School of Resources and Environment, University of Jinan, Jinan 250022, PR China.
School of Resources and Environment, University of Jinan, Jinan 250022, PR China.
Biosens Bioelectron. 2018 Oct 15;117:575-582. doi: 10.1016/j.bios.2018.06.050. Epub 2018 Jun 26.
A novel photoelectrochemical (PEC) bioassay protocol for diethylstilbestrol (DES) was systematically proposed. The Au/UiO-66(NH) hybrid with countless active sites was fabricated using an in situ reduction strategy and was subsequently decorated with CdS nanoparticles (NPs) by a sequential chemical bath deposition process. The resulting Au/UiO-66(NH)/CdS composites were exploited as a sensing matrix for the first time. The excellent photocurrent response of the as-prepared hybrid under visible light is attributed to its improved photo-electric conversion efficiency due to the local surface plasma resonance (LSPR) effect of Au and the matching energy-level structure between UiO-66(NH) and CdS. In addition, the competitive strategy for the detection of DES was devised by employing the direct Z-scheme Melem/CdTe heterojunction covalently conjugated with bovine serum albumin (BSA)-DES as signal tags. As a consequence, a cascade-like band-edge level was obtained, which could effectively promote the transfer of photogenerated charges and markedly improve the photocurrent. On the basis of the above strategy, the concentrations of DES could be detected through the competitive binding of DES antibodies (Anti-DES) with either Melem/CdTe/BSA-DES or free DES. Under optimal conditions, the linear range for the detection of DES was 0.1 pg mL to 20 ng mL. The detection limit was as low as 0.06 pg mL (S/N = 3). Furthermore, the designed PEC DES-sensing approach has acceptable selectivity, reproducibility, and stability and offers great promise for the detection of small molecules in biomedical, food and environmental samples.
系统地提出了一种用于检测己烯雌酚(DES)的光电化学(PEC)生物分析新方案。采用原位还原策略制备了具有无数活性位点的 Au/UiO-66(NH)杂化材料，随后通过顺序化学浴沉积过程用 CdS 纳米粒子(NPs)进行修饰。首次将所得的 Au/UiO-66(NH)/CdS 复合材料用作传感基质。由于 Au 的局部表面等离子体共振(LSPR)效应和 UiO-66(NH)与 CdS 之间的匹配能级结构，所制备的杂化材料在可见光下表现出优异的光电流响应。此外，通过采用直接 Z 型 Melem/CdTe 异质结共价键合牛血清白蛋白(BSA)-DES 作为信号标签，设计了用于检测 DES 的竞争策略。因此，获得了级联能带结构，这可以有效地促进光生载流子的转移，并显著提高光电流。基于上述策略，可以通过 DES 抗体(Anti-DES)与 Melem/CdTe/BSA-DES 或游离 DES 的竞争结合来检测 DES 的浓度。在最佳条件下，检测 DES 的线性范围为 0.1 pg/mL 至 20 ng/mL。检测限低至 0.06 pg/mL(S/N = 3)。此外，所设计的 PEC DES 传感方法具有可接受的选择性、重现性和稳定性，为生物医学、食品和环境样品中小分子的检测提供了广阔的前景。
