Journal
ELECTROCHIMICA ACTA
Volume 55, Issue 22, Pages 6601-6610Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.electacta.2010.06.014
Keywords
Palladium nanoparticles; Chitosan; Carbon nanoparticles; Carbon dioxide; Nanocomposite; Formic acid; Fuel cell; Screen-printed electrode; Flow cell; Voltammetry; Buffer; Sensor
Categories
Funding
- CSC (China Scholarship Council) [2008695013]
- EPSRC [EP/F025726/1, EP/G03768X/1]
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The electrochemical formation of a palladium nanoparticle catalyst composite material has been investigated. A carbon nanoparticle-chitosan host film deposited onto a carbon substrate electrode has been employed to immobilize PdCl2 as catalyst precursor. A one-step electrochemical reduction process gave Pd nanoparticles within the chitosan matrix with different levels of loading, on different carbon substrates, and with a reproducible catalyst particle diameter of ca. 3-5 nm. High activity for formic acid oxidation has been observed in aqueous phosphate buffer medium. The oxidation of formic acid has been investigated as a function of pH and maximum catalyst activity was observed at pH 6. When varying the formic acid concentration, limiting behaviour consistent with a resistance effect has been observed. A flow cell system based on a screen-printed carbon electrode has been employed to establish the effect of hydrodynamic conditions on the formic acid oxidation. Both increasing the convective-diffusion mass transport rate and increasing the concentration of formic acid caused the oxidation peak current to converge towards the same resistance limit. A mechanistic model to explain the resistance effect based on CO2 flux and localized CO2 gas bubble formation at the Pd nanoparticle modified carbon nanoparticle-chitosan host film has been proposed. (C) 2010 Elsevier Ltd. All rights reserved.
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