaces are theoretically predicted to yield hydrocarbons. However, these were found experimentally to favour the production of H2. Only when roughness and defects are introduced, for example through an electrochemical etchingor a plasmatreatment, significant amounts of hydrocarbons are generated. These results clearly indicate that structural and morphological effects are the key factors determining the catalytic selectivity of CO2RR.

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Language(s): eng - English
 Dates: 2021-03-022021-05-122021-05-212021-08-23
 Publication Status: Published in print
 Pages: 7
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/ange.202103102
 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
  Abbreviation : Angew. Chem.
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: 7 Volume / Issue: 133 (35) Sequence Number: - Start / End Page: 19318 - 19324 Identifier: ISSN: 0044-8249
CoNE: https://pure.mpg.de/cone/journals/resource/954926979058_1