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  Enhanced Formic Acid Oxidation over SnO2-decorated Pd Nanocubes

Rettenmaier, C., Aran Ais, R., Timoshenko, J., Rizo, R., Jeon, H., Kühl, S., et al. (2020). Enhanced Formic Acid Oxidation over SnO2-decorated Pd Nanocubes. ACS Catalysis, 10(24), 14540-14551. doi:10.1021/acscatal.0c03212.

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acscatal.0c03212.pdf (Verlagsversion), 5MB
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2020
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 Urheber:
Rettenmaier, Clara1, Autor           
Aran Ais, Rosa1, Autor           
Timoshenko, Janis1, Autor           
Rizo, Ruben1, Autor           
Jeon, Hyosang1, Autor           
Kühl, Stefanie1, Autor           
Chee, See Wee1, Autor           
Bergmann, Arno1, Autor           
Roldan Cuenya, Beatriz1, Autor           
Affiliations:
1Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              

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 Zusammenfassung: The formic acid oxidation reaction (FAOR) is one of the key reactions that can be used at the anode of low-temperature liquid fuel cells. To allow the knowledge-driven development of improved catalysts, it is necessary to deeply understand the fundamental aspects of the FAOR, which can be ideally achieved by investigating highly active model catalysts. Here, we studied SnO2-decorated Pd nanocubes (NCs) exhibiting excellent electrocatalytic performance for formic acid oxidation in acidic medium with a SnO2 promotion that boosts the catalytic activity by a factor of 5.8, compared to pure Pd NCs, exhibiting values of 2.46 A mg–1Pd for SnO2@Pd NCs versus 0.42 A mg–1Pd for the Pd NCs and a 100 mV lower peak potential. By using ex situ, quasi in situ, and operando spectroscopic and microscopic methods (namely, transmission electron microscopy, X-ray photoelectron spectroscopy, and X-ray absorption fine-structure spectroscopy), we identified that the initially well-defined SnO2-decorated Pd nanocubes maintain their structure and composition throughout FAOR. In situ Fourier-transformed infrared spectroscopy revealed a weaker CO adsorption site in the case of the SnO2-decorated Pd NCs, compared to the monometallic Pd NCs, enabling a bifunctional reaction mechanism. Therein, SnO2 provides oxygen species to the Pd surface at low overpotentials, promoting the oxidation of the poisoning CO intermediate and, thus, improving the catalytic performance of Pd. Our SnOx-decorated Pd nanocubes allowed deeper insight into the mechanism of FAOR and hold promise for possible applications in direct formic acid fuel cells.

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Sprache(n): eng - English
 Datum: 2020-10-232020-07-232020-12-18
 Publikationsstatus: Online veröffentlicht
 Seiten: 12
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1021/acscatal.0c03212
 Art des Abschluß: -

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Projektname : OPERANDOCAT - In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects
Grant ID : 725915
Förderprogramm : Horizon 2020 (H2020)
Förderorganisation : European Commission (EC)

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Titel: ACS Catalysis
  Kurztitel : ACS Catal.
Genre der Quelle: Zeitschrift
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Affiliations:
Ort, Verlag, Ausgabe: Washington, DC : ACS
Seiten: 12 Band / Heft: 10 (24) Artikelnummer: - Start- / Endseite: 14540 - 14551 Identifikator: ISSN: 2155-5435
CoNE: https://pure.mpg.de/cone/journals/resource/2155-5435