School of Chemistry and Chemical Engineering, Shandong University , Jinan, 250100, China.
Department of Chemistry and Biochemistry, The University of Southern Mississippi , Hattiesburg, Mississippi 39406-0001, United States.
Anal Chem. 2016 Jul 5;88(13):6947-53. doi: 10.1021/acs.analchem.6b01821. Epub 2016 Jun 16.
Conventional electrochemiluminescence (ECL) research has been performed by detecting the total photons (i.e., the ECL intensity). Herein, systematic spectral exploration on the ECL of dual-stabilizers-capped ternary CdZnSe nanocrystals (NCs) and its sensing application were carried out on a homemade ECL spectral acquiring system. The ternary CdZnSe NCs could be repeatedly injected with electrons via some electrochemical ways and then result in strong cathodic ECL with the coupling of ammonium persulfate. ECL spectrum of the CdZnSe NCs was almost identical to corresponding photoluminescence spectrum, indicating that the excited states of CdZnSe NCs in ECL were essentially the same as those in photoluminescence. Importantly, after being labeled to the probe antibody (Ab2) of α-fetal protein (AFP) antigen, the ternary NCs in the Ab2|NCs conjugates could preserve their ECL spectrum very well. A spectrum-based ECL immunoassay was consequently proposed with the CdZnSe NCs as ECL tags and AFP as target molecules. The limit of detection is 0.010 pg/mL, with a signal-to-noise (S/N) ratio of 3, indicating a sensitive ECL sensing strategy that was different from the conventional ones. This work might open a pathway to the spectrally resolved ECL analysis with even-higher S/N ratios than the fluorescent analysis.
传统的电化学发光(ECL)研究通过检测总光子(即 ECL 强度)来进行。本文在自制的 ECL 光谱采集系统上,对双稳定剂封端的三元 CdZnSe 纳米晶体(NCs)的 ECL 进行了系统的光谱探索及其传感应用。通过一些电化学方法,三元 CdZnSe NCs 可以反复注入电子,然后与过硫酸铵耦合产生强阴极 ECL。CdZnSe NCs 的 ECL 光谱几乎与相应的光致发光光谱完全一致,这表明 ECL 中 CdZnSe NCs 的激发态与光致发光中的激发态基本相同。重要的是,经过标记α-胎儿蛋白(AFP)抗原的探针抗体(Ab2)后,Ab2|NCs 缀合物中的三元 NCs 能够很好地保持其 ECL 光谱。因此,提出了一种基于光谱的 ECL 免疫分析方法,以 CdZnSe NCs 作为 ECL 标记物,以 AFP 作为靶分子。检测限为 0.010 pg/mL,信噪比(S/N)为 3,表明这是一种与传统方法不同的灵敏 ECL 传感策略。这项工作可能为光谱分辨 ECL 分析开辟了一条途径,其 S/N 比甚至高于荧光分析。