Cao Yue, Zhang Ziyi, Li Lingling, Zhang Jian-Rong, Zhu Jun-Jie
State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering , Nanjing University , Nanjing 210023 , PR China.
Anal Chem. 2019 Jul 2;91(13):8607-8614. doi: 10.1021/acs.analchem.9b01918. Epub 2019 Jun 13.
Low-toxic trivalent bismuth, with an isoelectronic structure (6s6p) and a similar ionic radius to divalent lead, represents a promising candidate for constructing lead-free perovskites. Herein, cesium bismuth halide perovskite quantum dots (CsBiBr QDs) were synthesized via a comprehensively improved ligand-assisted reprecipitation method with the addition of γ-butyrolactone, trace distilled water, and tetrabutylammonium bromide, as well as the aid of ultrasonic technology. The as-prepared QDs displayed remarkable monodispersity, outstanding stability, and highly passivated surfaces with a near-single-component PL decay, thus affording superb optical properties with a photoluminescence quantum yield up to 37%, outperforming all the reported bismuth-based perovskites. Furthermore, CsBiBr QDs were first attempted for electrochemiluminescence (ECL) and exhibited a stable and efficient ECL response following either an annihilation or a coreaction ECL mechanism. Not only were the optical properties and stability of CsBiBr QDs greatly improved in this work, but their electrochemical behaviors and ECL natures were also investigated systematically for the first time, demonstrating the significant potential to extend this environmentally friendly bismuth-based perovskite into the ECL domain.
低毒三价铋具有等电子结构(6s6p)且离子半径与二价铅相似,是构建无铅钙钛矿的一个有前景的候选材料。在此,通过全面改进的配体辅助再沉淀法,添加γ-丁内酯、微量蒸馏水和四丁基溴化铵,并借助超声技术,合成了卤化铯铋钙钛矿量子点(CsBiBr QDs)。所制备的量子点表现出显著的单分散性、出色的稳定性以及表面高度钝化且具有近单组分的光致发光衰减,从而具有高达37%的光致发光量子产率,展现出优异的光学性能,优于所有已报道的铋基钙钛矿。此外,首次尝试将CsBiBr QDs用于电化学发光(ECL),并在湮灭或共反应ECL机制下表现出稳定且高效的ECL响应。在这项工作中,不仅CsBiBr QDs的光学性能和稳定性得到了极大改善,而且其电化学行为和ECL性质也首次得到系统研究,证明了将这种环境友好的铋基钙钛矿扩展到ECL领域的巨大潜力。