Institute of Innovation Materials and Energy, School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, 225002, China.
Institute of Innovation Materials and Energy, School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, 225002, China; School of Chemistry and Chemical Engineering, Yancheng Institute of Technology, Yancheng, 224051, China.
Biosens Bioelectron. 2024 Jun 15;254:116201. doi: 10.1016/j.bios.2024.116201. Epub 2024 Mar 11.
Developing highly sensitive and selective methods that incorporate specific recognition elements is crucial for detecting small molecules because of the limited availability of small molecule antibodies and the challenges in obtaining sensitive signals. In this study, a generalizable photoelectrochemical-colorimetric dual-mode sensing platform was constructed based on the synergistic effects of a molecularly imprinted polymer (MIP)-aptamer sandwich structure and nanoenzymes. The MIP functionalized peroxidase-like FeO (FeO@MIPs) and alkaline phosphatase mimic Zr-MOF labeled aptamer (Zr-mof@Apt) were used as the recognition elements. By selectively accumulating dibutyl phthalate (DBP), a small molecule target model, on FeO@MIPs, the formation of Zr-MOF@Apt-DBP- FeO@MIPs sandwich structure was triggered. FeO@MIPs oxidized TMB to form blue-colored oxTMB. However, upon selective accumulation of DBP, the catalytic activity of FeO@MIPs was inhibited, resulting in a lighter color that was detectable by the colorimetric method. Additionally, Zr-mof@Apt effectively catalyzed the hydrolysis of L-Ascorbic acid 2-phosphate sesquimagnesium salt hydrate (AAPS), generating ascorbic acid (AA) that could neutralize the photogenerated holes to decrease the photocurrent signals for PEC sensing and reduce oxTMB for colorimetric testing. The dual-mode platform showed strong linearity for different concentrations of DBP from 1.0 pM to 10 μM (PEC) and 0.1 nM to 0.5 μM (colorimetry). The detection limits were 0.263 nM (PEC) and 30.1 nM (colorimetry) (S/N = 3), respectively. The integration of dual-signal measurement mode and sandwich recognition strategy provided a sensitive and accurate platform for the detection of small molecules.
开发包含特异性识别元件的高灵敏度和高选择性方法对于小分子的检测至关重要，因为小分子抗体的可用性有限，并且难以获得敏感的信号。在本研究中，基于分子印迹聚合物（MIP）-适配体夹心结构和纳米酶的协同作用，构建了一种可推广的光电化学-比色双模式传感平台。将功能化过氧化物酶样的 FeO（FeO@MIPs）和碱性磷酸酶模拟 Zr-MOF 标记的适配体（Zr-mof@Apt）作为识别元件。通过在 FeO@MIPs 上选择性地积累小分子目标物邻苯二甲酸二丁酯（DBP），触发 Zr-MOF@Apt-DBP-FeO@MIPs 夹心结构的形成。FeO@MIPs 将 TMB 氧化为蓝色的 oxTMB。然而，当 DBP 被选择性地积累时，FeO@MIPs 的催化活性被抑制，导致颜色变浅，可以通过比色法检测。此外，Zr-mof@Apt 有效地催化 L-抗坏血酸 2-磷酸半镁盐水合物（AAPS）的水解，生成抗坏血酸（AA），可以中和光生空穴，减少 PEC 传感的光电流信号，并减少比色测试中的 oxTMB。该双模式平台对不同浓度的 DBP 表现出较强的线性关系，从 1.0 pM 到 10 μM（PEC）和 0.1 nM 到 0.5 μM（比色法）。检测限分别为 0.263 nM（PEC）和 30.1 nM（比色法）（S/N = 3）。双信号测量模式和夹心识别策略的集成为小分子的检测提供了一个灵敏、准确的平台。
