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Nucleation and aggregative growth of palladium nanoparticles on carbon electrodes : experiment and kinetic model
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Kim, Yang-Rae, Lai, Stanley Chi Shing, McKelvey, Kim M., Zhang, Guohui, Perry, David, Miller, Thomas S. and Unwin, Patrick R. (2015) Nucleation and aggregative growth of palladium nanoparticles on carbon electrodes : experiment and kinetic model. The Journal of Physical Chemistry C, 119 (30). pp. 17389-17397. doi:10.1021/acs.jpcc.5b03513
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Official URL: http://dx.doi.org/10.1021/acs.jpcc.5b03513
Abstract
The mechanism and kinetics of the electrochemical nucleation and growth of Pd nanoparticles (NPs) on carbon electrodes have been investigated using a microscale meniscus cell on both highly oriented pyrolytic graphite and a carbon coated transmission electron microscopy (TEM) grid. Using a microscale meniscus cell, it is possible to monitor the initial stage of electrodeposition electrochemically, while the ability to measure directly on a TEM grid allows subsequent high resolution microscopy characterization which provides detailed nanoscopic and kinetic information. TEM analysis clearly shows that Pd is electrodeposited in the form of NPs (approximately 1 − 2 nm diameter) that aggregate into extensive nanocrystal-type structures comprised of NPs. This gives rise to a high NP density. This mechanism is shown to be consistent with double potential step chronoamperometry measurements on HOPG, where a forward step generates electrodeposited Pd and the reverse step oxidizes the surface of the electrodeposited Pd to Pd oxide. The charge passed in these transients can be used to estimate the amounts of NPs electrodeposited and their size. Good agreement is found between the electrochemically determined parameters and the microscopy measurements. A model for electrodeposition based on the nucleation of NPs that aggregate to form stable structures is proposed that is used to analyze data and extract kinetics. This simple model reveals considerable information on the NP nucleation rate, the importance of aggregation in the deposition process and quantitative values for the aggregation rate.
| Item Type: | Journal Article | ||||||||||
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| Subjects: | Q Science > QD Chemistry | ||||||||||
| Divisions: | Faculty of Science > Chemistry Faculty of Science > Molecular Organisation and Assembly in Cells (MOAC) |
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| Library of Congress Subject Headings (LCSH): | Electrochemical analysis, Nanostructured materials | ||||||||||
| Journal or Publication Title: | The Journal of Physical Chemistry C | ||||||||||
| Publisher: | American Chemical Society | ||||||||||
| ISSN: | 1932-7447 | ||||||||||
| Official Date: | 30 July 2015 | ||||||||||
| Dates: |
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| Date of first compliant deposit: | 31 December 2015 | ||||||||||
| Volume: | 119 | ||||||||||
| Number: | 30 | ||||||||||
| Number of Pages: | 9 | ||||||||||
| Page Range: | pp. 17389-17397 | ||||||||||
| DOI: | 10.1021/acs.jpcc.5b03513 | ||||||||||
| Status: | Peer Reviewed | ||||||||||
| Publication Status: | Published | ||||||||||
| Access rights to Published version: | Restricted or Subscription Access | ||||||||||
| Funder: | European Research Council (ERC), National Research Foundation of Korea (NRF) | ||||||||||
| Grant number: | ERC- 2009-AdG 247143 QUANTIF (ERC), 2012R1A6A3A03039226 (NRF) | ||||||||||
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