Ordered hydroxyls on Ca3Ru2O7(001)

Daniel Halwidl, Wernfried Mayr-Schmölzer, David Fobes, Jin Peng, Zhiqiang Mao, Michael Schmid, Florian Mittendorfer, Josef Redinger, Ulrike Diebold

Research output: Contribution to journalArticle

6 Citations (Scopus)

Abstract

As complex ternary perovskite-type oxides are increasingly used in solid oxide fuel cells, electrolysis and catalysis, it is desirable to obtain a better understanding of their surface chemical properties. Here we report a pronounced ordering of hydroxyls on the cleaved (001) surface of the Ruddlesden-Popper perovskite Ca3Ru2O7 upon water adsorption at 105 K and subsequent annealing to room temperature. Density functional theory calculations predict the dissociative adsorption of a single water molecule (E ads = 1.64 eV), forming an (OH)ads group adsorbed in a Ca-Ca bridge site, with an H transferred to a neighboring surface oxygen atom, Osurf. Scanning tunneling microscopy images show a pronounced ordering of the hydroxyls with (2 × 1), c(2 × 6), (1 × 3), and (1 × 1) periodicity. The present work demonstrates the importance of octahedral rotation and tilt in perovskites, for influencing surface reactivity, which here induces the ordering of the observed OH overlayers.

Original languageEnglish (US)
Article number23
JournalNature communications
Volume8
Issue number1
DOIs
StatePublished - Dec 1 2017

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Hydroxyl Radical
Oxides
Adsorption
Scanning Tunnelling Microscopy
Electrolysis
Surface Properties
Water
Periodicity
Catalysis
Oxygen
Temperature
adsorption
Scanning tunneling microscopy
electrolysis
perovskites
solid oxide fuel cells
Solid oxide fuel cells (SOFC)
chemical properties
Chemical properties
water

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Biochemistry, Genetics and Molecular Biology(all)
  • Physics and Astronomy(all)

Cite this

Halwidl, D., Mayr-Schmölzer, W., Fobes, D., Peng, J., Mao, Z., Schmid, M., ... Diebold, U. (2017). Ordered hydroxyls on Ca3Ru2O7(001). Nature communications, 8(1), [23]. https://doi.org/10.1038/s41467-017-00066-w
Halwidl, Daniel ; Mayr-Schmölzer, Wernfried ; Fobes, David ; Peng, Jin ; Mao, Zhiqiang ; Schmid, Michael ; Mittendorfer, Florian ; Redinger, Josef ; Diebold, Ulrike. / Ordered hydroxyls on Ca3Ru2O7(001). In: Nature communications. 2017 ; Vol. 8, No. 1.
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Halwidl, D, Mayr-Schmölzer, W, Fobes, D, Peng, J, Mao, Z, Schmid, M, Mittendorfer, F, Redinger, J & Diebold, U 2017, 'Ordered hydroxyls on Ca3Ru2O7(001)', Nature communications, vol. 8, no. 1, 23. https://doi.org/10.1038/s41467-017-00066-w

Ordered hydroxyls on Ca3Ru2O7(001). / Halwidl, Daniel; Mayr-Schmölzer, Wernfried; Fobes, David; Peng, Jin; Mao, Zhiqiang; Schmid, Michael; Mittendorfer, Florian; Redinger, Josef; Diebold, Ulrike.

In: Nature communications, Vol. 8, No. 1, 23, 01.12.2017.

Research output: Contribution to journalArticle

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AU - Halwidl, Daniel

AU - Mayr-Schmölzer, Wernfried

AU - Fobes, David

AU - Peng, Jin

AU - Mao, Zhiqiang

AU - Schmid, Michael

AU - Mittendorfer, Florian

AU - Redinger, Josef

AU - Diebold, Ulrike

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N2 - As complex ternary perovskite-type oxides are increasingly used in solid oxide fuel cells, electrolysis and catalysis, it is desirable to obtain a better understanding of their surface chemical properties. Here we report a pronounced ordering of hydroxyls on the cleaved (001) surface of the Ruddlesden-Popper perovskite Ca3Ru2O7 upon water adsorption at 105 K and subsequent annealing to room temperature. Density functional theory calculations predict the dissociative adsorption of a single water molecule (E ads = 1.64 eV), forming an (OH)ads group adsorbed in a Ca-Ca bridge site, with an H transferred to a neighboring surface oxygen atom, Osurf. Scanning tunneling microscopy images show a pronounced ordering of the hydroxyls with (2 × 1), c(2 × 6), (1 × 3), and (1 × 1) periodicity. The present work demonstrates the importance of octahedral rotation and tilt in perovskites, for influencing surface reactivity, which here induces the ordering of the observed OH overlayers.

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Halwidl D, Mayr-Schmölzer W, Fobes D, Peng J, Mao Z, Schmid M et al. Ordered hydroxyls on Ca3Ru2O7(001). Nature communications. 2017 Dec 1;8(1). 23. https://doi.org/10.1038/s41467-017-00066-w