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Simultaneous topography and reaction flux mapping at and around electrocatalytic nanoparticles

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Kang, Minkyung, Perry, David, Bentley, Cameron Luke, West, Geoffrey D., Page, Ashley M. and Unwin, Patrick R. (2017) Simultaneous topography and reaction flux mapping at and around electrocatalytic nanoparticles. ACS Nano, 11 (9). pp. 9525-9535. doi:10.1021/acsnano.7b05435

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Official URL: http://doi.org/10.1021/acsnano.7b05435

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Abstract

The characterization of electrocatalytic reactions at individual nanoparticles (NPs) is presently of considerable interest but very challenging. Herein, we demonstrate how simple-to-fabricate nanopipette probes with diameters of approximately 30 nm can be deployed in a scanning ion conductance microscopy (SICM) platform to simultaneously visualize electrochemical reactivity and topography with high spatial resolution at electrochemical interfaces. By employing a self-referencing hopping mode protocol, whereby the probe is brought from bulk solution to the near-surface at each pixel, and with potential-time control applied at the substrate, current measurements at the nanopipette can be made with high precision and resolution (30 nm resolution, 2600 pixels μm–2, <0.3 s pixel−1) to reveal a wealth of information on the substrate physicochemical properties. This methodology has been applied to image the electrocatalytic oxidation of borohydride at ensembles of AuNPs on a carbon fiber support in alkaline media, whereby the depletion of hydroxide ions and release of water during the reaction results in a detectable change in the ionic composition around the NPs. Through the use of finite element method simulations, these observations are validated and analyzed to reveal important information on heterogeneities in ion flux between the top of a NP and the gap at the NP-support contact, diffusional overlap and competition for reactant between neighboring NPs, and differences in NP activity. These studies highlight key issues that influence the behavior of NP assemblies at the single NP level and provide a platform for the use of SICM as an important tool for electrocatalysis studies.

Item Type: Journal Article
Subjects: Q Science > QD Chemistry
Divisions: Faculty of Science > Chemistry
Faculty of Science > Molecular Organisation and Assembly in Cells (MOAC)
Faculty of Science > WMG (Formerly the Warwick Manufacturing Group)
SWORD Depositor: Library Publications Router
Library of Congress Subject Headings (LCSH): Electrocatalysis, Nanoparticles
Journal or Publication Title: ACS Nano
Publisher: American Chemical Society (ACS)
ISSN: 1936-086X
Official Date: 26 September 2017
Dates:
DateEvent
26 September 2017Published
1 September 2017Available
1 September 2017Accepted
Date of first compliant deposit: 22 November 2017
Volume: 11
Number: 9
Page Range: pp. 9525-9535
DOI: 10.1021/acsnano.7b05435
Status: Peer Reviewed
Publication Status: Published
Access rights to Published version: Open Access
RIOXX Funder/Project Grant:
Project/Grant IDRIOXX Funder NameFunder ID
Chancellor’s International ScholarshipUniversity of Warwickhttp://dx.doi.org/10.13039/501100000741
UNSPECIFIEDLeverhulme Trusthttp://dx.doi.org/10.13039/501100000275
EP/F500378/1Engineering and Physical Sciences Research Councilhttp://dx.doi.org/10.13039/501100000266
702048 NEILH2020 Marie Skłodowska-Curie Actionshttp://dx.doi.org/10.13039/100010665
UNSPECIFIEDUniversity of Warwick. Molecular Organisation and Assembly in Cells (MOAC)UNSPECIFIED

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