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Leveraging material properties in fluorescence anion sensor arrays: A general approach

机译:利用荧光阴离子传感器阵列中的材料特性:通用方法

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As the demand for probes suitable for sensor development increases, investigation of approaches that utilize known successful receptors gains in general importance. This study describes a two-prong approach that can be used as a guide to developing sensors from known receptors. First, the conversion of a simple receptor, calix[4]pyrrole, into a fluorescent probe to establish a ratiometric signal is described. Secondly, the sensors that employ an output from a single ratiometric calix[4]pyrrole probe are fabricated by using poly(ether-urethane) hydrogel copolymers. These hydrogels are designed to absorb, internalize and transport aqueous electrolytes. A sensor array of ten different poly(ether-urethane) matrices with varying comonomer proportions were doped with a single probe and were exposed to eight different anions: acetate, benzoate, fluoride, chloride, phosphate, pyrophosphate, hydrogen sulfide, and cyanide, eight urine samples and anti-inflammatory drugs (NSAIDs). The poly(ether-urethane) matrices comprise different proportions of anion-binding urethane moieties and different hydrophilicity given by the ratio between ethylene glycol ether and butylene glycol ether. This diversity in the hydration behavior provides different environment polarity, in which the recognition and self-assembly processes display enough diverse behavior to allow for unique response of the probe to the analytes. Furthermore, a single probe is shown to recognize eight different aqueous anions and eight urine samples when embedded in ten different polyurethanes in an array that displays 100 % classification accuracy. To demonstrate the potential of the concept for quantitative studies, an estimation of non-steroidal anti-inflammatory drugs ibuprofen and diclofenac in water and in saliva was performed. A limit of detection of 0.1 ppm and a dynamic range of 0.1-0.6 and 0.05-60 ppm was observed, respectively. Given the general difficulty of chemosensors to recognize aqueous anions, the fact that one probe recognizes eight different analytes attests to an enormous effect of the polymer environment on the recognition process. This method could be used to generate a variety of sensor arrays for various analyses including species that are difficult to recognize, such as small-molecule- and inorganic anions. One for all, all for one: A single fluorescent probe is shown to recognize eight different aqueous anions and eight urine samples when embedded in ten different polyurethanes in an array that displays 100 % classification accuracy (see figure). To demonstrate the potential of the concept for quantitative studies, an estimation of non-steroidal anti-inflammatory drugs, ibuprofen and diclofenac, in water and in saliva was performed.
机译:随着对适合于传感器开发的探针的需求增加,利用已知成功的受体的方法的研究具有普遍的重要性。这项研究描述了两种方法,可以用作从已知受体开发传感器的指南。首先,描述了将简单的受体杯[4]吡咯转换为荧光探针以建立比例信号。其次,通过使用聚(醚-尿烷)水凝胶共聚物制造采用单个比率杯[4]吡咯探针的输出的传感器。这些水凝胶旨在吸收,内化和运输水性电解质。用单个探针对具有不同共聚单体比例的十种不同聚(醚-氨基甲酸酯)基质的传感器阵列进行掺杂,并使其暴露于八种不同的阴离子:乙酸根,苯甲酸根,氟离子,氯离子,磷酸根,焦磷酸根,硫化氢和氰化物中,八种尿液样本和抗炎药(NSAIDs)。聚(醚-氨基甲酸酯)基质包含不同比例的阴离子结合氨基甲酸酯部分和由乙二醇醚与丁二醇醚之间的比例给出的不同亲水性。水化行为的这种多样性提供了不同的环境极性,其中识别和自组装过程显示出足够多样的行为,以允许探针对分析物的独特响应。此外,显示了一个探针,当以阵列形式显示100%分类准确度时,可将十种不同的聚氨酯嵌入八种不同的含水阴离子和八种尿液样品。为了证明该概念在定量研究中的潜力,对水和唾液中非甾体抗炎药布洛芬和双氯芬酸进行了评估。分别观察到检测极限为0.1 ppm和动态范围为0.1-0.6和0.05-60 ppm。鉴于化学传感器通常难以识别水性阴离子,因此一个探针可识别八种不同分析物的事实证明了聚合物环境对识别过程的巨大影响。该方法可用于生成各种传感器阵列以用于各种分析,包括难以识别的物质,例如小分子阴离子和无机阴离子。一劳永逸:一枚荧光探针嵌入十种不同聚氨酯中,可识别八种不同的水性阴离子和八种尿液样品,它们的分类精度为100%(见图)。为了证明该概念在定量研究中的潜力,对水和唾液中的非甾体抗炎药布洛芬和双氯芬酸进行了评估。

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