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Nanoscale structure dynamics within electrocatalytic materials
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Bentley, Cameron Luke, Kang, Minkyung and Unwin, Patrick R. (2017) Nanoscale structure dynamics within electrocatalytic materials. Journal of the American Chemical Society, 139 (46). pp. 16813-16821. doi:10.1021/jacs.7b09355 ISSN 1520-5126.
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Official URL: http://doi.org/10.1021/jacs.7b09355
Abstract
Electrochemical interfaces used for sensing, (electro)catalysis, and energy storage are usually nanostructured to expose particular surface sites, but probing the intrinsic activity of these sites is often beyond current experimental capability. Herein, it is demonstrated how a simple meniscus imaging probe of just 30 nm in size can be deployed for direct electrochemical and topographical imaging of electrocatalytic materials at the nanoscale. Spatially resolved topographical and electrochemical data are collected synchronously to create topographical images in which step-height features as small as 2 nm are easily resolved and potential-resolved electrochemical activity movies composed of hundreds of images are obtained in a matter of minutes. The technique has been benchmarked by investigating the hydrogen evolution reaction on molybdenum disulfide, where it is shown that the basal plane possesses uniform activity, while surface defects (i.e., few to multilayer step edges) give rise to a morphology-dependent (i.e., height-dependent) enhancement in catalytic activity. The technique was then used to investigate the electro-oxidation of hydrazine at the surface of electrodeposited Au nanoparticles (AuNPs) supported on glassy carbon, where subnanoentity (i.e., sub-AuNP) reactivity mapping has been demonstrated. We show, for the first time, that electrochemical reaction rates vary significantly across an individual AuNP surface and that these single entities cannot be considered as uniformly active. The work herein provides a road map for future studies in electrochemical science, in which the activity of nanostructured materials can be viewed as quantitative movies, readily obtained, to reveal active sites directly and unambiguously.
Item Type: | Journal Article | ||||||||||||
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Subjects: | Q Science > QD Chemistry | ||||||||||||
Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry | ||||||||||||
SWORD Depositor: | Library Publications Router | ||||||||||||
Library of Congress Subject Headings (LCSH): | Electrochemistry, Electrocatalysis , Scanning electrochemical microscopy, Nanoparticles | ||||||||||||
Journal or Publication Title: | Journal of the American Chemical Society | ||||||||||||
Publisher: | American Chemical Society (ACS) | ||||||||||||
ISSN: | 1520-5126 | ||||||||||||
Official Date: | 22 November 2017 | ||||||||||||
Dates: |
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Volume: | 139 | ||||||||||||
Number: | 46 | ||||||||||||
Page Range: | pp. 16813-16821 | ||||||||||||
DOI: | 10.1021/jacs.7b09355 | ||||||||||||
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: | 23 October 2018 | ||||||||||||
RIOXX Funder/Project Grant: |
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