Chen Xiaoyan, Li Qiuju, Yuan Taoyue, Ma Mengtao, Ye Ziwei, Wei Xiaojie, Fang Xian, Mao Shun
Department of Chemistry and Materials Science, College of Science, Nanjing Forestry University, 159 Longpan Road, Nanjing, Jiangsu210037, China.
College of Environmental Science and Engineering, State Key Laboratory of Pollution Control and Resource Reuse, Tongji University, 1239 Siping Road, Shanghai200092, China.
ACS Sens. 2023 Feb 24;8(2):858-866. doi: 10.1021/acssensors.2c02562. Epub 2023 Jan 26.
Two-dimensional (2D) black phosphorus (BP) has been reported to have appealing semiconducting properties as the sensing channel in field-effect transistor (FET) sensors. However, the intrinsic instability of BP in water greatly hinders its application, and little is known about its sensing performance and mechanism in aqueous medium. Herein, a water-stable BP FET sensor for antibiotic detection is reported. A novel surface engineering strategy with Ag coordination and melamine cyanurate (MC) supramolecular passivation is utilized to enhance the stability and transistor performance of BP. With molecularly imprinted polymers (MIPs) as the detection probe for tetracycline, the BP/MC/MIPs sensor shows high sensitivity to tetracycline with a detection limit of 7.94 nM and a quick response within 6 s as well as high selectivity against other antibiotics with similar molecular structures. A new sensing mechanism relying on the conjugation effect of the probe structure is proposed, and new knowledge about alkalinity-enhanced and ionic strength-related response from the electrostatic gating effect is given based on the solution chemistry impact study. This work offers an efficient surface engineering strategy to enable the application of 2D BP for antibiotic detection in aqueous medium and presents a new sensing mechanism in chemical analysis by FET sensors.
二维（2D）黑磷（BP）据报道作为场效应晶体管（FET）传感器中的传感通道具有吸引人的半导体特性。然而，BP在水中的固有不稳定性极大地阻碍了其应用，并且对于其在水性介质中的传感性能和机制知之甚少。在此，报道了一种用于抗生素检测的水稳定BP FET传感器。采用一种具有银配位和三聚氰胺氰尿酸盐（MC）超分子钝化的新型表面工程策略来增强BP的稳定性和晶体管性能。以分子印迹聚合物（MIPs）作为四环素的检测探针，BP/MC/MIPs传感器对四环素显示出高灵敏度，检测限为7.94 nM，在6秒内快速响应，并且对其他具有相似分子结构的抗生素具有高选择性。提出了一种基于探针结构共轭效应的新传感机制，并基于溶液化学影响研究给出了关于静电门控效应引起的碱度增强和离子强度相关响应的新知识。这项工作提供了一种有效的表面工程策略，以实现二维BP在水性介质中用于抗生素检测的应用，并展示了FET传感器在化学分析中的一种新传感机制。
