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Perylene diimide and g-C3N4 nanosheet as potential-resolved cathode luminophores for ultrasensitive ratiometric electrochemiluminescence immunosensor
Sensors and Actuators B: Chemical ( IF 8.4 ) Pub Date : 2022-08-06 , DOI: 10.1016/j.snb.2022.132492
Wei Zhang , Xiaomin Cui , Fenghua Li , Wei Yan , Yunyun Wang , Lei Shang , Rongna Ma , Liping Jia , Chuan Li , Huaisheng Wang

In electrochemiluminescence(ECL) field, the shortage of potential-resolved luminophores severiously limited the development of biosensors for accurate assay such as ratiometric biosensors. In this work, N,N′-dimethyl-3,4,9,10-perylenedicarboximide(PDI-CH3) and graphite-like carbon nitride(g-C3N4) nanosheet was firstly reported to produce potential-resolved ECL with coreactant K2S2O8 between 0 and − 1.2 V. And there was good overlap between the ECL spectrum of g-C3N4 and the absorption spectra of PDI-CH3. Moreover, PDI-CH3 and g-C3N4 were used to construct ECL ratiometric system for sandwiched immunosensors to detect tumor marker carcinoembryonic antigen (CEA), in which g-C3N4 was used as ECL platform and PDI-CH3 was used as ECL label of secondary antibody(Ab2). Increasing the CEA concentration, the loading of PDI-CH3 on the electrode stepwisely increased, which leaded to gradual increase of ECLPDI-CH3 at − 0.5 V and significant decrease of ECLg-C3N4 at − 1.2 V due to the high quenching effects of PDI-CH3 to g-C3N4 through dual-quenching mechanism: competitive consumption of coreactant and ECL resonance energy transfer. And the ECLPDI-CH3/ECLg-C3N4 showed ultrasensitive linear response for CEA between 0.1 fg mL−1 and 1 ng mL−1 with detection limit 0.052 fg mL−1 according to IUPAC criterion. In addition, the proposed ratiometric biosensor exhibited good recovery in human serum samples.



中文翻译:

苝二亚胺和 g-C3N4 纳米片作为电位分辨阴极发光体用于超灵敏比率电化学发光免疫传感器

在电化学发光(ECL)领域,电位分辨发光体的短缺严重限制了生物传感器的发展,例如比例生物传感器。在这项工作中,首次报道了N,N'-二甲基-3,4,9,10-苝二甲酰亚胺(PDI-CH 3)和类石墨氮化碳(gC 3 N 4)纳米片与共反应物产生电位分辨的ECL K 2 S 2 O 8介于0和-1.2 V之间。gC 3 N 4的ECL光谱和PDI-CH 3的吸收光谱有很好的重叠。此外,PDI-CH 3和 gC 3 N 4以gC 3 N 4为ECL平台,PDI-CH 3为二抗(Ab 2 )的ECL标记,构建了夹层免疫传感器ECL比率系统检测肿瘤标志物癌胚抗原(CEA )。随着 CEA 浓度的增加,电极上 PDI-CH 3的负载量逐步增加,导致 ECL PDI-CH3在 - 0.5 V 时逐渐增加,而 ECL g-C3N4在 - 1.2 V 时由于高淬火效应显着降低PDI-CH 3至 gC 3 N 4通过双重淬灭机制:共反应物的竞争消耗和 ECL 共振能量转移。根据 IUPAC 标准,ECL PDI-CH3 /ECL g-C3N4对 CEA 在 0.1 fg mL -1和 1 ng mL -1之间显示出超灵敏的线性响应,检测限为 0.052 fg mL -1 。此外,所提出的比率生物传感器在人血清样品中表现出良好的恢复。

更新日期:2022-08-11
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