College of Chemistry, Chemical Engineering and Materials Science, Collaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of Shandong, Key Laboratory of Molecular and Nano Probes, Ministry of Education, Shandong Provincial Key Laboratory of Clean Production of Fine Chemicals , Shandong Normal University , Jinan 250014 , China.
School of Chemistry and Chemical Engineering , Shandong University , Jinan , Shandong 250100 , China.
ACS Appl Mater Interfaces. 2020 Feb 19;12(7):7966-7973. doi: 10.1021/acsami.9b21943. Epub 2020 Feb 4.
We demonstrate the aggregation-induced electrochemiluminescence (AIECL) generated by 1,1,2,2-tetrakis(4-bromophenyl)ethane (TBPE)-based conjugated microporous polymers (TBPE-CMPs) and its biosensing application. We synthesized three TBPE-CMPs (i.e., TBPE-CMP-1, -2, -3) using three different molecules including tris(4-ethynylphenyl)amine (TEPA), 4,4'-diethynylbiphenyl (DEP), and 2,4,6-tris(4-ethynylphenyl)-1,3,5-triazine (TEPT). The TBPE-CMPs can act as electrochemiluminescence (ECL) emitters to generate AIECL. Among them, TBPE-CMP-1 exhibits the highest ECL efficiency (1.72%) due to the improved electron-hole recombination efficiency and efficient suppression of nonradiative transition. Moreover, the ECL properties of TBPE-CMPs can be tuned by the introduction of different conjugated molecules that can decrease the energy gap to facilitate the injection of an electron into the conjugated polymer backbone. Importantly, TBPE-CMP-1 can be used to construct an ECL sensor for the detection of dopamine, whose electro-oxidation products (e.g., leucodopaminechrome (LDC), dopaminechrome (DC), 5,6-dihydroxyindole (DHI), and 5,6-indolequinone (IDQ)) may function as energy acceptors to quench the ECL emission of TBPE-CMP-1. This ECL sensor exhibits high sensitivity and good anti-interference capability against ascorbic acid and uric acid.
我们展示了基于 1,1,2,2-四(4-溴苯基)乙烷(TBPE)的共轭微孔聚合物(TBPE-CMP)的聚集诱导电化学发光(AIECL)及其生物传感应用。我们使用三种不同的分子合成了三种 TBPE-CMP(即 TBPE-CMP-1、-2、-3)，包括三(4-乙炔基苯基)胺(TEPA)、4,4'-二乙炔基联苯(DEP)和 2,4,6-三(4-乙炔基苯基)-1,3,5-三嗪(TEPT)。TBPE-CMP 可以作为电化学发光(ECL)发射器产生 AIECL。其中，TBPE-CMP-1 由于电子空穴复合效率的提高和非辐射跃迁的有效抑制，表现出最高的 ECL 效率(1.72%)。此外，通过引入不同的共轭分子可以调节 TBPE-CMP 的 ECL 性质，从而降低能隙，有利于电子注入共轭聚合物主链。重要的是，TBPE-CMP-1 可用于构建用于检测多巴胺的 ECL 传感器，其电氧化产物(例如，左旋多巴醌(LDC)、多巴醌(DC)、5,6-二羟基吲哚(DHI)和 5,6-吲哚醌(IDQ))可以作为能量受体来猝灭 TBPE-CMP-1 的 ECL 发射。该 ECL 传感器对多巴胺具有高灵敏度和良好的抗抗干扰能力，对抗坏血酸和尿酸具有良好的抗干扰能力。
