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Vancomycin Determination by Disrupting Electron-Transfer in a Fluorescence Turn-On Squaraine–Anthraquinone Triad
ACS Sensors ( IF 8.2 ) Pub Date : 2018-05-24 00:00:00 , DOI: 10.1021/acssensors.8b00188
Shue Mei Ng 1 , Xiangyang Wu 1 , M. Faisal Khyasudeen 1 , Paweł J. Nowakowski 1 , Howe-Siang Tan 1 , Bengang Xing 1 , Edwin K. L. Yeow 1
Affiliation  

A highly sensitive and selective probe for Vancomycin (Van) in aqueous and serum samples is developed in this study. The probe is based on a triad consisting of a near-infrared squaraine dye (Seta-640) conjugated to two anthraquinone molecules via Lys-d-Ala-d-Ala peptides. In the absence of Van, the close proximity and efficient electron-transfer from the excited Seta-640 dye to anthraquinone result in significant fluorescence quenching of the dye (“off”-state). When Van is added, the antibiotic molecules bind with high affinity to the -d-Ala-d-Ala ligands in a 2:1 stoichiometry (Van:triad), resulting in fluorescence recovery that is as high as 30 times (“on”-state). Even though bound Van enhances the fluorescence by reducing the rate of (intrinsic) polarity-induced nonradiative decay process, this effect plays only a minor role. Instead, the main reason behind the observed fluorescence recovery after drug binding is the effective inhibition of electron-transfer; plausibly arising from a steric-induced lengthening of the spatial separation between electron donor and acceptor. The probe has detection limits of 7.0 and 96.9 nM in buffer and human serum, respectively, operates in the clinically relevant range, is insensitive to Van crystalline degradation product (CDP-1), and is easy to operate by using a commonly available fluorescence spectrometer.

中文翻译:

万古霉素的测定是通过破坏荧光开启的花氨酸-蒽醌三联体中的电子传递来进行的。

在这项研究中开发了一种高灵敏度和选择性的水溶液和血清样品中的万古霉素(Van)探针。探针是基于由近红外squaraine染料的三联体(濑-640)缀合于两个蒽醌分子经由赖氨酸- d -Ala- d -Ala肽。在没有Van的情况下,从激发的Seta-640染料到蒽醌的紧密接近和有效的电子转移导致该染料发生明显的荧光猝灭(“关闭”状态)。当加入Van时,抗生素分子与-d -Ala- d高亲和力结合-Ala配体的化学计量比为2:1(Van:triad),导致荧光回收率高达30倍(“接通”状态)。即使结合的Van通过降低(本征)极性诱导的非辐射衰变过程的速率来增强荧光,但这种作用仅起很小的作用。相反,药物结合后观察到的荧光恢复的主要原因是有效抑制了电子转移。可能是由于空间空间诱导的电子供体和受体之间空间间隔的延长而引起的。该探针在缓冲液和人血清中的检出限分别为7.0和96.9 nM,在临床相关范围内操作,对Van结晶降解产物(CDP-1)不敏感,并且易于使用常用的荧光光谱仪进行操作。
更新日期:2018-05-24
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