Fluorescent and electrochemical sensing of (poly)phosphate nucleotides by ferrocene functionalised with two (ZnII-TACN-pyrene) complexes

Zeng, Zhanghua, Torriero, Angel A. J., Bond, Alan M. and Spiccia, Leone 2010, Fluorescent and electrochemical sensing of (poly)phosphate nucleotides by ferrocene functionalised with two (ZnII-TACN-pyrene) complexes, Chemistry - a European journal, vol. 16, no. 30, pp. 9154-9163, doi: 10.1002/chem.201000882.

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Title Fluorescent and electrochemical sensing of (poly)phosphate nucleotides by ferrocene functionalised with two (ZnII-TACN-pyrene) complexes
Author(s) Zeng, Zhanghua
Torriero, Angel A. J.ORCID iD for Torriero, Angel A. J. orcid.org/0000-0001-8616-365X
Bond, Alan M.
Spiccia, Leone
Journal name Chemistry - a European journal
Volume number 16
Issue number 30
Start page 9154
End page 9163
Total pages 10
Publisher Wiley - V C H Verlag GmbH & Co. KGaA
Place of publication Weinheim, Germany
Publication date 2010-08-09
ISSN 0947-6539
Summary The [Fc[BOND]bis{ZnII(TACN)(Py)}] complex, comprising two ZnII(TACN) ligands (Fc=ferrocene; Py=pyrene; TACN=1,4,7-triazacyclononane) bearing fluorescent pyrene chromophores linked by an electrochemically active ferrocene molecule has been synthesised in high yield through a multistep procedure. In the absence of the polyphosphate guest molecules, very weak excimer emission was observed, indicating that the two pyrene-bearing ZnII(TACN) units are arranged in a trans-like configuration with respect to the ferrocene bridging unit. Binding of a variety of polyphosphate anionic guests (PPi and nucleotides di- and triphosphate) promotes the interaction between pyrene units and results in an enhancement in excimer emission. Investigations of phosphate binding by 31P NMR spectroscopy, fluorescence and electrochemical techniques confirmed a 1:1 stoichiometry for the binding of PPi and nucleotide polyphosphate anions to the bis(ZnII(TACN)) moiety of [Fc[BOND]bis{ZnII(TACN)(Py)}] and indicated that binding induces a trans to cis configuration rearrangement of the bis(ZnII(TACN)) complexes that is responsible for the enhancement of the pyrene excimer emission. Pyrophosphate was concluded to have the strongest affinity to [Fc[BOND]bis{ZnII(TACN)(Py)}] among the anions tested based on a six-fold fluorescence enhancement and 0.1 V negative shift in the potential of the ferrocene/ferrocenium couple. The binding constant for a variety of polyphosphate anions was determined from the change in the intensity of pyrene excimer emission with polyphosphate concentration, measured at 475 nm in CH3CN/Tris-HCl (1:9) buffer solution (10.0 mM, pH 7.4). These measurements confirmed that pyrophosphate binds more strongly (Kb=(4.45±0.41)×106 M−1) than the other nucleotide di- and triphosphates (Kb=1–50×105 M−1) tested.
Language eng
DOI 10.1002/chem.201000882
Field of Research 030604 Electrochemistry
030102 Electroanalytical Chemistry
Socio Economic Objective 970103 Expanding Knowledge in the Chemical Sciences
HERDC Research category C1.1 Refereed article in a scholarly journal
Persistent URL http://hdl.handle.net/10536/DRO/DU:30038947

Document type: Journal Article
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