Ultrastable CsPbBr3@CsPb2Br5@TiO2 Composites for Photocatalytic and White Light-Emitting Diodes

Abstract

Although cesium halide lead (CsPbX3, X = Cl, Br,I) perovskite quantum dots (QDs) have excellent photovoltaic properties, their unstable characteristics are major limitations to application. Previous research has demonstrated that the core−shell structure can significantly improve the stability of CsPbX3 QDs and form heterojunctions at interfaces, enabling multifunctionalization of perovskite materials. In this article, we propose a convenient method to construct core−shell-structured perovskite materials, in which CsPbBr3@CsPb2Br5 core−shell micrometer crystals can be prepared by controlling the ratio of Cs+/Pb2+ in the precursor and the reaction time. The materials exhibited enhanced optical properties and stability that provided for further postprocessing. Subsequently, CsPbBr3@CsPb2Br5@TiO2 composites were obtained by coating a layer of dense TiO2 nanoparticles on the surfaces of micrometer crystals through hydrolysis of titanium precursors. According to density functional theory (DFT) calculations and experimental results, the presence of surface TiO2 promoted delocalization of photogenerated electrons and holes, enabling the CsPbBr3@CsPb2Br5@TiO2 composites to exhibit excellent performance in the field of photocatalysis. In addition, due to passivation of surface defects by CsPb2Br5 and TiO2 shells, the luminous intensity of white light-emitting diodes prepared with the materials only decayed by 2%−3% at high temperatures (>100 °C) when working for 24 h.