Effect of surface immobilization on the electrochemiluminescence of ruthenium-containing metallopolymers

L Dennany, C F Hogan, T E Keyes, R J Forster

Research output: Contribution to journalArticle

65 Citations (Scopus)

Abstract

The effect of surface confinement on the electrochemiluminescence (ECL) properties of metallopolymer [Ru(bpy)(2)(PVP)(10)](2+), where bpy is 2,2'-bipyridyl and PVP is poly(4-vinylpyridine), is reported. Immobilizing a luminescent material on an electrode surface can substantially modulate its photophysical properties. Significantly, our study revealed that the overall efficiency of the ECL reaction for the metallopolymer film is almost four times higher, at 0.15%, than the highest value obtained for [Ru(bpy)(2)(PVP)(10)](2+) dissolved in solution, (phi(ECL) = 0.04%). Electrochemistry has been used to create well-defined concentrations of the quencher Ru3+ within the film. Analysis of both the steady-state luminescence and lifetimes of the film reveals that static quenching by electron transfer between the photoexcited Ru2+* and the Ru3+ centers is the dominant quenching mechanism. The bimolecular rate of electron transfer is (2.5 +/- 0.4) x 10(6) M-1 s(-1). The implications of these findings for ECL-based sensors, in terms of optimum luminophore loading, is considered.

LanguageEnglish
Pages1412-1417
Number of pages6
JournalAnalytical Chemistry
Volume78
Issue number5
DOIs
Publication statusPublished - 1 Mar 2006

Fingerprint

Ruthenium
Quenching
2,2'-Dipyridyl
Electrons
Electrochemistry
Luminescence
Electrodes
Sensors
bis(bipyridyl)ruthenium(II)

Keywords

  • electrogenerated chemiluminescence
  • electron-transfer
  • ultrathin films
  • chemiluminescence
  • solvent
  • electrochemistry
  • complexes
  • dna

Cite this

Dennany, L ; Hogan, C F ; Keyes, T E ; Forster, R J . / Effect of surface immobilization on the electrochemiluminescence of ruthenium-containing metallopolymers. In: Analytical Chemistry. 2006 ; Vol. 78, No. 5. pp. 1412-1417.
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Effect of surface immobilization on the electrochemiluminescence of ruthenium-containing metallopolymers. / Dennany, L ; Hogan, C F ; Keyes, T E ; Forster, R J .

In: Analytical Chemistry, Vol. 78, No. 5, 01.03.2006, p. 1412-1417.

Research output: Contribution to journalArticle

TY - JOUR

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N2 - The effect of surface confinement on the electrochemiluminescence (ECL) properties of metallopolymer [Ru(bpy)(2)(PVP)(10)](2+), where bpy is 2,2'-bipyridyl and PVP is poly(4-vinylpyridine), is reported. Immobilizing a luminescent material on an electrode surface can substantially modulate its photophysical properties. Significantly, our study revealed that the overall efficiency of the ECL reaction for the metallopolymer film is almost four times higher, at 0.15%, than the highest value obtained for [Ru(bpy)(2)(PVP)(10)](2+) dissolved in solution, (phi(ECL) = 0.04%). Electrochemistry has been used to create well-defined concentrations of the quencher Ru3+ within the film. Analysis of both the steady-state luminescence and lifetimes of the film reveals that static quenching by electron transfer between the photoexcited Ru2+* and the Ru3+ centers is the dominant quenching mechanism. The bimolecular rate of electron transfer is (2.5 +/- 0.4) x 10(6) M-1 s(-1). The implications of these findings for ECL-based sensors, in terms of optimum luminophore loading, is considered.

AB - The effect of surface confinement on the electrochemiluminescence (ECL) properties of metallopolymer [Ru(bpy)(2)(PVP)(10)](2+), where bpy is 2,2'-bipyridyl and PVP is poly(4-vinylpyridine), is reported. Immobilizing a luminescent material on an electrode surface can substantially modulate its photophysical properties. Significantly, our study revealed that the overall efficiency of the ECL reaction for the metallopolymer film is almost four times higher, at 0.15%, than the highest value obtained for [Ru(bpy)(2)(PVP)(10)](2+) dissolved in solution, (phi(ECL) = 0.04%). Electrochemistry has been used to create well-defined concentrations of the quencher Ru3+ within the film. Analysis of both the steady-state luminescence and lifetimes of the film reveals that static quenching by electron transfer between the photoexcited Ru2+* and the Ru3+ centers is the dominant quenching mechanism. The bimolecular rate of electron transfer is (2.5 +/- 0.4) x 10(6) M-1 s(-1). The implications of these findings for ECL-based sensors, in terms of optimum luminophore loading, is considered.

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