State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, P.R. China.
School of Mechanical and Materials Engineering, Washington State University, Pullman, Washington 99164, United States.
Anal Chem. 2020 Mar 3;92(5):4123-4130. doi: 10.1021/acs.analchem.0c00070. Epub 2020 Feb 21.
Lead halide perovskites have been promising electrochemiluminescence (ECL) candidates because of their excellent photophysical attributes, but their poor stability has severely restricted ECL applications. Herein, the in situ assembly of all-inorganic perovskite CsPbBr nanocrystals (CPB) into hollow graphitic carbon nitride nanospheres (HCNS) were described as a novel ECL emitter. The architecture guaranteed not only improved stability because of the peripheral HCNS protecting shell but also high-performance ECL of CPB because of a matching band-edge arrangement. Dual-ECL readouts were obtained from the nanocomposite including an anodic ECL from CPB and a cathodic ECL from HCNS. The former displayed prominent color purity to construct an efficient ECL resonance energy transfer system, and the latter served as an internal standard for a ratiometric analysis. A well-designed DNA probe was further utilized for the targeting of CD44 receptors on the MCF-7 cell surface and the double signal amplification. The sensing strategy exhibited good analytical performance for MCF-7 cells, ranging from 1.0 × 10 to 3.2 × 10 cells mL with a detection limit of 320 cells mL. Sensitive and accurate evaluation of CD44 expression was finally achieved at 0.22 pM. This work is the first attempt to use halide perovskite for reliable ECL bioanalysis and provides a perspective to design a perovskite-based nanocomposite as a high-performance ECL emitter for its exclusive ECL system.
卤铅钙钛矿因其优异的光物理性质而成为很有前途的电致化学发光(ECL)候选材料,但它们的稳定性差严重限制了 ECL 的应用。在此,将全无机钙钛矿 CsPbBr 纳米晶体(CPB)原位组装到空心石墨相氮化碳纳米球(HCNS)中,作为一种新型 ECL 发射器。该结构不仅保证了由于外围 HCNS 保护壳而提高的稳定性,而且由于匹配的能带边缘排列,保证了 CPB 的高性能 ECL。从纳米复合材料中获得了双 ECL 读出,包括来自 CPB 的阳极 ECL 和来自 HCNS 的阴极 ECL。前者显示出突出的颜色纯度,构建了高效的 ECL 共振能量转移系统,后者作为比率分析的内部标准。进一步利用精心设计的 DNA 探针对 MCF-7 细胞表面的 CD44 受体进行靶向和双重信号放大。该传感策略对 MCF-7 细胞表现出良好的分析性能,检测范围从 1.0×10到 3.2×10 细胞 mL,检测限为 320 细胞 mL。最终以 0.22 pM 的检测限实现了对 CD44 表达的灵敏和准确评估。这项工作首次尝试将卤铅钙钛矿用于可靠的 ECL 生物分析,并为设计基于钙钛矿的纳米复合材料作为其独特的 ECL 系统的高性能 ECL 发射器提供了新视角。