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首页> 外文期刊>Chemistry: A European journal >Fluorescent and electrochemical sensing of polyphosphate nucleotides by ferrocene functionalised with two Zn~(II)(TACN)(pyrene) complexes
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Fluorescent and electrochemical sensing of polyphosphate nucleotides by ferrocene functionalised with two Zn~(II)(TACN)(pyrene) complexes

机译：用两个Zn〜（II）（TACN）（py）配合物官能化的二茂铁对聚磷酸核苷酸的荧光和电化学传感

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摘要

The [Fc-bis{Zn~(II)(TACN)-(Py)}] complex, comprising two Zn ~(II)-(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 pyrenebearing Zn~(II)(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 diand triphosphate) promotes the interaction between pyrene units and results in an enhancement in excimer emission. Investigations of phosphate binding by~(31)P NMR spectroscopy, fluorescence and electrochemical techniques confirmed a 1:1 stoichiometry for the binding of PPi and nucleotide polyphosphate anions to the bis(Zn~(II)-(TACN)) moiety of [Fc-bis{Zn~(II)-(TACN)(Py)}] and indicated that binding induces a trans to cis configuration rearrangement of the bis(Zn~(II)(TACN)) complexes that is responsible for the enhancement of the pyrene excimer emission. Pyrophosphate was concluded to have the strongest affinity to [Fc-bis{Zn~(II)(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 CH _3CN/Tris-HCl (1:9) buffer solution (10.0 mm, pH 7.4). These measurements confirmed that pyrophosphate binds more strongly (K_b = (4.45 ± 0.41)×10~6M~(-1)) than the other nucleotide di-and triphosphates (K~b = 1-50× 10~5 M~(-1)) tested.
机译：[Fc-bis {Zn〜（II）（TACN）-（Py）}]络合物，包含两个Zn〜（II）-（TACN）配体（Fc =二茂铁; Py = ;; TACN = 1,4,7已经通过多步骤程序以高收率合成了带有由电化学活性二茂铁分子连接的带有荧光pyr发色团的-三氮杂环壬烷）。在不存在多磷酸盐客体分子的情况下，观察到非常弱的准分子发射，表明两个pyr基的Zn（II）（TACN）单元相对于二茂铁桥联单元以反型构型排列。各种多磷酸盐阴离子客体（PPi和核苷酸二磷酸三磷酸酯）的结合促进pyr单元之间的相互作用，并导致受激准分子发射的增强。通过〜（31）P NMR光谱，荧光和电化学技术对磷酸盐结合的研究证实了PPi和核苷酸多磷酸根阴离子与[Fc]的双（Zn〜（II）-（TACN））部分结合的1：1化学计量。 -bis {Zn〜（II）-（TACN）（Py）}]，并指出结合诱导了bis（Zn〜（II）（TACN））配合物的反式至顺式构型重排，这是导致双（Zn〜（II）（TACN）（Py）} exc准分子发射。基于二茂铁电位的六倍荧光增强和0.1 V负移，得出结论，焦磷酸对[Fc-bis {Zn〜（II）（TACN）（Py）}]具有最强的亲和力/ ferrocenium夫妇。在CH _3CN / Tris-HCl（1：9）缓冲溶液（10.0 mm，pH 7.4）中于475 nm下测得的of准分子发射强度随多磷酸盐浓度的变化确定了各种多磷酸盐阴离子的结合常数。 。这些测量结果证实焦磷酸盐与其他核苷酸二磷酸和三磷酸核苷酸（K〜b = 1-50×10〜5 M〜（-）的结合更牢固（K_b =（4.45±0.41）×10〜6M〜（-1））。 1））经过测试。

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