Efficient and Stable CsPbBr3 Quantum-Dot Powders Passivated and Encapsulated with a Mixed Silicon Nitride and Silicon Oxide Inorganic Polymer Matrix

摘要

Despite the excellent optical features of fully inorganic cesium lead halide (CsPbX3) perovskite quantum dots (PeQDs), their unstable nature has limited their use in various optoelectronic devices. To mitigate the instability issues of PeQDs, we demonstrate the roles of dual-silicon nitride and silicon oxide ligands of the polysilazane (PSZ) inorganic polymer to passivate the surface defects and form a barrier layer coated onto green CsPbBr3 QDs to maintain the high photoluminescence quantum yield (PLQY) and improve the environmental stability. The mixed SiNx/SiNxOy/SiOy passivated and encapsulated CsPbBr3/PSZ core/shell composite can be prepared by a simple hydrolysis reaction involving the addition of adding PSZ as a precursor and a slight amount of water into a colloidal CsPbBr3 QD solution. The degree of the moisture-induced hydrolysis reaction of PSZ can affect the compositional ratio of SiNx, SiNxOy, and SiOy liganded to the surfaces of the CsPbBr3 QDs to optimize the PLQY and the stability of CsPbBr3/PSZ core/shell composite, which shows a high PLQY (similar to 81.7%) with improved thermal, photo, air, and humidity stability as well under coarse conditions where the performance of CsPbBr3 QDs typically deteriorate. To evaluate the suitability of the application of the CsPbBr3/PSZ powder to down-converted white-light-emitting diodes (DC-WLEDs) as the backlight of a liquid crystal display (LCD), we fabricated an on-package type of tricolor-WLED by mixing the as-synthesized green CsPbBr3/PSZ composite powder with red K2SiF6:Mn4+ phosphor powder and a poly(methylmethacrylate)-encapsulating binder and coating this mixed paste onto a cup-type blue LED. The fabricated WLED show high luminous efficacy of 138.6 lm/W (EQE = 51.4%) and a wide color gamut of 128% and 111% without and with color filters, respectively, at a correlated color temperature of 6762 K.