Key Laboratory of Luminescent and Real-Time Analytical Chemistry (Southwest University), Ministry of Education, College of Chemistry and Chemical Engineering , Southwest University , Chongqing 400715 , PR China.
Anal Chem. 2019 Nov 19;91(22):14618-14623. doi: 10.1021/acs.analchem.9b03736. Epub 2019 Nov 6.
For the first time, simultaneous cathodic and anodic electrochemiluminescence (ECL) emissions of bull serum albumin stabilized Au nanoclusters (Au NCs) as highly efficient bipolar ECL probes were constructed for the single-step and synchronous determination of carcinoembryonic antigen (CEA) and mucin 1 (MUC1) based on different coreactant and coreaction accelerators. Under the potential cathodic scanning, TiO nanosheets (TiO NSs) as cathodic coreaction accelerators could catalyze the reduction of coreactant dissolved O for promoting cathodic ECL emission of Au NCs, while, under the potential anodic scanning, CuO@Cu nanoparticles (CuO@Cu NPs) as anodic coreaction accelerators could stimulate the oxidation of coreactant ,-diethylethylenediamine (DEDA) for enhancing anodic ECL emission of Au NCs. Thus, the proposed strategy easily solved one main technical challenge of cross reactions of dual-luminophors for dual-biomarker detection, resulting in great sensitivity and accuracy toward the detection of CEA down to 0.43 pg/mL and MUC1 down to 5.8 fg/mL. As a proof of concept, this work realized single-step and simultaneous detection of dual biomarkers, which initiates a new thought in realizing a new generation of dual-biomarker ECL detection beyond the traditional ones in sensing analysis and diagnostic sensing.
首次构建了牛血清白蛋白稳定的金纳米簇(Au NCs)作为高效双极电致化学发光(ECL)探针的同时阴极和阳极 ECL 发射,用于基于不同共反应物和共反应加速剂的癌胚抗原(CEA)和黏蛋白 1(MUC1)的单步和同步测定。在阴极扫描电位下,TiO 纳米片(TiO NSs)作为阴极共反应加速剂可以催化溶解 O 的还原,以促进 Au NCs 的阴极 ECL 发射,而在阳极扫描电位下,CuO@Cu 纳米颗粒(CuO@Cu NPs)作为阳极共反应加速剂可以刺激共反应物,-二乙基亚乙基二胺(DEDA)的氧化,以增强 Au NCs 的阳极 ECL 发射。因此,该策略轻松解决了双发光体交叉反应用于双重生物标志物检测的一个主要技术挑战,从而实现了对 CEA 的检测灵敏度达到 0.43 pg/mL,对 MUC1 的检测灵敏度达到 5.8 fg/mL。作为概念验证,本工作实现了双重生物标志物的单步和同时检测,这在传感分析和诊断传感领域超越了传统的检测方法,为新一代双重生物标志物 ECL 检测开辟了新的思路。