Active-Phase Formation and Stability of Gd/Pt(111) Electrocatalysts for Oxygen Reduction: An In Situ Grazing Incidence X-Ray Diffraction Study

Maria Escudero Escribano, Anders Filsøe Pedersen, Elisabeth Therese Ulrikkeholm, Kim Degn Jensen, Martin H. Hansen, Jan Rossmeisl, Ifan E. L. Stephens, Ib Chorkendorff*

*Corresponding author for this work

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Abstract

Alloys of platinum and gadolinium present significant activity enhancement over pure Pt for the oxygen reduction reaction (ORR), both in the form of extended electrode surfaces and nanoparticulate catalysts. The active phase consists of a compressed Pt overlayer formed on Pt5Gd electrodes upon exposure to the electrolyte by acid leaching. Here, we investigate the formation, strain and correlation lengths of the active Pt overlayer by using in situ synchrotron grazing incidence X-ray diffraction on Gd/Pt(111) single-crystalline electrodes. The overlayer forms upon exposure to electrolyte under open circuit conditions; the compressive strain relaxes slightly upon repeated electrochemical cycling in the potential range 0.6 to 1.0 V versus the reversible hydrogen electrode (RHE). In addition, the strain relaxes strongly when exposing the electrode to 1.2 V versus RHE, and the thickness of the crystalline portion of the overlayer increases with potential above 1.3 V versus RHE.
Original languageEnglish
JournalChemistry: A European Journal
Volume24
Issue number47
Pages (from-to)12280-12290
Number of pages11
ISSN0947-6539
DOIs
Publication statusPublished - 2018

Cite this

Escribano, Maria Escudero ; Pedersen, Anders Filsøe ; Ulrikkeholm, Elisabeth Therese ; Jensen, Kim Degn ; Hansen, Martin H. ; Rossmeisl, Jan ; Stephens, Ifan E. L. ; Chorkendorff, Ib. / Active-Phase Formation and Stability of Gd/Pt(111) Electrocatalysts for Oxygen Reduction: An In Situ Grazing Incidence X-Ray Diffraction Study. In: Chemistry: A European Journal. 2018 ; Vol. 24, No. 47. pp. 12280-12290.
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abstract = "Alloys of platinum and gadolinium present significant activity enhancement over pure Pt for the oxygen reduction reaction (ORR), both in the form of extended electrode surfaces and nanoparticulate catalysts. The active phase consists of a compressed Pt overlayer formed on Pt5Gd electrodes upon exposure to the electrolyte by acid leaching. Here, we investigate the formation, strain and correlation lengths of the active Pt overlayer by using in situ synchrotron grazing incidence X-ray diffraction on Gd/Pt(111) single-crystalline electrodes. The overlayer forms upon exposure to electrolyte under open circuit conditions; the compressive strain relaxes slightly upon repeated electrochemical cycling in the potential range 0.6 to 1.0 V versus the reversible hydrogen electrode (RHE). In addition, the strain relaxes strongly when exposing the electrode to 1.2 V versus RHE, and the thickness of the crystalline portion of the overlayer increases with potential above 1.3 V versus RHE.",
author = "Escribano, {Maria Escudero} and Pedersen, {Anders Fils{\o}e} and Ulrikkeholm, {Elisabeth Therese} and Jensen, {Kim Degn} and Hansen, {Martin H.} and Jan Rossmeisl and Stephens, {Ifan E. L.} and Ib Chorkendorff",
year = "2018",
doi = "10.1002/chem.201801587",
language = "English",
volume = "24",
pages = "12280--12290",
journal = "Chemistry: A European Journal",
issn = "0947-6539",
publisher = "Wiley - V C H Verlag GmbH & Co. KGaA",
number = "47",

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Active-Phase Formation and Stability of Gd/Pt(111) Electrocatalysts for Oxygen Reduction: An In Situ Grazing Incidence X-Ray Diffraction Study. / Escribano, Maria Escudero; Pedersen, Anders Filsøe; Ulrikkeholm, Elisabeth Therese; Jensen, Kim Degn; Hansen, Martin H.; Rossmeisl, Jan; Stephens, Ifan E. L.; Chorkendorff, Ib.

In: Chemistry: A European Journal, Vol. 24, No. 47, 2018, p. 12280-12290.

Research output: Contribution to journalJournal articleResearchpeer-review

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T1 - Active-Phase Formation and Stability of Gd/Pt(111) Electrocatalysts for Oxygen Reduction: An In Situ Grazing Incidence X-Ray Diffraction Study

AU - Escribano, Maria Escudero

AU - Pedersen, Anders Filsøe

AU - Ulrikkeholm, Elisabeth Therese

AU - Jensen, Kim Degn

AU - Hansen, Martin H.

AU - Rossmeisl, Jan

AU - Stephens, Ifan E. L.

AU - Chorkendorff, Ib

PY - 2018

Y1 - 2018

N2 - Alloys of platinum and gadolinium present significant activity enhancement over pure Pt for the oxygen reduction reaction (ORR), both in the form of extended electrode surfaces and nanoparticulate catalysts. The active phase consists of a compressed Pt overlayer formed on Pt5Gd electrodes upon exposure to the electrolyte by acid leaching. Here, we investigate the formation, strain and correlation lengths of the active Pt overlayer by using in situ synchrotron grazing incidence X-ray diffraction on Gd/Pt(111) single-crystalline electrodes. The overlayer forms upon exposure to electrolyte under open circuit conditions; the compressive strain relaxes slightly upon repeated electrochemical cycling in the potential range 0.6 to 1.0 V versus the reversible hydrogen electrode (RHE). In addition, the strain relaxes strongly when exposing the electrode to 1.2 V versus RHE, and the thickness of the crystalline portion of the overlayer increases with potential above 1.3 V versus RHE.

AB - Alloys of platinum and gadolinium present significant activity enhancement over pure Pt for the oxygen reduction reaction (ORR), both in the form of extended electrode surfaces and nanoparticulate catalysts. The active phase consists of a compressed Pt overlayer formed on Pt5Gd electrodes upon exposure to the electrolyte by acid leaching. Here, we investigate the formation, strain and correlation lengths of the active Pt overlayer by using in situ synchrotron grazing incidence X-ray diffraction on Gd/Pt(111) single-crystalline electrodes. The overlayer forms upon exposure to electrolyte under open circuit conditions; the compressive strain relaxes slightly upon repeated electrochemical cycling in the potential range 0.6 to 1.0 V versus the reversible hydrogen electrode (RHE). In addition, the strain relaxes strongly when exposing the electrode to 1.2 V versus RHE, and the thickness of the crystalline portion of the overlayer increases with potential above 1.3 V versus RHE.

U2 - 10.1002/chem.201801587

DO - 10.1002/chem.201801587

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JO - Chemistry: A European Journal

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SN - 0947-6539

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