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Quantitative nanoscale visualization of heterogeneous electron transfer rates in 2D carbon nanotube networks
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Guell, Aleix G., Ebejer, Neil, Snowden, Michael E., McKelvey, Kim M. (Kim Martin), Macpherson, Julie V. and Unwin, Patrick R. (2012) Quantitative nanoscale visualization of heterogeneous electron transfer rates in 2D carbon nanotube networks. Proceedings of the National Academy of Sciences, Volume 109 (Number 29). pp. 11487-11492. doi:10.1073/pnas.1203671109 ISSN 0027-8424.
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Official URL: http://dx.doi.org/10.1073/pnas.1203671109
Abstract
Carbon nanotubes have attracted considerable interest for electrochemical, electrocatalytic, and sensing applications, yet there remains uncertainty concerning the intrinsic electrochemical (EC) activity. In this study, we use scanning electrochemical cell microscopy (SECCM) to determine local heterogeneous electron transfer
(HET) kinetics in a random 2D network of single-walled carbon nanotubes (SWNTs) on an Si∕SiO2 substrate. The high spatial resolution of SECCM, which employs a mobile nanoscale EC cell as a probe for imaging, enables us to sample the responses of individual portions of a wide range of SWNTs within this complex arrangement. Using two redox processes, the oxidation of ferrocenylmethyl trimethylammonium and the reduction of ruthenium (III)
hexaamine, we have obtained conclusive evidence for the high intrinsic EC activity of the sidewalls of the large majority of SWNTs in networks. Moreover, we show that the ends of SWNTs and the points where two SWNTs cross do not show appreciably different HET kinetics relative to the sidewall. Using finite element method
modeling, we deduce standard rate constants for the two redox couples and demonstrate that HET based solely on characteristic defects in the SWNT side wall is highly unlikely. This is further confirmed by the analysis of individual line profiles taken as the SECCM probe scans over an SWNT. More generally, the studies
herein demonstrate SECCM to be a powerful and versatile method for activity mapping of complex electrode materials under conditions of high mass transport, where kinetic assignments can be made with confidence.
| Item Type: | Journal Article | ||||
|---|---|---|---|---|---|
| Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry Faculty of Science, Engineering and Medicine > Research Centres > Molecular Organisation and Assembly in Cells (MOAC) |
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| Journal or Publication Title: | Proceedings of the National Academy of Sciences | ||||
| Publisher: | National Academy of Sciences | ||||
| ISSN: | 0027-8424 | ||||
| Official Date: | 17 July 2012 | ||||
| Dates: |
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| Volume: | Volume 109 | ||||
| Number: | Number 29 | ||||
| Page Range: | pp. 11487-11492 | ||||
| DOI: | 10.1073/pnas.1203671109 | ||||
| Status: | Peer Reviewed | ||||
| Publication Status: | Published | ||||
| Access rights to Published version: | Restricted or Subscription Access |
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