Photocurrent Polarity Reversal Induced by Electron-Donor Release for the Highly Sensitive Photoelectrochemical Detection of Vascular Endothelial Growth Factor 165,Analytical Chemistry

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Photocurrent Polarity Reversal Induced by Electron-Donor Release for the Highly Sensitive Photoelectrochemical Detection of Vascular Endothelial Growth Factor 165
Analytical Chemistry ( IF 6.7 ) Pub Date : 2023-10-27 , DOI: 10.1021/acs.analchem.3c03982
Weisu Kong ₁ , Zhiyuan Xu ₁ , Tianrui Liu ₁ , Jianping Lei ₁ , Huangxian Ju ₁

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Photocurrent polarity reversal is a switching process between the anodic and cathodic pathways and is critical for eliminating false positivity and improving detection sensitivity in photoelectrochemical (PEC) sensing. In this study, we construct a PEC sensor with excellent photocurrent polarity reversal induced by ascorbic acid (AA) as an electron donor with the energy level matching the photoactive material zirconium metal–organic framework (ZrMOF). The ZrMOF-modified electrode demonstrates cathodic photocurrent in the presence of O₂ as an electron acceptor, while the anodic photocurrent is generated in the presence of AA, achieving photocurrent polarity reversal. By the in situ release of AA from AA-encapsulated apoferritin modified with DNA 2 (AA@APO-S2) as a detection tag in the presence of trypsin after the recognition of hairpin DNA-modified indium tin oxide to the reaction product of aptamer/DNA 1 with the target protein and the following rolling cycle amplification for introducing the detection tag to the sensing interface, the reversed photocurrent shows an enhanced photocurrent response to the target protein, leading to a highly sensitive PEC sensing strategy. This strategy realizes the detection of vascular endothelial growth factor 165 with good specificity, a wide linear range, and a low detection limit down to 5.3 fM. The actual sample analysis offers the detection results of the proposed PEC sensor comparable to those of commercial enzyme-linked immunosorbent assay tests, indicating the promising application of the photocurrent polarity reversal-based PEC sensing strategy in biomolecule detection and clinical diagnosis.

中文翻译：

电子供体释放诱导的光电流极性反转用于血管内皮生长因子 165 的高灵敏光电化学检测

光电流极性反转是阳极和阴极路径之间的切换过程，对于消除假阳性和提高光电化学（PEC）传感中的检测灵敏度至关重要。在本研究中，我们构建了一种 PEC 传感器，该传感器具有优异的光电流极性反转，由抗坏血酸（AA）作为电子供体诱导，其能级与光活性材料锆金属有机骨架（ZrMOF）相匹配。ZrMOF修饰电极在O ₂作为电子受体时表现出阴极光电流，而在AA存在时产生阳极光电流，实现光电流极性反转。以DNA 2修饰的AA封装的脱铁铁蛋白（AA@APO-S2）作为检测标签，在胰蛋白酶存在下，将发夹DNA修饰的氧化铟锡识别为适体/反应产物后，原位释放AA。 DNA 1 与目标蛋白以及随后的滚动循环扩增将检测标签引入到传感界面，反向光电流显示出对目标蛋白的增强的光电流响应，从而形成高度灵敏的 PEC 传感策略。该策略实现了血管内皮生长因子165的检测，特异性好，线性范围宽，检测限低至5.3 fM。实际样品分析提供的 PEC 传感器的检测结果与商业酶联免疫吸附测定测试的结果相当，表明基于光电流极性反转的 PEC 传感策略在生物分子检测和临床诊断中的应用前景。

更新日期：2023-10-27

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