One-step growth of 3-5 nm diameter palladium electrocatalyst in a carbon nanoparticle-chitosan host and characterization for formic acid oxidation

Niancai Cheng, Richard A Webster, Mu Pan, Shichun Mu, Liza Rassaei, Shik Chi Tsang, Frank Marken

Research output: Contribution to journalArticle

27 Citations (Scopus)

Abstract

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.
Original languageEnglish
Pages (from-to)6601-6610
Number of pages10
JournalElectrochimica Acta
Volume55
Issue number22
DOIs
Publication statusPublished - 1 Sep 2010

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formic acid
Electrocatalysts
Formic acid
Chitosan
Palladium
Carbon
Nanoparticles
Oxidation
Catalysts
Bubble formation
Electrodes
Substrates
Catalyst activity
Buffers
Phosphates
Mass transfer
Hydrodynamics
Gases
Fluxes

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One-step growth of 3-5 nm diameter palladium electrocatalyst in a carbon nanoparticle-chitosan host and characterization for formic acid oxidation. / Cheng, Niancai; Webster, Richard A; Pan, Mu; Mu, Shichun; Rassaei, Liza; Tsang, Shik Chi; Marken, Frank.

In: Electrochimica Acta, Vol. 55, No. 22, 01.09.2010, p. 6601-6610.

Research output: Contribution to journalArticle

Cheng, Niancai ; Webster, Richard A ; Pan, Mu ; Mu, Shichun ; Rassaei, Liza ; Tsang, Shik Chi ; Marken, Frank. / One-step growth of 3-5 nm diameter palladium electrocatalyst in a carbon nanoparticle-chitosan host and characterization for formic acid oxidation. In: Electrochimica Acta. 2010 ; Vol. 55, No. 22. pp. 6601-6610.
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