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Impact of surface chemistry on nanoparticle–electrode interactions in the electrochemical detection of nanoparticle collisions
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Chen, Chang-Hui, Ravenhill, Emma R., Momotenko, Dmitry, Kim, Yang-Rae, Lai, Stanley C. S. and Unwin, Patrick R. (2015) Impact of surface chemistry on nanoparticle–electrode interactions in the electrochemical detection of nanoparticle collisions. Langmuir, 31 (43). pp. 11932-11942. doi:10.1021/acs.langmuir.5b03033 ISSN 0743-7463.
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Official URL: http://dx.doi.org/10.1021/acs.langmuir.5b03033
Abstract
The electrochemical detection of a single nanoparticle (NP) at a support electrode can provide key information on surface chemistry and fundamental electron transfer (ET) properties at the nanoscale. This study employs scanning electrochemical cell microscopy (SECCM) as a fluidic device to both deliver individual citrate-capped gold nanoparticles (AuNPs) and study the interactions between them and a range of alkanethiol-modified Au electrodes with different terminal groups, namely, −COOH, −OH, and −CH3. Single NP collisions were detected through the AuNP-mediated ET reaction of Fe(CN)64–/3– in aqueous solution. The collision frequency, residence time, and current–time characteristics of AuNPs are greatly affected by the terminal groups of the alkanethiol. Methods to determine these parameters, including the effect of the instrument response function, and derive ET kinetics are outlined. To further understand the interactions of AuNPs with these surfaces, atomic force microscopy (AFM) force measurements were performed using citrate-modified Au-coated AFM tips and the same alkanethiol-modified Au substrates in aqueous solution at the same potential bias as for the AuNP collision experiments. Force curves on OH-terminated surfaces showed no repulsion and negligible adhesion force. In contrast, a clear repulsion (on approach) was seen for COOH-terminated surface and adhesion forces (on retract) were observed for both COOH- and CH3-terminated surfaces. These interactions help to explain the residence times and collision frequencies in AuNP collisions. More generally, as the interfacial properties probed by AFM appear to be amplified in NP collision experiments, and new features also become evident, it is suggested that such experiments provide a new means of probing surface chemistry at the nanoscale.
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): | Surface chemistry, Nanoparticles, Charge exchange, Nanochemistry, Electrochemistry | ||||||
Journal or Publication Title: | Langmuir | ||||||
Publisher: | American Chemical Society | ||||||
ISSN: | 0743-7463 | ||||||
Official Date: | 8 October 2015 | ||||||
Dates: |
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Volume: | 31 | ||||||
Number: | 43 | ||||||
Page Range: | pp. 11932-11942 | ||||||
DOI: | 10.1021/acs.langmuir.5b03033 | ||||||
Status: | Peer Reviewed | ||||||
Publication Status: | Published | ||||||
Date of first compliant deposit: | 26 January 2017 | ||||||
Date of first compliant Open Access: | 26 January 2017 | ||||||
Funder: | European Research Council (ERC), Marie Curie Intra-European Fellowship (IEF), University of Warwick Chancellor's Scholarship, Han'guk Haksul Chinhŭng Chaedan [Korea Research Foundation] (HHCC) | ||||||
Grant number: | ERC-2009-AdG 247143 QUANTIF (ERC), 275450 VISELCAT, 626158 FU NICIS (IEF), 2012R1A6A3A03039226 (HHCC) |
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