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

Kunze, Sebastian; Grosse, Philipp; Bernal Lopez, Miguel; Sinev, Ilya; Zegkinoglou, Ioannis; Mistry, Hemma; Timoshenko, Janis; Hu, Michael Y.; Zhao, Jiyong; Alp, Ercan E.; Chee, See Wee; Roldan Cuenya, Beatriz

doi:10.1002/anie.202010535

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

Journal Article · Tue Oct 06 00:00:00 EDT 2020 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202010535· OSTI ID:1785375

^[1]; ^[1]; ^[2]; Sinev, Ilya ^[2]; ^[2]; Mistry, Hemma ^[2]; ^[3]; Hu, Michael Y. ^[4]; Zhao, Jiyong ^[4]; Alp, Ercan E. ^[4]; ^[3]; ^[3]

Ruhr Univ., Bochum (Germany); Fritz-Haber Institute of the Max Planck Society, Berlin (Germany)
Ruhr Univ., Bochum (Germany)
Fritz-Haber Institute of the Max Planck Society, Berlin (Germany)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Operando nuclear resonant inelastic X-ray scattering (NRIXS) and X-ray absorption fine-structure spectroscopy (XAFS) measurements were used to gain insight into the structure and surface composition of FeCu and FeAg nanoparticles (NPs) during the electrochemical CO₂ reduction (CO₂RR) and to extract correlations with their catalytic activity and selectivity. The formation of a core–shell structure during CO₂RR 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 KHCO₃ at -1.1 V vs. RHE, similar to that of pure Ag NPs. In contrast, a predominant selectivity towards H₂ 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 H₂ production.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: Deutsche Forschungsgemeinschaft (DFG); European Research Council (ERC); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1785375

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 50 Vol. 59; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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operando measurements

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

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