A high stability AuPd-ZrO2-multiwall carbon nanotubes supported-catalyst in a formic acid electro-oxidation reaction

B. Lesiak, A. Malolepszy, M. Mazurkiewicz-Pawlicka, L. Stobinski, L. Kövér, J. Tóth, B. Mierzwa, G. Trykowski

Research output: Contribution to journalArticle

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Abstract

Catalytic activity and stability in a formic acid electro-oxidation, chemical and structural properties of AuPd nanoparticles deposited (a polyol method) on ZrO2 decorated functionalised multiwall carbon nanotubes (f-MWCNTs) (a hydrothermal method) were investigated using a fuel cell test, scanning transmission electron microscopy (STEM), high resolution transmission electron microscopy (HR-TEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). Non-stoichiometric ZrOx nanoparticles of a cubic phase (C-phase) and average size of 5–10 nm (STEM, HR-TEM), 4.5–5.0 nm (XRD) are anchored by f-MWCNTs carboxylic group through Zr-O-C bonds. Decoration by AuPd nanoparticles leads to ternary Pd/AuPd/Au phase of 6.9 nm crystallite size (XRD) with metallic Pd, oxidised (PdO, PdO2) and Pd-O-Zr phases (XPS). Oxidation/reduction at 300 °C/200 °C leads to nanoparticles sintering, increasing/decreasing Pd surface coverage, oxides/oxygen groups content and ZrOx stoichiometry. Catalysts after oxidation (the largest nanoparticle size, Pd oxides content, ZrOx stoichiometry) showed the highest activity and stability. Activity of AuPd-ZrO2/f-MWCNTs catalysts is smaller than that of these catalysts without ZrO2, however, the stability is remarkably larger, i.e. AuPd-ZrO2/f-MWCNTs > Pd-ZrO2/f-MWCNTs > AuPd/f-MWCNTs > Pd/f-MWCNTs, what is attributed to electronic properties of AuPd and role of ZrOx and oxygen functional groups in COad desorption and oxidation to CO2 releasing catalyst active sites.

Original languageEnglish
Pages (from-to)289-297
Number of pages9
JournalApplied Surface Science
Volume451
DOIs
Publication statusPublished - Sep 1 2018

Fingerprint

formic acid
Carbon Nanotubes
Electrooxidation
Formic acid
Catalyst supports
Carbon nanotubes
Nanoparticles
Catalysts
High resolution transmission electron microscopy
X ray diffraction
Stoichiometry
Oxides
X ray photoelectron spectroscopy
Oxygen
Transmission electron microscopy
Oxidation
Scanning electron microscopy
Polyols
Crystallite size
Electronic properties

Keywords

  • Anode side
  • AuPd-ZrO/f-MWCNTs
  • Formic acid electro-oxidation in fuel cell
  • STEM/HR-TEM
  • XPS
  • XRD

ASJC Scopus subject areas

  • Surfaces, Coatings and Films

Cite this

A high stability AuPd-ZrO2-multiwall carbon nanotubes supported-catalyst in a formic acid electro-oxidation reaction. / Lesiak, B.; Malolepszy, A.; Mazurkiewicz-Pawlicka, M.; Stobinski, L.; Kövér, L.; Tóth, J.; Mierzwa, B.; Trykowski, G.

In: Applied Surface Science, Vol. 451, 01.09.2018, p. 289-297.

Research output: Contribution to journalArticle

Lesiak, B, Malolepszy, A, Mazurkiewicz-Pawlicka, M, Stobinski, L, Kövér, L, Tóth, J, Mierzwa, B & Trykowski, G 2018, 'A high stability AuPd-ZrO2-multiwall carbon nanotubes supported-catalyst in a formic acid electro-oxidation reaction', Applied Surface Science, vol. 451, pp. 289-297. https://doi.org/10.1016/j.apsusc.2018.04.233
Lesiak, B. ; Malolepszy, A. ; Mazurkiewicz-Pawlicka, M. ; Stobinski, L. ; Kövér, L. ; Tóth, J. ; Mierzwa, B. ; Trykowski, G. / A high stability AuPd-ZrO2-multiwall carbon nanotubes supported-catalyst in a formic acid electro-oxidation reaction. In: Applied Surface Science. 2018 ; Vol. 451. pp. 289-297.
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abstract = "Catalytic activity and stability in a formic acid electro-oxidation, chemical and structural properties of AuPd nanoparticles deposited (a polyol method) on ZrO2 decorated functionalised multiwall carbon nanotubes (f-MWCNTs) (a hydrothermal method) were investigated using a fuel cell test, scanning transmission electron microscopy (STEM), high resolution transmission electron microscopy (HR-TEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). Non-stoichiometric ZrOx nanoparticles of a cubic phase (C-phase) and average size of 5–10 nm (STEM, HR-TEM), 4.5–5.0 nm (XRD) are anchored by f-MWCNTs carboxylic group through Zr-O-C bonds. Decoration by AuPd nanoparticles leads to ternary Pd/AuPd/Au phase of 6.9 nm crystallite size (XRD) with metallic Pd, oxidised (PdO, PdO2) and Pd-O-Zr phases (XPS). Oxidation/reduction at 300 °C/200 °C leads to nanoparticles sintering, increasing/decreasing Pd surface coverage, oxides/oxygen groups content and ZrOx stoichiometry. Catalysts after oxidation (the largest nanoparticle size, Pd oxides content, ZrOx stoichiometry) showed the highest activity and stability. Activity of AuPd-ZrO2/f-MWCNTs catalysts is smaller than that of these catalysts without ZrO2, however, the stability is remarkably larger, i.e. AuPd-ZrO2/f-MWCNTs > Pd-ZrO2/f-MWCNTs > AuPd/f-MWCNTs > Pd/f-MWCNTs, what is attributed to electronic properties of AuPd and role of ZrOx and oxygen functional groups in COad desorption and oxidation to CO2 releasing catalyst active sites.",
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AU - Malolepszy, A.

AU - Mazurkiewicz-Pawlicka, M.

AU - Stobinski, L.

AU - Kövér, L.

AU - Tóth, J.

AU - Mierzwa, B.

AU - Trykowski, G.

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AB - Catalytic activity and stability in a formic acid electro-oxidation, chemical and structural properties of AuPd nanoparticles deposited (a polyol method) on ZrO2 decorated functionalised multiwall carbon nanotubes (f-MWCNTs) (a hydrothermal method) were investigated using a fuel cell test, scanning transmission electron microscopy (STEM), high resolution transmission electron microscopy (HR-TEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). Non-stoichiometric ZrOx nanoparticles of a cubic phase (C-phase) and average size of 5–10 nm (STEM, HR-TEM), 4.5–5.0 nm (XRD) are anchored by f-MWCNTs carboxylic group through Zr-O-C bonds. Decoration by AuPd nanoparticles leads to ternary Pd/AuPd/Au phase of 6.9 nm crystallite size (XRD) with metallic Pd, oxidised (PdO, PdO2) and Pd-O-Zr phases (XPS). Oxidation/reduction at 300 °C/200 °C leads to nanoparticles sintering, increasing/decreasing Pd surface coverage, oxides/oxygen groups content and ZrOx stoichiometry. Catalysts after oxidation (the largest nanoparticle size, Pd oxides content, ZrOx stoichiometry) showed the highest activity and stability. Activity of AuPd-ZrO2/f-MWCNTs catalysts is smaller than that of these catalysts without ZrO2, however, the stability is remarkably larger, i.e. AuPd-ZrO2/f-MWCNTs > Pd-ZrO2/f-MWCNTs > AuPd/f-MWCNTs > Pd/f-MWCNTs, what is attributed to electronic properties of AuPd and role of ZrOx and oxygen functional groups in COad desorption and oxidation to CO2 releasing catalyst active sites.

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