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  Steering the structure and selectivity of CO2 electroreduction catalysts by potential pulses

Timoshenko, J., Bergmann, A., Rettenmaier, C., Herzog, A., Aran Ais, R., Jeon, H., et al. (2022). Steering the structure and selectivity of CO2 electroreduction catalysts by potential pulses. Nature Catalysis, 5(4), 259-267. doi:10.1038/s41929-022-00760-z.

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 Creators:
Timoshenko, Janis1, Author              
Bergmann, Arno1, Author              
Rettenmaier, Clara1, Author              
Herzog, Antonia1, Author              
Aran Ais, Rosa1, Author              
Jeon, Hyosang1, Author              
Haase, Felix1, Author              
Hejral, Uta1, Author              
Grosse, Philipp1, Author              
Kühl, Stefanie1, Author              
Davis, Earl1, Author              
Tian, Jing2, Author
Magnussen, Olaf2, Author
Roldan Cuenya, Beatriz1, Author              
Affiliations:
1Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              
2Institute of Experimental and Applied Physics, Kiel University, Kiel, Germany, ou_persistent22              

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 Abstract: Convoluted selectivity trends and a missing link between reaction product distribution and catalyst properties hinder practical applications of the electrochemical CO2 reduction reaction (CO2RR) for multicarbon product generation. Here we employ operando X-ray absorption and X-ray diffraction methods with subsecond time resolution to unveil the surprising complexity of catalysts exposed to dynamic reaction conditions. We show that by using a pulsed reaction protocol consisting of alternating working and oxidizing potential periods that dynamically perturb catalysts derived from Cu2O nanocubes, one can decouple the effect of the ensemble of coexisting copper species on the product distribution. In particular, an optimized dynamic balance between oxidized and reduced copper surface species achieved within a narrow range of cathodic and anodic pulse durations resulted in a twofold increase in ethanol production compared with static CO2RR conditions. This work thus prepares the ground for steering catalyst selectivity through dynamically controlled structural and chemical transformations.

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Language(s): eng - English
 Dates: 2021-07-052022-02-282022-04-21
 Publication Status: Published online
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1038/s41929-022-00760-z
 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: Nature Catalysis
  Abbreviation : Nat. Catal.
Source Genre: Journal
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Publ. Info: New York : Nature Publishing Group
Pages: 9 Volume / Issue: 5 (4) Sequence Number: - Start / End Page: 259 - 267 Identifier: ISSN: 25201158
CoNE: https://pure.mpg.de/cone/journals/resource/25201158