School of Chemistry and Chemical Engineering , Shandong University , Jinan 250100 , P. R. China.
College of Chemistry, Chemical Engineering and Materials Science, Key Laboratory of Molecular and Nano Probes, Ministry of Education , Shandong Normal University , Jinan 250014 , P. R. China.
Anal Chem. 2019 Mar 5;91(5):3754-3758. doi: 10.1021/acs.analchem.9b00199. Epub 2019 Feb 22.
For the screening of novel toxic-element-free and biocompatible electrochemiluminophores, electrochemiluminescence (ECL) of multinary nanocrystals (NCs) was investigated for the first time with Zn-Ag-In-S (ZAIS) NCs as model. Aqueous soluble ZAIS NCs could bring out efficient reductive-oxidation ECL with tri- n-propylamine as coreactant, while coating the ZAIS NCs with a ZnS shell could reduce the surface defects of ZAIS NCs, and enable 6.7-fold enhanced ECL of ZAIS/ZnS NCs as compared to ZAIS NCs. ECL of ZAIS/ZnS NCs was about 4.2-fold that of ternary CuInS/ZnS NCs, spectrally similar to that of Ru(bpy) with maximum emission around 605 nm, and favorable for less electrochemical interference with a lowered triggering potential (∼0.95 V) than that of Ru(bpy). An ultrasensitive ECL microRNA sensor was fabricated with ZAIS/ZnS NCs as tags, which could sensitively and selectively determine microRNA-141 with a wide linearity range from 0.1 fmol/L to 20 pmol/L and a low limit of detection at 50 amol/L ( S/ N = 3). Multinary NCs might provide a promising alternative to the traditional binary NCs for both electrochemiluminophore screening and NC ECL modulating.
为了筛选新型无毒、生物相容的电化学发光体，我们首次研究了多元纳米晶体（NCs）的电化学发光（ECL），以 Zn-Ag-In-S（ZAIS）NCs 为模型。水溶性 ZAIS NCs 可以与三正丙胺作为共反应物产生有效的还原-氧化 ECL，而在 ZAIS NCs 表面涂覆 ZnS 壳可以减少 ZAIS NCs 的表面缺陷，并使 ZAIS/ZnS NCs 的 ECL 增强 6.7 倍，与 ZAIS NCs 相比。ZAIS/ZnS NCs 的 ECL 约为三元 CuInS/ZnS NCs 的 4.2 倍，光谱与 Ru(bpy)相似，最大发射波长约为 605nm，与 Ru(bpy)相比，触发电位（约 0.95V）更低，电化学干扰更小。我们使用 ZAIS/ZnS NCs 作为标记物构建了一种超灵敏的 ECL microRNA 传感器，该传感器可以对 microRNA-141 进行灵敏和选择性的测定，线性范围从 0.1 fmol/L 到 20 pmol/L，检测限低至 50 amol/L（S/N=3）。多元 NCs 可能为电化学发光体筛选和 NC ECL 调节提供一种有前途的传统二元 NCs 的替代方案。
