Volume 11, Issue 7 p. 1405-1415

Article

Oscillatory behaviour in Galvanostatic Formaldehyde Oxidation on Nanostructured Pt/Glassy Carbon Model Electrodes

Yvonne E. Seidel,

Yvonne E. Seidel

[email protected]

Institute of Surface Chemistry and Catalysis, Ulm University, 89081 Ulm (Germany), Fax: (+49) 731-5025452

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Zenonas Jusys Dr.,

Zenonas Jusys Dr.

[email protected]

Institute of Surface Chemistry and Catalysis, Ulm University, 89081 Ulm (Germany), Fax: (+49) 731-5025452

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Rakel W. Lindström Dr.,

Rakel W. Lindström Dr.

Applied Electrochemistry, School of Chemical Science and Engineering, KTH (Royal Institute of Technology), S-10044 Stockholm (Sweden)

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Marie Stenfeldt Dr.,

Marie Stenfeldt Dr.

Dept. of Applied Physics, Chalmers University of Technology, S-41296 Gothenburg (Sweden)

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Bengt Kasemo Prof. Dr.,

Bengt Kasemo Prof. Dr.

Dept. of Applied Physics, Chalmers University of Technology, S-41296 Gothenburg (Sweden)

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Katharina Krischer Prof. Dr.,

Katharina Krischer Prof. Dr.

Physik-Department E19a, Technische Universität München, James-Franck-Str. 1,D-85748 Garching (Germany)

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Yvonne E. Seidel,

Yvonne E. Seidel

[email protected]

Institute of Surface Chemistry and Catalysis, Ulm University, 89081 Ulm (Germany), Fax: (+49) 731-5025452

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Zenonas Jusys Dr.,

Zenonas Jusys Dr.

[email protected]

Institute of Surface Chemistry and Catalysis, Ulm University, 89081 Ulm (Germany), Fax: (+49) 731-5025452

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Rakel W. Lindström Dr.,

Rakel W. Lindström Dr.

Applied Electrochemistry, School of Chemical Science and Engineering, KTH (Royal Institute of Technology), S-10044 Stockholm (Sweden)

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Marie Stenfeldt Dr.,

Marie Stenfeldt Dr.

Dept. of Applied Physics, Chalmers University of Technology, S-41296 Gothenburg (Sweden)

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Bengt Kasemo Prof. Dr.,

Bengt Kasemo Prof. Dr.

Dept. of Applied Physics, Chalmers University of Technology, S-41296 Gothenburg (Sweden)

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Katharina Krischer Prof. Dr.,

Katharina Krischer Prof. Dr.

Physik-Department E19a, Technische Universität München, James-Franck-Str. 1,D-85748 Garching (Germany)

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First published: 03 May 2010

https://doi.org/10.1002/cphc.200901029

Citations: 15

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Graphical Abstract

Collective behavior of individual oscillators: The electrocatalytic oxidation of formaldehyde is investigated. The picture shows time-resolved electrode potential/CO₂ current efficiency oscillatory maps during galvanostatic formaldehyde oxidation at different applied current densities over a Pt nanostructure array fabricated onto a planar glassy carbon substrate.

Abstract

The electrocatalytic oxidation of formaldehyde, which results in CO₂ and HCOOH formation, was investigated under galvanostatic conditions on nanostructured Pt/glassy carbon (GC) electrodes fabricated by employing colloidal lithography (CL). The measurements were performed on structurally well-defined model electrodes of different Pt surface coverages under different applied currents (current densities) and at constant electrolyte transport in a thin-layer flow cell connected to a differential electrochemical mass spectrometry (DEMS) setup to monitor the dynamic response of the reaction selectivity under these conditions. Periodic oscillations of the electrode potential and the CO₂ formation rate appear not only for a continuous Pt film, but also for the nanostructured Pt/GC electrodes when a critical current density is exceeded. The critical current density for achieving regular osillation patterns increased with decreasing Pt nanodisk density. Lower oscillation frequencies of the electrode potential and lower CO₂ formation rate for nanostructured Pt/GC electrodes compared to continuous Pt film at similar applied current densities suggest that transport processes play an essential role. Moreover, from the simple periodic response of the nanostructured electrodes it follows that all individual Pt disks in the array oscillate in synchrony. This result is discussed in terms of the different modes of spatial coupling present in the system: global coupling, migration coupling and mass transport of the essential chemical species, and the coverage of corresponding adsorbates.

Supporting Information

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Volume11, Issue7

Special Issue: Interface Phenomena

May 17, 2010

Pages 1405-1415

Oscillatory behaviour in Galvanostatic Formaldehyde Oxidation on Nanostructured Pt/Glassy Carbon Model Electrodes

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Abstract

Supporting Information

References

Citing Literature

References

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Oscillatory behaviour in Galvanostatic Formaldehyde Oxidation on Nanostructured Pt/Glassy Carbon Model Electrodes

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Abstract

Supporting Information

References

Citing Literature

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