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  On the Activity/Selectivity and Phase Stability of Thermally Grown Copper Oxides during the Electrocatalytic Reduction of CO2

Velasco Vélez, J., Chuang, C.-H., Gao, D., Zhu, Q., Ivanov, D., Jeon, H. S., et al. (2020). On the Activity/Selectivity and Phase Stability of Thermally Grown Copper Oxides during the Electrocatalytic Reduction of CO2. ACS Catalysis, 10(19), 11510-11518. doi:10.1021/acscatal.0c03484.

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Velasco Vélez, Juan1, 2, Author              
Chuang, Cheng-Hao3, Author
Gao, Dunfeng4, 5, Author              
Zhu, Qingjun1, 2, Author              
Ivanov, Danail2, Author              
Jeon, Hyo Sang5, Author
Arrigo, Rosa6, Author
Mom, Rik2, Author              
Stotz, Eugen2, Author              
Wu, Heng-Liang7, Author
Jones, Travis2, Author              
Roldan Cuenya, Beatriz4, Author              
Knop-Gericke, Axel1, 2, Author              
Schlögl, Robert1, 2, Author              
Affiliations:
1Department of Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion, Mülheim an der Ruhr 45470, Germany, ou_persistent22              
2Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
3Department of Physics, Tamkang University, New Taipei City 25137, Taiwan, ou_persistent22              
4Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              
5State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China, ou_persistent22              
6School of Sciences, University of Salford, Environment and Life, Cockcroft building, M5 4 WT, Manchester, U.K, ou_persistent22              
7Center for Condensed Matter Sciences, National Taiwan University, Taipei 10617, Taiwan, ou_persistent22              

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 Abstract: Revealing the active nature of oxide derived copper (OD-Cu) is of key importance to understand its remarkable catalytic performance during the cathodic CO2 reduction reaction (CO2RR) to produce valuable hydrocarbons. Using advanced spectroscopy, electron microscopy and electro active surface area characterization techniques, the electronic structure and the changes in the morphology/roughness of thermally oxidized copper thin films were revealed during CO2RR. For this purpose we developed an in situ cell for X-ray spectroscopy able to be operated accurately in the presence of gases or liquids to unite the role of the initial thermal oxide-phase and its active phase during the electrocatalytic reduction of CO2. It was found that the Cu(I) species formed during the thermal treatment are readily reduced to Cu0 during the CO2RR, whereas Cu(II) species are hardly reduced. In addition, Cu(II) oxide electrode dissolution was found to yield a porous/void structure, where the lack of electrical connection between isolated islands prohibits the CO2RR. Therefore, the active/stable phase for CO2RR is metallic copper, independent of its initial phase, with a significant change in its morphology upon its reduction yielding the formation of a rougher surface with higher number of under coordinated sites. Thus, the initial thermal oxidation of copper in air controls the reaction activity/selectivity due to the changes induced in electrode surface morphology/roughness and the presence of more under coordinated sites during the CO2RR.

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Language(s): eng - English
 Dates: 2020-08-102020-10-022020-10-02
 Publication Status: Published online
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acscatal.0c03484
 Degree: -

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Project name : OPERANDOCAT - In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects
Grant ID : 725291
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)

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Title: ACS Catalysis
  Abbreviation : ACS Catal.
Source Genre: Journal
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Publ. Info: Washington, DC : ACS
Pages: 9 Volume / Issue: 10 (19) Sequence Number: - Start / End Page: 11510 - 11518 Identifier: ISSN: 2155-5435
CoNE: https://pure.mpg.de/cone/journals/resource/2155-5435