Department of Chemistry , Liaocheng University , Liaocheng 252059 , China.
College of Materials Science and Engineering , Nanjing Forestry University , Nanjing 210037 , China.
ACS Appl Mater Interfaces. 2019 Sep 18;11(37):33676-33683. doi: 10.1021/acsami.9b11416. Epub 2019 Sep 4.
In the field of clinical diagnosis, it is important to construct a potential-resolved multiplex electrochemiluminescence (ECL) biosensor for decreasing the false-positive rate and improving the diagnostic accuracy. However, the shortage of low-potential cathodic luminophores between -1 and 0 V (vs Ag/AgCl) severely limited the development of the biosensor. Herein, we synthesized a novel luminophore ,-bis-(3-dimethyl aminopropyl)-3,4,9,10-perylene tetracarboxylic acid diimide (PDI), which gave dual emissions at -0.25/-0.26 V with KSO as a co-reactant in aqueous solution. The ECL was assigned to excited J-type PDI dimers. Then, PDI and luminol were used as luminophores to respectively combine with graphite oxide and gold nanoparticles and form potential-resolved ECL nanoprobes. Also, this potential-resolved ECL nanoprobes were respectively functionalized by secondary antibodies (Ab) to construct a low-potential sandwiched ECL immunosensor for tumor markers carcinoembryonic antigen (CEA) and α-fetoprotein (AFP) simultaneous determination during linear scanning potential range from -0.6 to 0.6 V. The prepared multiplex immunosensor exhibited sensitive ECL response for CEA at -0.6 V due to PDI and that for AFP at 0.6 V due to luminol, and both linear semilogarithmical ranges were from 0.1 pg to 1 ng mL. In addition, PDI with dual ECL peaks showed enticing prospect of built-in self-calibration for a precise quantitative and bioimaging analysis.
在临床诊断领域,构建潜在解析的多重电化学发光(ECL)生物传感器对于降低假阳性率和提高诊断准确性非常重要。然而,-1 至 0 V(相对于 Ag/AgCl)之间的低电位阴极发光体的短缺严重限制了生物传感器的发展。在此,我们合成了一种新型发光体,β-双(3-二甲基氨基丙基)-3,4,9,10-苝四羧酸二酰亚胺(PDI),在水溶液中以 KSO 为共反应物,其在-0.25/-0.26 V 处给出双重发射。ECL 被分配给激发的 J 型 PDI 二聚体。然后,PDI 和鲁米诺分别用作发光体,与氧化石墨和金纳米粒子结合形成潜在解析的 ECL 纳米探针。此外,该潜在解析的 ECL 纳米探针分别通过二级抗体(Ab)功能化,以构建用于肿瘤标志物癌胚抗原(CEA)和α-胎蛋白(AFP)同时测定的低电位夹心 ECL 免疫传感器,在从-0.6 至 0.6 V 的线性扫描电位范围内。制备的多重免疫传感器在-0.6 V 处由于 PDI 对 CEA 表现出灵敏的 ECL 响应,在 0.6 V 处由于鲁米诺对 AFP 表现出灵敏的 ECL 响应,并且两者的线性半对数范围均为 0.1 pg 至 1 ng mL。此外,具有双重 ECL 峰的 PDI 为精确定量和生物成像分析提供了内置自校准的诱人前景。