Cao Yue, Zhu Wenlei, Li Lingling, Zhang Ziyi, Chen Zixuan, Lin Yuehe, Zhu Jun-Jie
State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, PR China.
Nanoscale. 2020 Apr 3;12(13):7321-7329. doi: 10.1039/d0nr00179a.
In this work, CsPbBr3 perovskite nanocrystals (NCs) synthesized via a ligand-assisted reprecipitation method (LCPB) were discovered to emit self-enhanced electrochemiluminescence (ECL) with the surface oleylamine as both a coreactant and a stabilizer. Solvent regulation and tri-n-octylphosphine post-treatment were manipulated for size-selected and surface-passivated LCPBs, which showed remarkable aqueous ECL performance with respect to efficiency and stability. Furthermore, thanks to the self-enhancement mode with a shorter charge transfer pathway and less energy loss, the ECL efficiency obtained for these as-synthesized LCPBs in aqueous solution without any additional coreactant was up to 57.08% using the Ru(bpy)32+-tripropylamine system as the standard. As a proof-of-concept, the products were successfully employed for the bioanalyses of hydrogen peroxide, ascorbic acid, and cancer cells based on inhibition, coreaction, and impedance detection principles, respectively. More importantly, the basic properties of LCPBs in aqueous media including surface chemistry, charge transfer process, and ECL mechanism were studied systematically. Such efforts are aimed at perfecting the fundamental research of all-inorganic perovskite NCs and opening an avenue for the design of highly crystalline and luminescent perovskites as advanced ECL emitters for applications in the ECL domain.
在这项工作中，通过配体辅助再沉淀法（LCPB）合成的CsPbBr3钙钛矿纳米晶体（NCs）被发现以表面油胺作为共反应剂和稳定剂发出自增强电化学发光（ECL）。对溶剂调节和三正辛基膦后处理进行了操作，以实现尺寸选择和表面钝化的LCPB，其在效率和稳定性方面表现出卓越的水性ECL性能。此外，由于具有较短电荷转移途径和较少能量损失的自增强模式，在不使用任何额外共反应剂的水溶液中，使用Ru(bpy)32+-三丙胺体系作为标准，这些合成的LCPB获得的ECL效率高达57.08%。作为概念验证，这些产物分别基于抑制、共反应和阻抗检测原理成功用于过氧化氢、抗坏血酸和癌细胞的生物分析。更重要的是，系统地研究了LCPB在水性介质中的基本性质，包括表面化学、电荷转移过程和ECL机制。这些努力旨在完善全无机钙钛矿NCs的基础研究，并为设计高度结晶和发光的钙钛矿开辟一条途径，作为用于ECL领域应用的先进ECL发射体。
