Improving the sensitivity of electrochemical sensors through a complementary luminescent mode: A new spectroelectrochemical approach
Improving the sensitivity of electrochemical sensors through a complementary luminescent mode: A new spectroelectrochemical approach
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DOI：
10.1016/j.snb.2018.10.093
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发表时间：
2019-04-01
影响因子：
8.4
通讯作者：
Basuray, Sagnik
中科院分区：
文献类型：
--
作者：
Chatterjee, Sayandev;Fujimoto, Meghan S.;Basuray, Sagnik
痕量和超痕量分析物的快速和灵敏的检测和定量对于环境修复、分析化学以及防御化学和生物污染物至关重要。尽管基于亲和性的电化学传感器已经获得了极大的普及，但是它们经常不满足期望的灵敏度和检测极限的要求。在这里，我们展示了一种互补发光模式，可以显着提高阻抗或伏安电化学传感器的灵敏度。我们的方法涉及使用氧化还原探针，其发光特性改变后，改变氧化态。通过定制系统，使得这些发光变化可以与目标分析物的捕获相关，与单独的电化学模式相比，我们能够显著降低检测限并提高检测效率。我们的概念验证演示，使用设计用于Ca 2+捕获的模型系统，说明发光模式使我们能够将检测限降低三个数量级，而不需要对电极设计或电池配置进行任何修改。此外，检测的线性范围在伏安法模式下为10（-8）至10（-3）M，在阻抗模式下为10（-8）至10（-5）M，在发光模式下为2.5x10（-11）至10（-7）M，提供了大范围的操作灵活性。
Rapid and sensitive detection and quantification of trace and ultra-trace analytes is critical to environmental remediation, analytical chemistry and defense from chemical and biological contaminants. Though affinity based electrochemical sensors have gained immense popularity, they frequently do not meet the requirements of desired sensitivity and detection limits. Here, we demonstrate a complementary luminescence mode that can significantly enhance sensitivity of impedance or voltammetric electrochemical sensors. Our methodology involves using a redox probe, whose luminescence properties change upon changing the oxidation state. By tailoring the system such that these luminescence changes can be correlated with the capture of target analytes, we are able to significantly lower the detection limit and improve the efficiency of detection compared to the electrochemical modes alone. Our proof-of-concept demonstration, using a model system designed for Ca2+ capture, illustrated that the luminescent mode allowed us to lower the limits of detection by three-orders of magnitude compared to the impedance or voltammetric modes alone without requiring any modification of electrode design or cell configuration. Further, the linear ranges of detection are 10(-8) to 10(-3) M in the voltammetry mode, 10(-8) to 10(-5) M in the impedance mode and 2.5x10(-11) to 10(-7) M in the luminescent mode, providing a large range of operational flexibility.