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Structure and Chemical Reactivity of Y‐Stabilized ZrO 2 Surfaces: Importance for the Water‐Gas Shift Reaction

Chen, Shuang 1; Pleßow, Philipp N. ORCID iD icon 2; Yu, Zairan 1; Sauter, Eric 1; Caulfield, Lachlan 1; Nefedov, Alexei 1; Studt, Felix 2,3; Wang, Yuemin 1; Wöll, Christof 1
1 Institut für Funktionelle Grenzflächen (IFG), Karlsruher Institut für Technologie (KIT)
2 Institut für Katalyseforschung und -technologie (IKFT), Karlsruher Institut für Technologie (KIT)
3 Institut für Technische Chemie und Polymerchemie (ITCP), Karlsruher Institut für Technologie (KIT)

Abstract:

The surface structure and chemical properties of Y-stabilized zirconia (YSZ) have been subjects of intense debate over the past three decades. However, a thorough understanding of chemical processes occurring at YSZ powders faces significant challenges due to the absence of reliable reference data acquired for well-controlled model systems. Here, we present results from polarization-resolved infrared reflection absorption spectroscopy (IRRAS) obtained for differently oriented, Y-doped ZrO$_2$ single-crystal surfaces after exposure to CO and D$_2$O. The IRRAS data reveal that the polar YSZ(100) surface undergoes reconstruction, characterized by an unusual, red-shifted CO band at 2132 cm$^{−1}$. Density functional theory calculations allowed to relate this unexpected observation to under-coordinated Zr$^{4+}$ cations in the vicinity of doping-induced O vacancies. This reconstruction leads to a strongly increased chemical reactivity and water spontaneously dissociates on YSZ(100). The latter, which is an important requirement for catalysing the water-gas-shift (WGS) reaction, is absent for YSZ(111), where only associative adsorption was observed. ... mehr


Verlagsausgabe §
DOI: 10.5445/IR/1000171542
Veröffentlicht am 12.06.2024
Originalveröffentlichung
DOI: 10.1002/anie.202404775
Scopus
Zitationen: 2
Web of Science
Zitationen: 2
Dimensions
Zitationen: 2
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Funktionelle Grenzflächen (IFG)
Institut für Katalyseforschung und -technologie (IKFT)
Institut für Technische Chemie und Polymerchemie (ITCP)
Publikationstyp Zeitschriftenaufsatz
Publikationsjahr 2024
Sprache Englisch
Identifikator ISSN: 1433-7851, 0570-0833, 1521-3773
KITopen-ID: 1000171542
HGF-Programm 43.33.11 (POF IV, LK 01) Adaptive and Bioinstructive Materials Systems
Erschienen in Angewandte Chemie - International Edition
Verlag John Wiley and Sons
Band 63
Heft 27
Seiten e202404775
Vorab online veröffentlicht am 17.05.2024
Nachgewiesen in Scopus
Dimensions
Web of Science
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