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Mobility and poisoning of mass-selected platinum nanoclusters during the oxygen reduction reaction
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Ustarroz, Jon, Ornelas, Isabel, Zhang, Guohui, Perry, David, Kang, Minkyung, Bentley, Cameron Luke, Walker, Marc and Unwin, Patrick R. (2018) Mobility and poisoning of mass-selected platinum nanoclusters during the oxygen reduction reaction. ACS Catalysis, 8 (8). pp. 6775-6790. doi:10.1021/acscatal.8b00553 ISSN 2155-5435.
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WRAP-mobility-poisoning-mass-selected-platinum-nanoclusters-oxygen-reduction-reaction-Perry-2018.pdf - Accepted Version - Requires a PDF viewer. Download (2579Kb) | Preview |
Official URL: https://doi.org/10.1021/acscatal.8b00553
Abstract
A major challenge in electrocatalysis is to understand the impact of electrochemical processes on the physicochemical properties of nanoparticle or nanocluster (NC) ensembles, especially for complex processes, such as the oxygen reduction reaction (ORR) considered herein. We describe an approach whereby electrocatalysis at a small number of well-defined mass-selected Pt NCs (Pt923±37, diameter, d ≈ 3 nm) deposited from a cluster beam source on carbon-coated TEM grids, can be measured by a scanning electrochemical cell microscopy (SECCM) setup, in tandem with a range of complementary microscopy and spectroscopy techniques. The SECCM set up delivers high mass transport rates and allows the effects of transient reactive intermediates to be elucidated for different Pt surface coverage (NC spacing). A major observation is that the ORR activity decreases during successive electrochemical (voltammetric) measurements. This is shown to be due to poisoning of the Pt NCs by carbon/oxygen containing moieties that are produced by the reaction of reactive oxygen intermediates (RIs), generated by ORR, with the carbon support. The effect is most prominent when the Pt surface coverage on the carbon support is low (< 6%). Furthermore, the NC deposition impact energy affects drastically the resulting Pt NC stability during electrochemistry. For lower impact energy, Pt NCs migrate as a consequence of the ORR and are rearranged in characteristic groups on the support. This previously unseen effect is caused by an uneven flux distribution around individual NCs within the ensemble and has important consequences for understanding the stability and activity of NC and nanoparticle arrays.
| Item Type: | Journal Article | |||||||||||||||
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| Subjects: | Q Science > QD Chemistry | |||||||||||||||
| Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry Faculty of Science, Engineering and Medicine > Science > Physics |
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| Library of Congress Subject Headings (LCSH): | Electrocatalysis, Nanoparticles, Scanning electrochemical microscopy, Platinum catalysts, Oxidation-reduction reaction, Catalyst poisoning | |||||||||||||||
| Journal or Publication Title: | ACS Catalysis | |||||||||||||||
| Publisher: | American Chemical Society | |||||||||||||||
| ISSN: | 2155-5435 | |||||||||||||||
| Official Date: | 4 June 2018 | |||||||||||||||
| Dates: |
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| Volume: | 8 | |||||||||||||||
| Number: | 8 | |||||||||||||||
| Page Range: | pp. 6775-6790 | |||||||||||||||
| DOI: | 10.1021/acscatal.8b00553 | |||||||||||||||
| Status: | Peer Reviewed | |||||||||||||||
| Publication Status: | Published | |||||||||||||||
| Reuse Statement (publisher, data, author rights): | This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Catalysis, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acscatal.8b00553 | |||||||||||||||
| Access rights to Published version: | Restricted or Subscription Access | |||||||||||||||
| Date of first compliant deposit: | 8 October 2018 | |||||||||||||||
| Date of first compliant Open Access: | 4 June 2019 | |||||||||||||||
| RIOXX Funder/Project Grant: |
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