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Label-Free Single-Molecule Electrical Sensor for Ultrasensitive and Selective Detection of Iodide Ions in Human Urine

ACS Sensors(2024)SCI 1区SCI 2区

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Abstract
Herein, a label-free single-molecule electrical sensor was first proposed for the ultrasensitive and selective detection of iodide ions in human urine. Single-molecule conductance measurements in different halogen ion solutions via scanning tunneling microscopy break junction (STM-BJ) clearly revealed that I- ions strongly affect the stability and displacement distance (Delta z) distribution of molecular junctions. Theoretical calculations prove that the specific adsorption of I- ions modifies the surface properties and weakens the molecular adsorption. Furthermore, the average conductance peak area versus the logarithm of the I- ion concentration has a very good linear relationship in the range of 5 x 10(-6) to 5 x 10(-10) M, with a correlation coefficient of 0.99. This quantitative analysis remains valid in the presence of interfering ions of SO42-, ClO4-, Br-, and Cl- as well as interfering molecules of ascorbic acid, uric acid, dopamine, and cysteine. A cross-comparison of the human urine detection results of this single-molecule electrical sensor with those of the clinical method of As3+-Ce4+ catalytic spectrophotometry revealed an average difference of 0.9%, which decreased the detection time of 2 h with the traditional method to approximately 15 min. This work proves the promising practical potential of the single-molecule electrical technique for relevant clinical analysis.
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single-molecule electrical sensor,scanning tunnelingmicroscopy break junction,molecular junctions,iodide ions detection,human urine
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要点】:本文首次提出了一种无标记的单分子电传感器,用于高灵敏度和高选择性地检测人尿中的碘离子。

方法】:通过扫描隧道显微镜断裂结(STM-BJ)技术在不同卤素离子溶液中进行单分子电导测量,并结合理论计算研究碘离子对分子连接稳定性和位移距离分布的影响。

实验】:实验在含有不同浓度碘离子的溶液中进行,使用的数据集为实验测得的电导峰值面积与碘离子浓度对数的线性关系,结果显示在5 x 10^(-6)到5 x 10^(-10) M范围内具有良好的线性关系,相关系数为0.99。在干扰离子和干扰分子存在的情况下,该定量分析依然有效。通过与临床方法As3+-Ce4+催化光谱法的检测结果进行交叉比较,该单分子电传感器在人尿检测中的平均差异为0.9%,并将检测时间从传统方法的2小时缩短至约15分钟。