Institute of Bismuth Science, School of Materials and Chemistry, University of Shanghai for Science and Technology, 334 Jungong Road, Shanghai 200093, China.
School of Energy Engineering, Huanghuai University, Zhumadian, Henan Province 463600, China.
Anal Chem. 2024 Feb 27;96(8):3645-3654. doi: 10.1021/acs.analchem.3c05782. Epub 2024 Feb 14.
Accurate measurement of cancer markers in urine is a convenient method for tumor monitoring. However, the concentration of cancer markers in urine is so low that it is difficult to achieve their measurement. Photoelectrochemical (PEC) sensors are a promising technology to realize the detection of trace cancer markers due to their high sensitivity. Currently, the interference of nonspecific biomolecules in urine is the main reason affecting the high sensitivity and selectivity of PEC sensors in detecting cancer markers. In this work, a strategy of oxygen vacancy (OV) modulation is proposed to construct a fouling-resistant PEC aptamer sensing platform for the detection of α-fetoprotein (AFP), a liver cancer marker. The introduction of OVs induces the formation of intermediate localized states in the photoelectric material, which not only facilitates the separation of photogenerated carriers but also leads to the redshift of the light absorption edge. More importantly, OVs with positive electrical properties can be employed to modify the antifouling layer (C-PEG) with negatively charged groups through an electrostatic interaction. The synergistic effect of OVs, antifouling layer, and aptamer resulted in a TiO/OVs/C-PEG-based PEC sensor achieves a wide linear range from 1 pg/mL to 100 ng/mL and a low detection limit of 0.3 pg/mL for AFP. In addition, the sensor successfully realized the determination of AFP in urine samples and accurately differentiated between normal people and liver cancer patients in the early and advanced stages. This project is of great significance in advancing the application of photoelectrochemical bioanalytical technology to achieve the detection of cancer markers in urine by investigating the construction of an OVs-regulated fouling-resistant sensing interface.
准确测量尿液中的癌症标志物是肿瘤监测的一种便捷方法。然而，由于癌症标志物在尿液中的浓度非常低，因此很难对其进行测量。光电化学（PEC）传感器是一种很有前途的技术，可以实现痕量癌症标志物的检测，因为它具有高灵敏度。目前，尿液中非特异性生物分子的干扰是影响 PEC 传感器检测癌症标志物的高灵敏度和选择性的主要原因。在这项工作中，提出了一种氧空位（OV）调制策略，用于构建用于检测肝癌标志物甲胎蛋白（AFP）的抗污染 PEC 适体传感平台。OV 的引入会在光电材料中形成中间局域态，这不仅有利于光生载流子的分离，而且还导致光吸收边缘的红移。更重要的是，具有正电性的 OV 可以通过静电相互作用来修饰带负电荷基团的抗污层（C-PEG）。OV、抗污层和适体的协同作用使基于 TiO/OVs/C-PEG 的 PEC 传感器实现了从 1 pg/mL 到 100 ng/mL 的宽线性范围和 0.3 pg/mL 的 AFP 低检测限。此外，该传感器成功实现了尿液样品中 AFP 的测定，并在早期和晚期准确地区分了正常人肝癌患者和。本项目在推进光电学生物分析技术在通过研究构建 OVs 调控的抗污染传感界面来实现尿液中癌症标志物检测中的应用方面具有重要意义。
