The effect of particle proximity on the oxygen reduction rate of size-selected platinum clusters

Markus Nesselberger; Melanie Röefzaad; R. Faycal Hamou; P. Ulrich Biedermann; Florian F. Schweinberger; Sebastian Kunz; Katrin Gabriele Hartl; Gustav Karl Henrik Wiberg; Sean James Ashton; Ueli Heiz; Karl Mayrhofer; Matthias Arenz

doi:10.1038/nmat3712

The effect of particle proximity on the oxygen reduction rate of size-selected platinum clusters

Markus Nesselberger, Melanie Röefzaad, R. Faycal Hamou, P. Ulrich Biedermann, Florian F. Schweinberger, Sebastian Kunz, Katrin Gabriele Hartl, Gustav Karl Henrik Wiberg, Sean James Ashton, Ueli Heiz, Karl Mayrhofer, Matthias Arenz

Department of Chemistry

237 Citations (Scopus)

Abstract

The diminished surface-area-normalized catalytic activity of highly dispersed Pt nanoparticles compared with bulk Pt is particularly intricate, and not yet understood. Here we report on the oxygen reduction reaction (ORR) activity of well-defined, size-selected Pt nanoclusters; a unique approach that allows precise control of both the cluster size and coverage, independently. Our investigations reveal that size-selected Pt nanoclusters can reach extraordinarily high ORR activities, especially in terms of mass-normalized activity, if deposited at high coverage on a glassy carbon substrate. It is observed that the Pt cluster coverage, and hence the interparticle distance, decisively influence the observed catalytic activity and that closely packed assemblies of Pt clusters approach the surface activity of bulk Pt. Our results open up new strategies for the design of catalyst materials that circumvent the detrimental dispersion effect, and may eventually allow the full electrocatalytic potential of Pt nanoclusters to be realized.

Original language	English
Journal	Nature Materials
Volume	12
Pages (from-to)	919-924
Number of pages	6
ISSN	1476-1122
DOIs	https://doi.org/10.1038/nmat3712
Publication status	Published - Oct 2013

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@article{d73e79ad9ff24cb9a88eb279a9cebc07,

title = "The effect of particle proximity on the oxygen reduction rate of size-selected platinum clusters",

abstract = "The diminished surface-area-normalized catalytic activity of highly dispersed Pt nanoparticles compared with bulk Pt is particularly intricate, and not yet understood. Here we report on the oxygen reduction reaction (ORR) activity of well-defined, size-selected Pt nanoclusters; a unique approach that allows precise control of both the cluster size and coverage, independently. Our investigations reveal that size-selected Pt nanoclusters can reach extraordinarily high ORR activities, especially in terms of mass-normalized activity, if deposited at high coverage on a glassy carbon substrate. It is observed that the Pt cluster coverage, and hence the interparticle distance, decisively influence the observed catalytic activity and that closely packed assemblies of Pt clusters approach the surface activity of bulk Pt. Our results open up new strategies for the design of catalyst materials that circumvent the detrimental dispersion effect, and may eventually allow the full electrocatalytic potential of Pt nanoclusters to be realized.",

author = "Markus Nesselberger and Melanie R{\"o}efzaad and Hamou, {R. Faycal} and Biedermann, {P. Ulrich} and Schweinberger, {Florian F.} and Sebastian Kunz and Hartl, {Katrin Gabriele} and Wiberg, {Gustav Karl Henrik} and Ashton, {Sean James} and Ueli Heiz and Karl Mayrhofer and Matthias Arenz",

year = "2013",

month = oct,

doi = "10.1038/nmat3712",

language = "English",

volume = "12",

pages = "919--924",

journal = "Nature Materials",

issn = "1476-1122",

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TY - JOUR

T1 - The effect of particle proximity on the oxygen reduction rate of size-selected platinum clusters

AU - Nesselberger, Markus

AU - Röefzaad, Melanie

AU - Hamou, R. Faycal

AU - Biedermann, P. Ulrich

AU - Schweinberger, Florian F.

AU - Kunz, Sebastian

AU - Hartl, Katrin Gabriele

AU - Wiberg, Gustav Karl Henrik

AU - Ashton, Sean James

AU - Heiz, Ueli

AU - Mayrhofer, Karl

AU - Arenz, Matthias

PY - 2013/10

Y1 - 2013/10

N2 - The diminished surface-area-normalized catalytic activity of highly dispersed Pt nanoparticles compared with bulk Pt is particularly intricate, and not yet understood. Here we report on the oxygen reduction reaction (ORR) activity of well-defined, size-selected Pt nanoclusters; a unique approach that allows precise control of both the cluster size and coverage, independently. Our investigations reveal that size-selected Pt nanoclusters can reach extraordinarily high ORR activities, especially in terms of mass-normalized activity, if deposited at high coverage on a glassy carbon substrate. It is observed that the Pt cluster coverage, and hence the interparticle distance, decisively influence the observed catalytic activity and that closely packed assemblies of Pt clusters approach the surface activity of bulk Pt. Our results open up new strategies for the design of catalyst materials that circumvent the detrimental dispersion effect, and may eventually allow the full electrocatalytic potential of Pt nanoclusters to be realized.

AB - The diminished surface-area-normalized catalytic activity of highly dispersed Pt nanoparticles compared with bulk Pt is particularly intricate, and not yet understood. Here we report on the oxygen reduction reaction (ORR) activity of well-defined, size-selected Pt nanoclusters; a unique approach that allows precise control of both the cluster size and coverage, independently. Our investigations reveal that size-selected Pt nanoclusters can reach extraordinarily high ORR activities, especially in terms of mass-normalized activity, if deposited at high coverage on a glassy carbon substrate. It is observed that the Pt cluster coverage, and hence the interparticle distance, decisively influence the observed catalytic activity and that closely packed assemblies of Pt clusters approach the surface activity of bulk Pt. Our results open up new strategies for the design of catalyst materials that circumvent the detrimental dispersion effect, and may eventually allow the full electrocatalytic potential of Pt nanoclusters to be realized.

U2 - 10.1038/nmat3712

DO - 10.1038/nmat3712

M3 - Journal article

SN - 1476-1122

VL - 12

SP - 919

EP - 924

JO - Nature Materials

JF - Nature Materials

ER -

The effect of particle proximity on the oxygen reduction rate of size-selected platinum clusters

Abstract

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