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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 ISSN 1936-086X.
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Official URL: http://doi.org/10.1021/acsnano.7b05435
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 | ||||||||||||||||||
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| Subjects: | Q Science > QD Chemistry | ||||||||||||||||||
| Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry Faculty of Science, Engineering and Medicine > Research Centres > Molecular Organisation and Assembly in Cells (MOAC) Faculty of Science, Engineering and Medicine > Engineering > WMG (Formerly the Warwick Manufacturing Group) |
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| 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: |
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| 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 (Creative Commons) | ||||||||||||||||||
| Date of first compliant deposit: | 22 November 2017 | ||||||||||||||||||
| Date of first compliant Open Access: | 1 September 2018 | ||||||||||||||||||
| RIOXX Funder/Project Grant: |
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