Skip to content Skip to navigation
University of Warwick
  • Study
  • |
  • Research
  • |
  • Business
  • |
  • Alumni
  • |
  • News
  • |
  • About

University of Warwick
Publications service & WRAP

Highlight your research

  • WRAP
    • Home
    • Search WRAP
    • Browse by Warwick Author
    • Browse WRAP by Year
    • Browse WRAP by Subject
    • Browse WRAP by Department
    • Browse WRAP by Funder
    • Browse Theses by Department
  • Publications Service
    • Home
    • Search Publications Service
    • Browse by Warwick Author
    • Browse Publications service by Year
    • Browse Publications service by Subject
    • Browse Publications service by Department
    • Browse Publications service by Funder
  • Help & Advice
University of Warwick

The Library

  • Login
  • Admin

Mobility and poisoning of mass-selected platinum nanoclusters during the oxygen reduction reaction

Tools
- Tools
+ Tools

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.

[img]
Preview
PDF
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

Request Changes to record.

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
Subjects: Q Science > QD Chemistry
Divisions: Faculty of Science, Engineering and Medicine > Science > Chemistry
Faculty of Science, Engineering and Medicine > Science > Physics
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:
DateEvent
4 June 2018Published
4 June 2018Accepted
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:
Project/Grant IDRIOXX Funder NameFunder ID
12I7816NFonds Wetenschappelijk Onderzoekhttp://dx.doi.org/10.13039/501100003130
Wolfson Research Merit Award[RS] Royal Societyhttp://dx.doi.org/10.13039/501100000288
UNSPECIFIEDLeverhulme Trusthttp://dx.doi.org/10.13039/501100000275
Chancellor’s International ScholarshipUniversity of Warwickhttp://dx.doi.org/10.13039/501100000741

Request changes or add full text files to a record

Repository staff actions (login required)

View Item View Item

Downloads

Downloads per month over past year

View more statistics

twitter

Email us: wrap@warwick.ac.uk
Contact Details
About Us