Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Institute of Physical Chemistry, College of Chemistry and Materials Science, Zhejiang Normal University, Jinhua 321004, China.
ACS Sens. 2024 Oct 25;9(10):5578-5586. doi: 10.1021/acssensors.4c02025. Epub 2024 Oct 16.
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 (Δ) 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 × 10 to 5 × 10 M, with a correlation coefficient of 0.99. This quantitative analysis remains valid in the presence of interfering ions of SO, ClO, 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 As-Ce 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.
本文首次提出了一种无标记的单分子电学传感器,用于在人体尿液中对碘离子进行超灵敏和选择性检测。通过扫描隧道显微镜断键(STM-BJ)在不同卤离子溶液中单分子电导测量清楚地表明,I 离子强烈影响分子结的稳定性和位移距离(Δ)分布。理论计算证明,I 离子的特异性吸附改变了表面性质并减弱了分子吸附。此外,在 5×10 到 5×10 M 的范围内,平均电导峰面积与 I 离子浓度的对数具有非常好的线性关系,相关系数为 0.99。这种定量分析在存在 SO、ClO、Br 和 Cl 等干扰离子以及抗坏血酸、尿酸、多巴胺和半胱氨酸等干扰分子的情况下仍然有效。与临床的 As-Ce 催化分光光度法相比,这种单分子电学传感器对人体尿液检测结果的交叉比较显示平均差异为 0.9%,将传统方法的检测时间从 2 小时缩短到了约 15 分钟。这项工作证明了单分子电学技术在相关临床分析中的有前途的实际潜力。