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Nanoscale electrochemical patterning reveals the active sites for catechol oxidation at graphite surfaces
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Patel, Anisha N., McKelvey, Kim M. (Kim Martin) and Unwin, Patrick R. (2012) Nanoscale electrochemical patterning reveals the active sites for catechol oxidation at graphite surfaces. Journal of the American Chemical Society, Volume 134 (Number 50). pp. 20246-20249. doi:10.1021/ja3095894 ISSN 0002-7863.
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WRAP_Patel, JACS, 2012b.pdf - Accepted Version Download (1226Kb) | Preview |
Official URL: http://dx.doi.org/10.1021/ja3095894
Abstract
Graphite-based electrodes (graphite, graphene, and nanotubes) are used widely in electrochemistry, and there is a long-standing view that graphite step edges are needed to catalyze many reactions, with the basal surface considered to be inert. In the present work, this model was tested directly for the first time using scanning electrochemical cell microscopy reactive patterning and shown to be incorrect. For the electro-oxidation of dopamine as a model process, the reaction rate was measured at high spatial resolution across a surface of highly oriented pyrolytic graphite. Oxidation products left behind in a pattern defined by the scanned electrochemical cell served as surface-site markers, allowing the electrochemical activity to be correlated directly with the graphite structure on the nanoscale. This process produced tens of thousands of electrochemical measurements at different locations across the basal surface, unambiguously revealing it to be highly electrochemically active, with step edges providing no enhanced activity. This new model of graphite electrodes has significant implications for the design of carbon-based biosensors, and the results are additionally important for understanding electrochemical processes on related sp2-hybridized materials such as pristine graphene and nanotubes.
Item Type: | Journal Article | ||||
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Subjects: | Q Science > QD Chemistry | ||||
Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry | ||||
Library of Congress Subject Headings (LCSH): | Electrochemistry, High resolution electron microscopy, Electron microscopy, Graphite, Graphene | ||||
Journal or Publication Title: | Journal of the American Chemical Society | ||||
Publisher: | American Chemical Society | ||||
ISSN: | 0002-7863 | ||||
Official Date: | 2012 | ||||
Dates: |
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Volume: | Volume 134 | ||||
Number: | Number 50 | ||||
Page Range: | pp. 20246-20249 | ||||
DOI: | 10.1021/ja3095894 | ||||
Status: | Peer Reviewed | ||||
Publication Status: | Published | ||||
Access rights to Published version: | Restricted or Subscription Access | ||||
Date of first compliant deposit: | 23 December 2015 | ||||
Date of first compliant Open Access: | 23 December 2015 | ||||
Funder: | European Research Council (ERC), Engineering and Physical Sciences Research Council (EPSRC), University of Warwick. Molecular Organisation and Assembly in Cells, Birmingham Science City, Advantage West Midlands (AWM), European Regional Development Fund (ERDF) | ||||
Grant number: | ERC-2009-AdG247143 QUANTIF (ERC), EP/F064861/1e (EPSRC) |
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