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  Operando NRIXS and XAFS Investigation of Segregation Phenomena in Fe‐Cu and Fe‐Ag Nanoparticle Catalysts during CO2 Electroreduction

Kunze, S., Grosse, P., Lopez, M. B., Sinev, I., Zegkinoglou, I., Mistry, H., et al. (2020). Operando NRIXS and XAFS Investigation of Segregation Phenomena in Fe‐Cu and Fe‐Ag Nanoparticle Catalysts during CO2 Electroreduction. Angewandte Chemie International Edition, 59(50), 22667-22674. doi:10.1002/anie.202010535.

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 Creators:
Kunze, Sebastian1, 2, Author           
Grosse, Philipp1, 2, Author           
Lopez, Miguel Bernal1, Author
Sinev, Ilya1, Author
Zegkinoglou, Ioannis1, Author
Mistry, Hemma1, Author
Timoshenko, Janis2, Author           
Hu, Michael Y.3, Author
Zhao, Jiyong3, Author
Alp, Ercan E.3, Author
Chee, See Wee2, Author           
Roldan Cuenya, Beatriz2, Author           
Affiliations:
1Departement of Physics, Ruhr-University Bochum, 44780 Bochum, Germany, ou_persistent22              
2Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              
3Advanced Photon Source, Argonne National Laboratory, Chichago, USA, ou_persistent22              

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 Abstract: Operando nuclear resonant inelastic X‐ray scattering (NRIXS) and X‐ray absorption fine‐structure spectroscopy (XAFS) measurements have been used to gain insight into the structure and surface composition of FeCu and FeAg nanoparticles (NPs) during the CO 2 electrochemical reduction (CO 2 RR) and to extract correlations with their catalytic activity and selectivity. The formation of a core‐shell structure during CO 2 RR for FeAg NPs was inferred from the analysis of the operando NRIXS data (phonon density of states, PDOS) and XAFS measurements. Electrochemical analysis of the FeAg NPs revealed a faradaic selectivity of ~ 36 % for CO in 0.1 M KHCO 3 at ‐1.1 V vs RHE, similar to that of pure Ag NPs. In contrast, a predominant selectivity towards H 2 evolution is obtained in the case of the FeCu NPs, analogous to the results obtained for pure Fe NPs, although small Cu NPs have also been shown to favor H 2 production. These results, together with the findings from NRIXS and XAFS, revealed that Ag is preferentially present on the surface of the FeAg NPs during CO 2 RR, while Cu is also likely to be mainly distributed on the surface of the FeCu NPs but with a larger degree of intermixing with Fe.

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Language(s): eng - English
 Dates: 2020-08-012020-08-242020-10-062020-12-07
 Publication Status: Published in print
 Pages: 8
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/anie.202010535
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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: 8 Volume / Issue: 59 (50) Sequence Number: - Start / End Page: 22667 - 22674 Identifier: ISSN: 1433-7851
CoNE: https://pure.mpg.de/cone/journals/resource/1433-7851