Zhang Hong, Li Bo, Wang Ruiying, Miao Qiannan, Cui Xiaomin, Shang Lei, Ma Rongna, Jia Liping, Li Chuan, Li Fenghua, He Shuijian, Zhang Wei, Wang Huaisheng
Chemistry of Department, Liaocheng University, Liaocheng, Shandong, 252059, China.
Department of Gastrointestinal Surgery, Shandong Provincial Third Hospital, Shandong University, China.
Talanta. 2023 Jul 1;259:124489. doi: 10.1016/j.talanta.2023.124489. Epub 2023 Mar 29.
To design highly efficient electrochemistry system was important for construct simple and sensitive biosensors, which was crucial in clinical diagnosis and therapy. In this work, a novel electrochemistry probe N,N'-di (1-hydroxyethyl dimethylaminoethyl) perylene diimide (HDPDI) with positive charges was reported to show two-electron redox behavior in neutral phosphate buffer solution between 0 and -1.0 V. And KSO in solution could significantly increase the reduction current of HDPDI at -0.29 V, which was interpreted with cyclic catalysis mechanism of KSO. Moreover, HDPDI as electrochemical probe and KSO as signal enhancer was used to design aptasensors for protein detection. Thrombin was used as target model protein. Thiolate ssDNA with thrombin-binding sequence was immobilized on gold electrode to selectively capture thrombin and adsorb HDPDI. The thiolate ssDNA without binding with thrombin was with random coil structure and could adsorb HDPDI through electrostatic attraction interaction. However, the thiolate ssDNA binding with thrombin became G-quadruplex structure and hardly adsorbed HDPDI. Thus, with increasing the concentration of thrombin, the current signal stepwisely decreased and was taken as detection signal. Compared with other aptasensors based on electrochemistry molecules without signal enhancer, the proposed aptasensors exhibited wider linear response for thrombin between 1 pg mL and 100 ng mL with lower detection limit 0.13 pg mL. In addition, the proposed aptasensor showed good feasibility in human serum samples.
设计高效的电化学系统对于构建简单且灵敏的生物传感器至关重要,这在临床诊断和治疗中起着关键作用。在这项工作中,报道了一种新型带正电荷的电化学探针N,N'-二(1-羟乙基二甲基氨基乙基)苝二酰亚胺(HDPDI),其在0至-1.0 V的中性磷酸盐缓冲溶液中表现出双电子氧化还原行为。溶液中的KSO可显著增加HDPDI在-0.29 V处的还原电流,这可以用KSO的循环催化机制来解释。此外,HDPDI作为电化学探针,KSO作为信号增强剂,用于设计蛋白质检测的适配体传感器。凝血酶用作目标模型蛋白。将具有凝血酶结合序列的硫醇化单链DNA固定在金电极上以选择性捕获凝血酶并吸附HDPDI。未与凝血酶结合的硫醇化单链DNA具有无规卷曲结构,可通过静电吸引相互作用吸附HDPDI。然而,与凝血酶结合的硫醇化单链DNA变成G-四链体结构,几乎不吸附HDPDI。因此,随着凝血酶浓度的增加,电流信号逐步降低,并将其作为检测信号。与其他基于无信号增强剂的电化学分子的适配体传感器相比,所提出的适配体传感器对凝血酶在1 pg mL至100 ng mL之间表现出更宽的线性响应,检测限更低,为0.13 pg mL。此外,所提出的适配体传感器在人血清样品中显示出良好的可行性。