College of Environmental Science and Engineering, Hunan University, Changsha 410082, China.
Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082, China.
Anal Chem. 2021 Jul 6;93(26):9129-9138. doi: 10.1021/acs.analchem.1c00929. Epub 2021 Jun 21.
With the high sensitivity and anti-interference provided by a dual Z-scheme structure photoanode and a two-electrode system, a high-performance self-powered photoelectrochemical (PEC) aptasensor for oxytetracycline (OTC) detection was established in this work. Graphitic carbon nitride (g-CN) with excellent photoelectric properties was used to be combined with WO and MnO to form a kind of dual Z-scheme heterojunction. The designed unique structure and the complementary performances of the three materials collectively guaranteed the highly stable photocurrent output of the photoanode due to the wide range of light absorption and the high separation rate of electron-hole pairs. The aptamer-based cathode modified with reduced graphene oxide (rGO) and Au nanoparticles (Au NPs) provided high conductivity and aptamer-binding sites, which brought excellent selective recognition of OTC as well as the self-powered capacity by receiving electrons from the photoanode. In the PEC sensing of OTC, the device presented a wide detection range from 1 pM to 150 nM and a low detection limit of 0.1 pM. Besides, the developed PEC aptasenor showed good selectivity, reproducibility, and stability, so as to be applied to real samples. The proposed PEC sensing method can be considered an effective and promising direction for the detection of antibiotics in the future.
本工作构建了一种基于双 Z 型结构光阳极和两电极系统的高灵敏度和抗干扰性能的自供电光电化学（PEC）适体传感器，用于检测土霉素（OTC）。具有优异光电性能的石墨相氮化碳（g-CN）与 WO 和 MnO 结合，形成一种双 Z 型异质结。设计的独特结构和三种材料的互补性能共同保证了光阳极由于宽的光吸收范围和高的电子-空穴对分离率而具有高度稳定的光电流输出。基于适配体的阴极用还原氧化石墨烯（rGO）和金纳米粒子（Au NPs）修饰，提供了高导电性和适配体结合位点，从而对 OTC 具有优异的选择性识别能力，并通过从光阳极接收电子而具有自供电能力。在 OTC 的 PEC 传感中，该器件的检测范围从 1 pM 到 150 nM，检测限低至 0.1 pM。此外，所开发的 PEC 适体传感器表现出良好的选择性、重现性和稳定性，可用于实际样品。该提出的 PEC 传感方法可被视为未来抗生素检测的一种有效且有前景的方向。
